Emerging Pollutants

Emerging Pollutants

Katherine Y. Bell1*, Martha J.M. Wells2, Kathy A. Traexler3, Marie-Laure Pellegrin4,

Audra Morse5, Jeff Bandy6

ABSTRACT: Water and wastewater quality research and Overview management pertaining to emerging pollutants, chemical or The term Emerging Pollutants primarily refers to biological, for which discussion of occurrence surveys, fate those for which no regulations currently require monitoring and transport investigations, treatment processes, modeling, or public reporting of their presence in our water supply or and/or toxicity/risk assessment appearing in the peer- wastewater discharges. Many constituents described as reviewed literature during 2010, are presented. emerging pollutants are pharmaceuticals and personal care

products (PPCPs) that may enter the environment through

KEYWORDS: wastewater treatment, water treatment, excretion in human and animal urine and feces, through pharmaceuticals and personal care products, endocrine flushing of unused medications, household uses, or bathing, disrupting compounds, toxicity, risk assessment, modeling and result in nanogram-per-liter (ng/L) to microgram-per-

liter (µg/L) concentrations in the environment. Many doi:10.2175/106143011X13075599870298 contaminants are increasingly detected because of

———————— improvements in detection methods, and while this is an

1*CDM, 210 25th Avenue North, Suite 1102, Nashville, Tennessee important aspect of advancing the overall understanding

37203; Tel. 615-340-6528; Fax. 931-372-6346; e-mail: emerging pollutants, analytical methods are described in [email protected] other venues and are not included in this review unless 2Midway College School of Pharmacy, Paintsville, Kentucky specific information on occurrence, fate and transport,

3CDM, Inc., Maitland, Florida treatment, modeling, and/or toxicity/risk assessment are

also provided. Further, release of pharmaceuticals from 4HDR Inc., Tampa, Florida manufacturing facilities is regulated in the United States

5Texas Tech University, Lubbock, Texas (US) and is not a major contributor of these constituents to

the environment in this country; therefore, research 6Jeff Bandy, Carollo Engineers, Boise, Idaho conducted in those facilities is not included in this review

unless there is information that is directly applicable to

treatment of municipal water or wastewater.

1906 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Related to the occurrence of emerging pollutants wastewater, surface water, and groundwater issues; in the environment, reviews and opinion pieces, including however, selected topics related to drinking water and editorials or letters to the editor, were published in drinking water treatment methodologies that might be scientific journals in 2010, such as the editorial by Fatta- applied to wastewater are included.

Kassinos and Ledin (2010), Shrivastava, et al. (2010), Research on the topic of emerging pollutants

Ternes and von Gunten (2010), and Snyder and Benotti continues to advance, in part, because of the ability to

(2010). These documents provide overviews and focus detect these compounds. There is a growing body of attention on current and future needs for research, information on analytical methods related to this topic and particularly for manufactured chemicals, active while it is not specifically part of this review, it is worth pharmaceutical ingredients including steroids and mentioning some of the important reviews on this topic hormones (Pal, et al., 2010), illicit drugs (Huerta-Fontela et such as that by Wu, et al. (2010) who provided a review on al., 2010; Liu et al., 2010) and nanomaterials (Yan et al., the analysis of emerging contaminants in aquatic

2010). Selected contributions of interest to practitioners and environment. Richardson (2010) also published a biennial researchers are noted here such as the information review of developments in environmental mass presented by Benotti, et al. (2010) who reviewed historical spectrometry for analyses of emerging environmental water quality data from Lake Mead showing that even contaminants covering the period of 2008 and 2009, noting climatic conditions, such as drought can impact the that crystals formed by the combination of melamine and concentration of EDCs and PPCPs in the environment. cyanuric acid are contaminants on the horizon. Krauss, et

In This Journal, the previous topical review of the al. (2010) reviewed the environmental analysis of polar literature on Emerging Pollutants appeared last year (Wells micropollutants—from target analysis to suspects screening et al., 2010), in conjunction with associated reviews on to non-target screening. Petrovic, et al. (2010) presented an microconstituents including Detection, Occurrence, and overview of the determination of trace organic

Fate of Pharmaceuticals and Steroidal Hormones in contaminants in environmental samples concentrating on

Agricultural Environments (Snow et al., 2010); Membrane five groups of emerging contaminants including

Processes (Pellegrin et al., 2010); Activated Sludge and pharmaceuticals, drugs of abuse, polar pesticides,

Other Aerobic Suspended Culture Processes (Schmit et al., perflorinated compounds and nanoparticles. And, Daghir

2010); Effects of Pollution on Freshwater Organisms and Markuszewski (2010) provided an extensive review of

(Harmon et al., 2010); and the Fate of Environmental methods that could be used to detect illicit drugs in various

Pollutants (Darnault and Köken, 2010). Health Effects sample matrices. Svobodova and Cajthaml (2010) reviewed

Associated with Wastewater Treatment, Reuse, and upgrades on reporter genes assays performed in the last

Disposal (Ikehata et al., 2010). This review concentrates on decade and found that improvements had increased both the

1907 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation speed and accuracy of the tests which now represent a high (diazinon, methoxychlor, and dieldrin), and PPCPs (17α- throughput system for screening chemicals for hormonal ethinylstradiol, carbamazepine, 17β-estradiol, diethyl activity. toluamide [DEET], triclosan, acetaminophen and estrone)

Researchers have also made strides in developing because they occur frequently in the freshwater perspective on the issues of emerging pollutants with environment and pose a human health hazard at respect to understanding the public awareness of managing environmental concentrations. Rodriguez-Mozaz, et al. pharmaceutical disposal (Leal, et al., 2010) conducted a (2010) also presented discussions from the Environmental literature review and developed a public awareness survey. Health Summit in November 2008, including the source,

Results of the survey showed that there is a need to develop fate, and transport of pharmaceuticals, their exposure more public awareness of pharmaceuticals in the effects and potential risks to human and ecosystems, and environment and that educational efforts focused on proper best management practices to address these issues. disposal of medications are essential in helping to reduce Recommendations placed emphasis on research needs as drinking water contamination. And, once these compounds well as education, communication, prevention and are in the environment, Stanford, et al. (2010) provided a intervention programs, and other public health solutions. review of wastewater-derived EDCs and PPCPs in drinking waters in the US and highlights the uncertainty of what Sampling, Screening and Monitoring risk, if any, the presence of trace-level concentrations of As noted, this review does not include a these compounds poses as well as the need to consider the comprehensive review of analytical methods for measuring cost the public is willing to bear to pay for potentially emerging pollutants. However, there is information on costly mitigation efforts with regard to importance of EDCs sampling and monitoring techniques that directly impact and PPCPs in surface waters and drinking water relative to the results reported in studies on this topic. Thus, research other public health and environmental concerns. Additional on the topic of environmental sampling and monitoring as research on trace pollutants and emerging contaminants in they are related to research on defining the environmental freshwater was prioritized in a review published by Murray occurrence, fate, transport and risk are included here. et al. (2010) who examined literature on the occurrence, Sampling for PPCPs and illicit drugs in sewers use, and toxicity of 71 individual compounds classified into and wastewater treatment plant (WWTP) influents is three broad classes of chemicals—industrials, pesticides, mostly carried out according to existing tradition or and PPCPs. They concluded that the highest priority standard laboratory protocols as reported by Ort, et al. pollutants for regulation and treatment should include (2010c) in an analysis of 87 peer-reviewed journal articles. industrials (perfluorooctanoic acid, perfluorooctanic They concluded that it is unclear for the majority of sulfonate, and di(2-ethylhexyl)phthalate), pesticides reviewed studies whether observed variations can be

1908 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation attributed to “real” variations or if they simply reflect pharmaceutical POCIS. Endocrine disrupting compounds sampling artifacts. While there are challenges associated (EDCs) can also be sampled in water at a drinking water with measuring the variable and low concentrations of treatment plant using POCISs (Magi, et al., 2010) enabling emerging pollutants in environmental samples, there have the detection of low concentrations of bisphenol A, 4-n- been significant advances in sampling methods for this nonylphenol, and estrone to be measured in the inlet; in this purpose. For example, Grabic, et al. (2010) used polar study, none of the EDCs evaluated were detected in the organic chemical integrative samplers (POCISs) to monitor outlet of the plant, indicating their removal by the water

EDCs, pharmaceuticals and other micropollutants in two treatment plant. Others have presented assessment of rivers in the Czech Republic which allowed researchers to critical issues in experimental design, data interpretation determine that the wastewater entering the rivers had high and field application of passive samplers for hydrophobic concentrations of pharmaceuticals such as carbamazepine organic compounds in water (Prokes, et al., 2010). and diclofenac, but was not a major contributor of EDCs to To track sources of emerging pollutants in the the system. Other researchers (Li, et al., 2010a) have shown environment, gadolinium, a rare earth element that is used that water temperature and flow influence POCIS uptake as a contrasting agent in magnetic resonance imaging has rates, but these effects are relatively small and thus, under a been proposed as a conservative tracer. Verplanck, et al. narrow range of water temperatures and flows, it may not (2010) evaluated the behavior of gadolinium, through four be necessary to adjust the chemical-specific sampling rates full-scale metropolitan WWTPs that utilize several for POCIS. Demonstration of this finding was confirmed biosolids thickening, conditioning, stabilization, and by application of the chemical-specific sampling rates to dewatering processing technologies and showed that the

POCIS deployed for one month in Lake Ontario, Canada, organically complexed compound is stable in aquatic during the summers of 2006 and 2008 which yielded systems and is not sorbed to biosolids, thus, it has the estimates of PPCP and EDC concentrations that were potential to be utilized as a conservative tracer in WWTP. consistent with conventional concentration measurements While conservative tracers can be used for source of these compounds. Li et al. (2010b) did additional work tracking, screening tools are also valuable for quickly and to evaluate the influence of water flow rate on the uptake of inexpensively developing information. Veiga, et al. (2010) contaminants into POCISs with flow controlled field evaluated a multi-walled carbon nanotube, film-coated experiments in channel systems through which treated glassy carbon electrode for the voltammetric determination sewage effluent flowed at rates between 2.6 and 37 cm/s. of carbamazepine. The results showed that this simple

Results showed that pesticide POCIS had higher uptake modified electrode exhibited excellent electrocatalytic rates for PPCPs and EDCs than the pharmaceutical POCIS, activity towards the oxidation of this compound lending the but there are some practical advantages to using method to potential use as a measurement method for

1909 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation carbamazepine. Other analytical methods have been PXR-active chemicals in wastewater samples. They developed to separately determine acetaminophen and detected potent PXR activity in samples from a river

Phase II metabolites, acetaminophen glucuronide and moderately impacted by agricultural and urban inputs and acetaminophen sulfate, from wastewater in a single extract three effluents from sewage treatment works. Ericson

(Sunkara, et al., 2010). The method developed can serve as (2010) compared the results of test method, OECD 301B, a model for screening for the presence of other non- with that of OECD 314B for activated sludge steroidal pharmaceutical compounds and their Phase II biodegradation for five Pfizer drug substances. The use of metabolites in wastewater. Williams, et al. (2010) this new method (OECD 314) as an alternative to OECD employed an isotope exchange technique using radio- 301B would strengthen the fate testing screen in Phase II labeled carbamazepine as a model compound, to determine Tier A of the European Medical Agency environmental risk the amount of isotopic exchangeability of the compound in assessment as well as providing a characterization of a river sediment. This study demonstrates the availability of a substance’s potential for biotransformation and relatively quick and simple alternative to batch desorption mineralization during sewage treatment and a means for techniques for the assessment of the available fraction of revising predicted environmental concentration of surface organic compounds in sediments following their release water for amount removed during sewage treatment. Gust, into aquatic ecosystems. et al. (2010) developed an in situ exposure method using

Biochemical and biological screening tools are the New Zealand mudsnail to assess the impact of surface also discussed in recent literature. Reporter cell lines have water quality on its reproduction. The method detected been used to detect the activity of estrogen, androgen, significant impairment of the life traits of snails when pregnane X, glucocorticoid, progesterone, mineralo- exposed downstream of discharges that were correlated to corticoid, and aryl hydrocarbon receptors in samples from modulations of steroid levels in the river.

Tunisian WWTPs. Mnif, et al. (2010) characterized the There are many new monitoring strategies and endocrine-disrupting activity of the aqueous, suspended practices that have to be designed to monitor polluting particulate matter, and sludge fractions showing that the substances discharged into the aquatic environment, aqueous fraction exhibited estrogenic and androgenic including priority substances or emerging pollutants that activities; suspended particulate matter and sludge extracts might be present at low concentrations. Graveline, et al. showed estrogenic, aryl hydrocarbon and pregnane X (2010) reported on screening and monitoring emerging receptor (PXR) activities. Creusot et al. (2010) assessed the tools (SMETs) that allow users to conduct quick on-site or use of human PXR as a sensor for aquatic emerging in situ measurements, saving time and allowing the pollutants and employed an in vitro reporter gene assay to acquisition of a larger number of observations. However, screen a panel of environmental chemicals and to assess extensive adoption of SMETs by European Union (EU)

1910 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation water monitoring stakeholders is not expected to take place Europe and the Middle East. Research on in a short time period due to the costs of implementation. occurrence of emerging contaminants in Spain is prolific

with reports on the topic in Portugal also being frequent.

Occurrence Surveys Nine sulfonamides and one acetylated metabolite were

The occurrence of emerging contaminants monitored in the Llobregat and Anoia Rivers in Catalonia continues to be a primary subject of investigation with Spain by Garcia-Galan, et al. (2010). Concentrations surveys being conducted worldwide. In fact, there is ranged from 0.74 ng/L (sulfamethizole) to 2,482 ng/L enough literature available that Fictorie (2010) provided a (sulfamethazine) in the Llobregat River, and from 0.27

Book Review of the occurrence and fate of PPCPs in the ng/L (sulfamethizole) to 168 ng/L (sulfamethoxazole) in environment Monteiro and Boxall (2010) also provided a the Anoia River. Sulfamethoxazole and sulfapyridine were review on the occurrence and fate of human the most frequently detected sulfonamides (80% and 71%, pharmaceuticals in the environment. Boles et al. (2010) respectively). N4-acetylsulfamethazine was detected in both provided a review of the identification and quantitation of rivers—in 4% of the samples from the Anoia River and the non-ecstasy amphetamine-type stimulants (ATSs) 43% of those from the Llobregat River. Concentrations amphetamine and methamphetamine in lakes, rivers, were not usually higher than 50 ng/L; however, in some wastewater treatment plant influents, effluents, and cases, near the mouth of the Llobregat River, biosolids. Zhang and Geißen (2010) conducted a review of concentrations were greater than 5,000 ng/L. Gomez, et al. carbamazepine concentrations in the WWTP effluents in 68 (2010) developed an analytical method for a rapid countries/regions and developed a predictive model based screening and confirmation of a large number of organic on the sale volume, the water consumption, the disposal microcontaminants (almost 400) in surface and wastewater rate, the excretion rate, and the removal efficiency by the in Spain. The method has been applied revealing that most sewage systems. The prediction results demonstrated that of the pharmaceutically active compounds detected were there is global aquatic contamination by this compound present at ng/L and µg/L concentrations, and in most of the with most of developed economies having a concentration samples between 2 and 15 pesticides were also detected. greater than 500 ng/L. There have also been numerous Additionally, some degradation products were found, occurrence studies of emerging pollutants in the liquid demonstrating the method as a useful screening tool for the phase that can be presented by region where the occurrence analysis of organic microcontaminants in water. A has been documented using both newly developed and comparison of passive sampling techniques relative to spot established analytical methods; a summary of the findings sampling by Kuster, et al. (2010) in field trials from those reports is provided here, by region. demonstrated the detection of estriol using passive

sampling that was not identified with spot sampling.

1911 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Irrigation channels near Barcelona, Spain were sampled Teijon, et al. (2010) conducted a monitoring and results showed that some of the most environmentally survey of water samples from a tertiary WWTP (Depurbaix relevant estrogens—estradiol, estrone, estriol, ethynyl – Barcelona, Spain), treated waste water with an additional estradiol, estrone sulphate and estradiol glucuronide were treatment of ultrafiltration, reverse osmosis, and ultraviolet detected with the passive sampling device which were not (UV) irradiation disinfection. Groundwater samples from detected by grab sampling at these locations. the aquifer receiving recharge were also analyzed. The

Bueno, et al. (2010) reported on the presence of pharmaceutical group of substances was detected in

88 contaminants belonging to several chemical groups sampled waters at concentrations rarely exceeding a few

(PPCPs, disinfectants, and pesticides) in rivers near μg/L, among the compounds caffeine, nicotine and

Madrid, Spain; results were used to classify contaminants galaxolide (musk fragrance) were found to be present in into two categories: emergent or priority pollutants. more than 60% of the samples; diuron was the only priority

Camacho-Munoz, et al. (2010a) conducted a study in substance detected. Alonso, et al. (2010) studied the

Donana Park (South of Spain) watersheds showing that occurrence of psychoactive pharmaceuticals in the primary pharmaceuticals, as water pollutants, are continually rivers of the metropolitan area of Madrid, Spain—one of discharged into Donana waterbodies; wastewater treatment the most densely populated areas in Europe. Sampling was implemented in the area are insufficient to remove conducted upstream and downstream of WWTPs. Residues pharmaceuticals, and a requirement for better wastewater of the antidepressants fluoxetine were observed at 80% of treatments is needed to reduce pharmaceutical active the sampling sites, citalopram at 60%, and venlafaxine at compounds in the environment. López-Roldán et al. (2010) 100%; the anxiolytics nordiazepam at 90%, oxazepam at investigated the occurrence of 28 pharmaceuticals and 10 80%, and 7-aminoflunitrazepam at 10%; and the estrogens in waters from the lower part of the Llobregat anticonvulsant carabamazepine at 70%.

River basin, the main source of drinking water for Jonkers, et al. (2010) studied the occurrence and

Barcelona (Spain). The same mass of water was monitored sources of phenolic EDCs in this Ria de Aveiro (Portugal). on its way down the river to reflect inputs from discharges, All the studied phenolic EDCs were detected in the study contribution from subsidiaries plus persistence of the area, with high levels found in some of the rivers compounds in the surface water with results showing that discharging into the lagoon, and generally low concentrations of target compounds increased along the concentrations in the lagoon itself. Madureira, et al. (2010) river flow. Gonzalez, et al. (2010) also reported on the quantified pharmaceutical compounds in the Douro River occurrence of psychoactive pharmaceuticals of rivers in the estuary (Portugal) showing that carbamazepine was the metropolitan areas near Madrid (Spain). most ubiquitous compound and the one quantified at the

highest concentration and at all sampling sites. The spatial

1912 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation distribution of the pharmaceuticals along the Douro River can be present at significant levels in the aquatic estuary showed an overall trend of higher concentrations in environment as demonstrated by analysis of drainage, river, the most urbanized areas. Salgado, et al. (2010) studied 65 and WWTP effluent water from sites in Switzerland.

PPCPs in five WWTPs in Portugal. The pharmaceutically Morasch et al. (2010) monitored the concentrations of 58 active compound concentrations detected were in the range pharmaceuticals, EDCs, corrosion inhibitors, biocides and of 0.050—100 µg/L in the influent and up to 50 µg/L in the pesticides in a WWTP and Viday Bay of Lake Geneva. effluent. The non-steroidal anti-inflammatory drugs The experimental results were compared to the results

(NSAIDs) were most abundant (particularly ibuprofen) and predicted by the framework presented in Perazzolo et al. frequently detected. Some musks were detected up to 11.5 (2010). The measured concentrations were greater than the

µg/L in the influent and 0.9 µg/L in the effluent, and in the predicted concentrations, which could be because the sludge up to 22.6 µg/g. The antihypertensives (particularly predicted occurrence is based on sales information. enalapril), caffeine, and clofibric acid were also present in Additional work in northern Europe with respect relatively high concentrations in the influent and effluent. to understanding the overall fate and transport of emerging

Additional research in northern Europe has also pollutants includes work by Varga et al. (2010) who been reported using new and previously developed measured selected acidic pharmaceuticals from water and analytical methods. An analytical method was developed sediment along the Danube River at Budapest (Hungary). by Prasse, et al. (2010) for the determination of nine According to results, concentration ratios of the two phases antiviral drugs and one active metabolite in raw and treated linearly depended on the total organic carbon content wastewater, as well as in surface water. Concentrations in (TOC) of the sediments at each sampling date. Further, the Hessian Ried, Germany, were in the lower ng/L range, Magner, et al. (2010) evaluated 10 pharmaceuticals in with a maximum of 190 and 170 ng/L for acyclovir and surface water close to the effluent of a WWTP and along a zidovudine, respectively. Ratios of oseltamivir to coastal gradient from a WWTP effluent near the central bay oseltamivir carboxylate were approximately a factor of 10 of Stockholm. Four pharmaceuticals revealed different higher for the Rhine than for the other rivers and streams migration patterns along the gradient. ter Laak et al. (2010) indicating a significant contribution from other sources calculated annual loads of pharmaceuticals transported by such as discharges from manufacturing facilities. the Rhine at Lobith from measured pharmaceutical

Schenzel et al. (2010) had previously developed concentrations, and compared this to the annual sales detection methods for two mycotoxins, naturally occurring upstream of Lobith. This mass balance approach shows that secondary metabolites of fungi colonizing agricultural substantial fractions of the 20 most frequently observed products on the field or during storage, and shown that two pharmaceuticals sold in the Rhine catchment area are common mycotoxins, i.e., zearalenone and deoxynivalenol, recovered in the Rhine at Lobith.

1913 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Among all EU member countries, Cyprus is In Jordan, Alahmad and Alawi (2010) monitored currently the leading country in antibiotic consumption and effluent and influent from WWTPs and found that the is likely to have a high consumption of pharmaceuticals treatment technologies used at these facilities were not overall. Thus, Makris and Snyder (2010) conducted a proficient at removal of several pharmaceutically active reconnaissance project to investigate the occurrence of 16 compounds that were reported at concentrations that were pharmaceuticals, six known or suspected EDCs, two flame much higher than for similar facilities in Europe. retardants, one insect repellant, and one fragrance in water North America. Because there are already supplies of Cyprus. Groundwater samples from sites that numerous reports in the literature on the occurrence of were located beneath farms scattered around Cyprus, emerging pollutants in various regions of North America, wastewater influent and tertiary-treated effluent, raw and researchers are beginning to summarize this information to finished surface water, and household potable water more clearly define the distribution of these compounds. samples were analyzed. Most of the tested compounds were For example, Wiener and Sandheinrich (2010) synthesized at minimum reporting limit, except for ibuprofen (mean of a great deal of information that has been previously

1.4 ng/L) and bisphenol A (mean of 50 ng/L), which were collected on selected contaminants in the Upper Mississippi detected in more than one out of the five groundwater River, summarized regulatory measures enacted to reduce sampling sites. Certain compounds were found in large pollution, and described biotic and ecosystem responses to concentrations in the wastewater influent (caffeine 82,000 regulatory actions. The river receives hundreds of recently ng/L, sulfamethoxazole 240 ng/L, ibuprofen 4,300 ng/L, synthesized chemicals, and the behavior and effects of most and triclosan 480 ng/L). Further, in inland waters and of these compounds in aquatic ecosystems are largely wastewaters discharged in the area of Thermaikos Gulf, unknown. Klecka, et al. (2010) presented an analysis of

Thessaloniki, Northern Greece, Arditsoglou and Voutsa exposure to chemicals of emerging concern in the Great

(2010) studied the occurrence and distribution of phenolic Lakes Basin based on existing data. Dougherty, et al. and steroid EDCs. Results revealed the presence of (2010) reported on the occurrence of herbicides and PPCPs phenolic EDCs in all water and wastewater samples but in surface water and groundwater around Liberty Bay, steroid EDCs were not detected. Concentrations of EDCs Puget Sound, Washington. Further, evaluations of were similar to minimally impacted surface waters concentration of wastewater contaminants including worldwide, but concentrations for nonylphenol and pharmaceuticals and EDCs in Lake Mead, a raw water octylphenol occasionally were above proposed quality supply, and inflows to the lake showed that deterioration of standards, revealing the impact of urban, industrial, and the water supply quality was due to the decrease in volume agricultural activities. of the lake which has been attributed to drought (Benotti, et

al., 2010). MacLeod and Wong (2010) did a comparison of

1914 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation time-weighted average pharmaceutical concentrations, Schulz, et al. (2010) conducted a study of loadings and enantiomer fractions among treated antidepressant pharmaceuticals in two US effluent- wastewater from one rural aerated lagoon and from two impacted streams and documented the occurrence and fate urban tertiary WWTPs in Alberta, Canada. Their results of the target compounds in water and sediment. indicate that measured loadings, weighted by population Researchers also conducted an evaluation to assess the served by WWTPs, are a good predictor of other effluent selective uptake in fish neural tissue. concentrations, even among different treatment types. Asia. Occurrence studies of emerging pollutants

There is also ongoing research to broaden the in Asia are rapidly growing in the literature from understanding of the sources, fate and transport of these researchers using both newly developed and established compounds throughout North and South America. For analytical methods. Zhao, et al. (2010) analyzed for 10 example, Singh, et al. (2010) evaluated the occurrence and NSAIDs, 2 blood lipid regulators, and 2 antiepileptic drugs distribution of 15 hormones, steroids and selected in the Pearl River system in China (i.e., Liuxi, Zhujiang, micropollutants in the Florida Keys. Researchers observed and Shijin Rivers) and four sewage effluents during the dry significant correlations between estrone and caffeine and and wet seasons, results were reported and the the study showed that localized sewers rather than transport environmental risks they posed were assessed. Yin, et al. affected the concentration levels observed in the study. In (2010) screened river water and tap water in China for the

Canada, the study of two rivers in a south Saskatchewan presence of β-lactam antibiotics. River water samples were basin indicated natural and synthetic organic contaminants collected from three locations, from upstream to with estrogen like activity were detected in every sample downstream, of a drainage river that connects with a analyzed and biological responses demonstrated. The 28 drainage ditch of the pharmaceutical factories located in contaminants monitored successfully identified municipal this area, and receives the effluent from two WWTPs. The wastewater and agricultural inputs into the river (Jeffries, et β-lactam antibiotics were found within the range of 0–9.56 al. 2010). Waiser, et al. (2010) reported on data from the µg/L in river water at the downstream of antibiotics city of Regina, Saskatchewan, Canada (population manufacturers, and none were detected in the tap water.

190,400) which treats its sewage at a modern tertiary Occurrence and fate of selected EDCs were investigated by

WWTP located on Wascana Creek. The continual exposure Zhou, et al. (2010) in three WWTPs in Beijing, China. All to a mixture of pharmaceuticals as well as concentrations of of the EDCs were detected in the influents of all three un-ionized ammonia that far exceed Canadian and WWTPs with bisphenol A being the most abundant

American water quality guidelines suggests that Wascana compound detected; concentrations of EDCs in the WWTP

Creek should be considered an ecosystem at risk. influent and effluent were also reported. In another study,

occurrence and removal of 13 pharmaceuticals and 2

1915 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation consumer products, including antibiotic, antilipidemic, anti- these compounds, except estrogens, doubled or even inflammatory, anti-hypertensive, anticonvulsant, stimulant, greater, compared to day-time levels. insect repellent and antipsychotics were investigated in four Al-Odaini, et al. (2010) developed a method for

WWTPs in Beijing, China (Sui, et al., 2010). Most of the simultaneous determination and quantification of 23 target compounds were detected, with the concentrations of pharmaceuticals and synthetic hormones from different

4.4 – 6.6 milligrams per liter (mg/L) and 2.2 – 320 ng/L in therapeutic classes in water samples and applied the the influents and secondary effluents, respectively. method to river water and WWTP effluents from Malaysia

Concentrations were consistent with their consumptions in with results showing that among target compounds,

China, and much lower than those reported in the US and chlorothiazide was found at the highest level, with

Europe. concentrations reaching up to 865 ng/L in WWTP effluent,

Lin, et al. (2010) simultaneously investigated the and 182 ng/L in river water. occurrence of sixty-one PPCPs using solid phase extraction These studies also elucidate sources of emerging and high-performance liquid chromatography-tandem mass pollutants and potential treatment options for reducing the spectrometry, evaluated removal efficiencies of target concentrations of these compounds to the environment. For

PPCPs in six WWTPs that discharge effluents into major example, Koo, et al. (2010) developed and applied a

Taiwanese rivers, and lastly examined matrix interference method for quantification of ten pharmaceuticals in surface during analysis of target PPCPs in water samples. The water samples from the major rivers in South Korea. twenty target PPCPs were chosen for their high detection Results showed that overall, surface water contamination frequencies, high influent concentrations, and stability near livestock WWTPs was higher than near domestic during wastewater treatment processes. Caffeine and WWTPs. Yoon, et al. (2010) collected samples from acetaminophen were detected at the highest concentrations upstream/downstream and effluent-dominated creeks along

(as high as 24,467 and 33,400 ng/L), but were effectively the Han River, Seoul (South Korea) and examined them for removed through the WWTPs (both 96%); other PPCPs selected emerging pollutants. Most target compounds were were detected in the high ng/L range but were not detected in both the Han River samples (63%) and in the effectively removed. Further, Lin, et al. (2010a, 2010cz) effluent dominated creek samples (79%). Iopromide, identified a method to determine the risk of pharmaceutical atenolol, tris-2-chloroisopropyl phosphate, TECP, musk compounds applied it to ten of the human-use ketone, naproxen, DEET, carbamazepine, caffeine, and pharmaceuticals detected in Taiwan’s Sindian River. benzophenone were frequently detected in both river and

Additionally, they showed that in river water samples, creek samples, although the mean concentrations in

NSAIDs, steroids, propranolol, and gemfibrozil were found effluent-dominated creek samples (102 – 3745 ng/L) were at ng/L to mg/L levels with night-time concentrations of significantly higher than those in river samples (56– 1013

1916 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation ng/L). However, the steroid hormones 17β-estradiol, 17α- With regard to longer time scales, Musolff, et al. ethynylestradiol, progesterone, and testosterone, were not (2010) presented results from a one-year-monitoring detected (< 1 ng/L) in the river or creek samples. Sim, et al. program concerning concentrations of PPCPs and industrial

(2010) studied the occurrence and fate of pharmaceuticals chemicals in an urban drainage catchment in untreated and in WWTPs and rivers in Korea and found that treated wastewater, surface water and groundwater. pharmaceuticals were present; biological processes in the Correlation and principal component analysis revealed a

WWTP showed the greatest efficacy for reducing the pronounced pattern of xenobiotics in the surface water concentration of the pharmaceuticals. Additionally, in samples. Seasonal attenuation is assumed to be a major

Korea, a review of existing environmental data on process influencing the measured concentrations. Dilution polybrominated diphenyl ethers (PBDEs) and synthetic of xenobiotics the surface water was found to significantly musks prompted Kang, et al. (2010) to evaluate exposure influence the concentrations. Sodre, et al. (2010) levels of these pollutants in breast milk, maternal and cord investigated the occurrence of emerging contaminants in blood samples from Korean women. In comparison with drinking water of the city of Campinas, Brazil. Six previous data, higher and gradually increasing emerging contaminants (stigmasterol, cholesterol, concentrations for PBDEs were found in Korean breast bisphenol A, caffeine, estrone, and 17β-estradiol) were milk, although PBDEs concentrations in breast milk were found in the samples. The latter two were detected only lower in younger mothers and/or mothers with multiple during the dry season, with concentrations below parities. quantification limits. Stigmasterol showed the highest

Temporal Variability. Researchers have shown average concentration (0.34 ± 0.13 μg/L), followed by a clear temporal relationship of the presence of emerging cholesterol (0.27 ± 0.07 μg/L), caffeine (0.22 ± 0.06 μg/L), pollutants in various water samples. In some instances, and bisphenol A (0.16 ± 0.03μg/L). Seasonal variations in there are short-term variations and uncertainties associated the concentration profile of four analgesics and one lipid with measurements of loads of PPCPs in sewers and regulator were monitored on their way from a WWTP influents to WWTPs. Ort, et al. (2010a) assessed effluent, along a river, and into a lake (Daneshvar, et al., uncertainties associated with different sampling modes 2010). From December 2007 to December 2008, water when evaluating these compounds and found small scale samples were collected monthly (n=12) from an upstream heterogeneities in the influent stream to a WWTP and point, the effluent, four downstream points of the WWTP, cautioned that sampling intervals of 5 minutes or shorter and at the point where the river merges with the lake, and may be required to properly account for temporal PPCP the concentrations of ibuprofen, naproxen, bezafibrate, variations in influents. diclofenac, and ketoprofen were determined. The target

pharmaceuticals were found in the effluent at

1917 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation concentrations ranging from 31 to 1,852 ng/L, depending providing source characterization data for healthcare on season, with the mean mass flow of all analgesics being facility wastewaters containing commonly prescribed highest during winter, while the highest mean mass flow of cardiovascular APIs. Lin, et al. (2010b) investigated the the lipid regulator bezafibrate was observed in spring. occurrence of controlled drugs in two rivers, two WWTPs

and five hospital effluents in Taipei, Taiwan and of the

Sources target drugs, morphine, codeine, methamphetamines and

Along with defining the widespread occurrence ketamine were observed in significant quantities in hospital of emerging pollutants, there has also been a great deal of effluents. High concentrations of methamphetamine, work conducted to characterize the importance of various codeine and ketamine were also found in surface waters. sources of these compounds. A summary of the literature Because hospitals could directly be potential sources of focused on some of these sources is provided here. pharmaceuticals to the environment, Kosma, et al. (2010)

Hospital Wastewater Discharge. With research investigated the residues of 11 PPCPs in municipal and on emerging pollutants including pharmaceuticals, hospital WWTPs in Ioannina, Greece; they showed that 11 understanding the role of hospital wastewater to the compounds had higher removal efficiencies in the environment is an important topic. There have been a municipal WWTPs than in the hospital WWTPs. Verlicchi, number of studies documenting the occurrence of various et al. (2010) conducted a review to compare characteristics pharmaceuticals in treated and untreated hospital of hospital effluents and urban wastewaters. Additionally, wastewater effluent to understand the contribution to they evaluated treatment processes and provided

WWTPs and the environment. Methotrexate, azathioprine, recommendations for the most appropriate treatment for cyclophosphamide, ifosfamide and etoposide were detected hospital wastewater, concluding that there is a preferred in wastewater primarily from large hospitals and cancer sequence to provide a separate treatment to avoid dilution hospitals specializing in cancer treatment in China, due to mixing with urban sewage for cotreatment. suggesting that the hospital effluents are an important Additionally, biological treatment is necessary to remove source of certain cytostatic drugs (Yin, et al., 2010b). organic load and longer SRTs and high concentrations of

Nagarnaik, et al. (2010) reported on the composition and the biomass in the biological tanks favor all the magnitude of sixteen cardiovascular active pharmaceutical biodegradation processes. Ultrafiltration membrane ingredients (APIs) and two cardiovascular API metabolites technology seems to be a promising means for removal of in wastewater effluents from a hospital, nursing care, pharmaceuticals and ozonation. AOPs are also promising assisted living, and independent living facilities showing techniques due to the fact that they can react with many that combined loading for all four facilities was 16.2 g per recalcitrant compounds, resulting in a more biodegradable day. This research informs the risk management process by effluent and GAC and PAC can enhance the removal of

1918 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation many pharmaceuticals. Conversely, Ort, et al. (2010b) obtained from WWTP effluents proved that these “dual- presented data regarding the contribution of use-drugs”, with the exception of hydrochlorothiazide, pharmaceuticals from a hospital to a WWTP and their were mostly eliminated in the WWTP. In another study, measurements provided clear evidence that, for 28 of 59 cocaine, benzoylecgonine, morphine, methadone and its investigated substances, over 85% of the pharmaceutical main metabolite 2-ethylidene-1,5-dimethyl-3,3- residue loads did not originate from the hospital. Only two diphenylpyrrolidine have been measured in WWTP compounds, trimethoprim and roxithromycin, showed that influents and effluents by Berset, et al. (2010). River and the maximum observed contribution was from the hospital lake water were determined to contain trace amounts of was only for 2 substances. these compounds from the high pg/L to the low ng/L level.

Illicit Drugs and Municipal Sewage. Research Time series monitoring of illicit drug concentrations in on illicit drugs has been conducted with results showing WWTP influents and effluents suggested a consumption that the presence of these compounds have temporal preference on week-end days and after a major music event patterns that could be used to track use, but also that many which resulted in high influent concentrations of these of these compounds can be attenuated by WWTPs. compounds. Similarly, Terzic, et al. (2010) applied a

Metcalfe, et al. (2010) investigated the illicit drugs, wastewater analysis technique to monitor drug use patterns including cocaine and its major metabolites for illicit drugs and 2 common therapeutic opiates in benzoylicgonine (BE), amphetamine, methamphetamine Croatia. They found that wastewater analysis could observe and ecstasy, in three Canadian cities WWTPs. Cocaine was daily variations in use even at low mass loading, which the most widely used illicit drug at a median level for the 3 corresponded to low concentration and low frequency. As cities of 15.7 doses per day per 1000 people. For the other such, Verster (2010) provided an editorial suggesting that drugs, the median doses per day per 1000 people were 1.8 wastewater and air measurements could be used to detect for amphetamine, 4.5 for methamphetamine and 0.4 for illicit drug use in smaller communities such as drug ecstasy. Methamphetamine use was highest in the largest rehabilitation centers, hospitals, prisons, military city and cocaine use was lowest in the smallest city. compounds and schools. Castiglioni and Zuccato (2010)

Removal of the illicit drugs by wastewater treatment was also reported on illicit drugs in the environment as generally greater than 50% except in a WWTP that uses indicators of drug abuse. Karolak, et al. (2010) estimated primary treatment. Fr. Schroeder, et al. (2010) analyzed for the consumption of illicit drugs in the Paris area from the

“dual-use-drugs” applied either as anabolic, doping, and measurement of drug residues in sewage. lifestyle drugs or for treatment of diverse diseases in Municipal WWTP Discharges. It is evident that municipal wastewater. This study identified anabolic and municipal WWTPs are a potential source of emerging doping drugs in wastewater for the first time and results pollutants to the environment. Singer, et al. (2010)

1919 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation evaluated the input of hydrophilic biocides into the aquatic may represent a significant source of concern for legacy, environment and on the efficiency of their removal in new, and emerging chemicals in groundwater. Chemicals conventional wastewater treatment. In samples collected identified in the leachates at ng/L or µg/L concentrations from surface water and WWTPs in Switzerland, average include — chlorinated alkylphosphates such as tris(1- eliminations for all compounds were usually below 50% chloro-2-propyl) phosphate, n-butyl benzensulfonamide, and during rain events, increased amounts of biocidal the insect repellent DEET and personal care products such contaminants are discharged to receiving waters. Also, as the NSAID ibuprofen and polycyclic musk compounds.

Radke, et al. (2010) analyzed short-term dynamics of Among new and emerging contaminants, perfluorinated selected pharmaceuticals along a 13.6 kilometer long river compounds were measured in water at concentrations stretch, downstream of a WWTP, and quantified their exceeding 6,000 ng/L. In another study, Shala and Foster attenuation using a mass balance approach. The temporal (2010) measured pharmaceuticals and domestic-use dynamics were closely related to discharge of the WWTP chemicals in the Anacostia River (Washington, D.C) and and precipitation, and highest concentrations were observed found that concentrations were higher than expected based at the beginning of a discharge event. Dunlavey, et al. on concentrations in upstream WWTP effluents.

(2010) also discussed the fate and transport of EDCs and Additionally, concentrations these compounds were similar

PPCPs in the San Jose/Santa Clara, California Water in the northeast and northwest branches of the Anacostia

Pollution Control Facility and recommended additional River even though the NW Branch receives no WWTP analysis and monitoring to support future pollution discharge, calling into question the role of WWTP prevention and source control. discharge as the predominant sources versus the importance

With respect to contributions of pharmaceutical of alternate sources such a septic leaching, aging or leaky compounds, Van De Steen, et al. (2010) showed that sewer conduits, and landfills. pharmaceuticals are present in WWTP effluent when a Other sources, such as stormwater runoff or chemo-pharmaceutical company discharges waste to the wash-off have been identified as sources of emerging

WWTP. Confirming this finding, Phillips, et al. (2010) pollutants. In a simple batch test for measuring pesticide surveyed the effluent of 23 WWTPs across the country and wash-off potential from concrete surfaces, the dependence two rivers receiving WWTP discharge and pharmaceuticals of washable pesticide residues was evaluated on pesticide formulation faculties showing that effluents from these types, formulations, time exposed to outdoor conditions, facilities can increase the concentration of pharmaceuticals and number of washing cycles (Jiang et al., 2010). After entering aquatic environments. application to concrete, the washable fraction of four

Landfill Leachate and Other Sources. Eggen, pyrethroids and fipronil rapidly decreased, but the initial et al. (2010) demonstrated that municipal landfill leachates fast decrease was followed by a much slower declining

1920 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation phase with half-lives ranging from one week to two four irrigated plots in Guangzhou in southern China. Six months, and detectable residues were still found in the compounds including bisphenol-A, 4-nonylphenol, wash-off solution for most treatments after 112 days. triclosan, tric1ocarban, salicylic acid and c1ofibric acid

Breton, et al. also conducted research reporting the were detected with 4-nonylphenol having the highest contributions of car, truck, bus and subway wash station concentrations in both soils and irrigation water. Citluski discharges to stormwater pollution. and Farahbakhsh (2010) reviewed the fate of EDCs during

Soil and Land Application. When treated municipal biosolids stabilization, particularly using wastewater or biosolids are applied to soil, there is a bioassay approaches to help reduce public opposition and concern regarding the potential for the emerging pollutants distrust of biosolids reuse applications. They summarized contained in these media to be transferred into other what is currently known regarding EDC removal during environmental media or bioaccumulated through the food commonly used full scale biosolids treatment processes and chain. Nieto et al. (2010a, 2010b) developed a method that highlighted analytical challenges that are relevant when in they used to investigate the presence of hormones and vitro bioassays and chemical analyses are applied to conjugates, and pharmaceuticals that are partially or totally biosolids samples. To further enable the investigation of the removed from the influent wastewater and removed by occurrence and fate of PPCPs in biosolids and soil systems, sorption into the sewage sludge. Sewage sludge from two Wu, et al. (2010a) developed an extraction and analysis

WWTPs in the Tarragona area (Spain) for the period March procedure for 14 compounds, which was evaluated using

2007 until March 2008 were monitored and compounds field study samples. All of the compounds investigated, that showed the highest concentrations in both WWTPs except carbamazepine epoxcide, were found in the were roxithromycin and tylosin. Sorption isotherms with biosolids sample. Guo, et al. (2010) analyzed for polycyclic dewatered biosolids also indicated that tenofovir residues and nitro-musks in dewatered sludge samples and found are most likely partitioned into biosolids during wastewater their concentration ranged from 36 to 10,961 mg/kg. treatment (Al-Rajab, et al., 2010). Researchers have also Hospido, et al. (2010) used a life cycle assessment to shown that the fate of some pharmaceuticals in biosolids evaluate the reuse of anaerobically digested sludge in and solids from physical/chemical treatment processes is agricultural land relative to impacts caused by emerging related to factors such as pH, which play a significant role micropllutants and showed that differing operational in treatment (Kimura, et al. 2010). conditions applied during the anaerobic digestion process

Ultimately, emerging compounds can end up in had different impacts. Among the treatment alternatives soils either through application of the biosolids via studied, those with short SRT generally had a lower impact irrigation. Chen, et al. (2010) developed an analytical than those with longer SRT, but no clear influence of method that they applied to water and soil samples from temperature was noted. Six (galaxolide, tonalide, diazepam,

1921 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation ibuprofen, sulfamethoxazole and 17-α-ethinylestradiol) of perfluorinated compounds in two agricultural top soils;

13 substances considered accounted for more than 95% of they characterized adsorption using linear Freundlich the overall micropollutants impact. isotherms. Variability in sorption characteristics were

Pignatello, et al. (2010) emphasized the role of correlated using the organic carbon normalized sorption soils as sources, sinks and reaction catalysts for coefficient and perfluorinated compound molecular weight. microconstituents in surface and underground water There are many compounds that are partitioned to supplies. They reviewed topics covering novel advances in and disposed with the biosolids from a WWTP; some of analytical techniques, transport of infectious agents, these are readily degraded as reported by Al-Rajab, et al. occurrence and fate of veterinary pharmaceuticals, (2010b) who evaluated the environmental fate of diclofenac characterization of sorption mechanisms, biotic and abiotic through the application of municipal biosolids or transformation reactions, the role of soil components, wastewater indicating that compound is readily occurrence and fate in wastewater treatment systems, biodegradable in agricultural soils. While some compounds transport of engineered nanoparticles, groundwater have been demonstrated to degrade in laboratory studies, contamination resulting from urban runoff and issues in Waltres, et al. (2010) showed in an outdoor mesocosm water reuse. Understanding the critical transfer of emerging study in Baltimore, Maryland, that chemical half-lives pollutants from biosolids to soil media, Barron et al. (2010) determined empirically exceeded those reported from focused on evaluating the transfer of a selection of laboratory studies or predicted from fate models. These pharmaceutical residues from municipal sewage sludge to study results suggest that PPCPs shown in the laboratory to agricultural top soils and their fate therein after an be readily biotransformable can persist in soils for extended accelerated 6-month rainfall event. Twelve pharmaceuticals periods of time when applied in biosolids. This encompassing antibiotics, analgesics, antiinflammatories, phenomenon has been demonstrated by Al-Rajab, et al. beta-blockers, hyperlipidaemics and stimulants were (2010b) who evaluated the persistence of tenofovir in investigated. Results showed the distribution and separation agricultural soils; their experimental work showed that the of pharmaceuticals over a 100 millimeter soil depth, compound is degraded aerobically via a microbial process following typical biosolid application rates. Using with slow kinetics with no transformation products readily experimentally determined solid–water partition detected in samples. coefficients (Kd) and hydrophobicity distribution ratios While biodegradation is often the goal for final

(Dow), mobility and modes of interaction under dynamic treatment of emerging pollutants from biosolids, it may be conditions were discussed. Further, Enevoldsen and Juhler desirable to sequester some compounds such as

(2010) used a fully automated method for characterisation demonstrated by sorption of ciprofloxacin, ofloxacin and of soil adsorption and desorption to evaluate six norfloxacin to a surrogate Louisiana wastewater treatment

1922 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation wetland soil; the slow desorption from these soils provides then reducing their discharge by means of a comprehensive a major and potentially long-term removal pathway for pollution prevention program. The legislation defined a these antibiotics from wastewater (Conkle, et al., 2010). persistent pollutant as one that is toxic and persistent or

Ultimately, emerging pollutants can be taken up bioaccumulative; a broad definition that required evaluation in plants from biosolids, as reported Wu, et al. (2010b), of an extensive number and variety of chemicals. The who conducted a greenhouse experiment to study for three Oregon Department of Environmental Quality, in pharmaceuticals (carbamazepine, diphenhydramine, and consultation with a science workgroup, implemented a 12- fluoxetine) and two personal care products (triclosan and step process for identifying and prioritizing persistent triclocarban) by soybeans, from biosolids. Carbamazepine, pollutants consistent with this definition. And, while source triclosan, and triclocarban were found to be concentrated in control would be one of the most cost-effective methods for root tissues and translocated into above ground parts controlling the introduction of emerging pollutants to the including beans, whereas accumulation and translocation environment, there is continuing research on treatment for diphenhydramine and fluoxetine was limited. Because methods to address these compounds. A summary of a these compounds can be taken up in plants, there are also range of treatment methods that have recently been concenrns regarding impacts on higher organisms. investigated is provided.

Khalvati, et al. (2010) also reported on the influence of Onsite and Subsurface Treatment Systems. sewage sludge on bioavailility of plant matter to livestock Onsite wastewater treatment systems (OWTS) play and other farming uses. Additionally, maternal and fetal important roles in both control and introduction of trace tissue from sheep exposed to pasture treated with either organic and micropollutants in the environment. Conn, et inorganic fertilizer or with sewage sludge containing al. (2010a, 2010b) reported on the occurrence of PPCPs in polybrominated diphenyl ethers showed that exposure was raw wastewater and septic tank effluent from single-family not associated with increased maternal or fetal liver homes and demonstrated that OTWSs can effectively concentrations of selected EDCs, irrespective of the stage remove trace organics through sorption and of development at which they were measured and of biotransformation. However, they also reported that maternal tissue mobilization and EDC release during engineered pretreatment for soil treatment systems may not gestation (Rhind, et al., 2010). provide improvements in removal efficiencies. Katz, et al.

(2010) found that most organic wastewater compounds and

Source Control and Treatment pharmaceuticals were highly attenuated beneath septic tank

Hope, et al. (2010) reported on the 2007 State of drainfields overlying a karst aquifer. However, there were 5

Oregon enacted legislation aimed at identifying persistent wastewater compounds (caffeine, 1,7-dimethylxanthine, pollutants that could pose a threat to waters of the State and phenol, galaxolide, and tris(dichloroisotopropyl)phosphate)

1923 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation and 2 pharmaceutical compounds (acetaminophen and carbamazepine and clofibric acid, respectively, achieved sulfamethoxazole) detected in groundwater samples. under summer conditions after a retention time of 7 days

The sources, presence and potential fate of a with a fast adsorption step being followed by gradual selection of xenobiotic micropollutants in on-site greywater uptake of pharmaceuticals. Reinhold, et al. (2010) reported treatment systems were investigated by Donner, et al. on constructed treatment wetlands and demonstrated that

(2010). The authors presented the current state of they have the potential to reclaim wastewaters through knowledge with respect to the presence in greywater of removal of trace concentrations of emerging organic selected chemicals. Geochemical modeling results pollutants, including PPCPs and pesticides. The study indicated that removal during treatment is predominantly demonstrated that aquatic plants contributed both directly due to sludge/solid phase adsorption and therefore and indirectly to the aqueous depletion of emerging organic greywater treatment systems which periodically discharge pollutants through both active and passive processes. The sludge to sewers will be of limited benefit in terms of capacity of a horizontal subsurface flow constructed comprehensive source control. wetland system to remove emerging pollutants was

Wetlands and Natural Systems. Constructed investigated by Avila, et al. (2010) and the authors used a wetlands and other natural treatment systems such as bank continuous injection experiment to evaluate ibuprofen, filtration are attractive methods for treatment of emerging naproxen, diclofenac, tonalide, and bisphenol A removal. pollutants for aesthetics, cost of operation and removal The treatment system consisted of an anaerobic reactor as a efficiencies. Yan, et al. (2010) described the main primary treatment, followed by two wetlands working in categories and properties of emerging contaminants, as well parallel and connected to a third wetland operating in series as their occurrences and behavior, fate, and transport in and overall removal efficiencies ranged from 97% to 99%. natural and engineered systems. The fate of nanomaterials As with more highly engineered systems, researchers have in different environmental compartments, as well as their found that both sorption and biodegradation are important effects on human health and other fauna were also to the estrogens removal from algae or duckweed pond presented. Hijosa-Valsero, et al. (2010a, 2010b) conducted systems for wastewater treatment (Shi, et al., 2010). Other a comprehensive assessment of the design configuration for work by Maeng, et al. (2010) who analyzed a constructed wetlands with a focus on removal of PPCPs comprehensive database of organic micropollutants at bank from urban wastewaters and evaluated the performance of filtration and artificial recharge sites located near Lake full-scale of these natural systems for in small Tegel in Berlin (Germany) showed, through a principle communities. And, Dordio, et al. (2010) showed that components analysis, that redox conditions and degradation constructed wetland treatment of wastewaters showed potential with temperature to be the most important factors removal efficiencies of 96%, 97% and 75% for ibuprofen, in removal of these compounds.

1924 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Conventional Biological Treatment Processes. of SRT with respect to their sorption and biodegradation.

It is well known that conventional wastewater treatment The sorption affinity of target compounds was not affected processes will attenuate at least some emerging pollutants. by SRT, with the exception of 4-n-nonylphenol for which

And, in fact, Omil et al. (2010) published an overview of higher values of sorption coefficients were calculated at criteria for designing WWTPs for enhanced removal of SRT of 3 days. organic micropollutants. Physico-chemical properties and While in-vitro recombinant yeast bioassays biodegradability of representative compounds were showed that wastewater treatment via primary and discussed in the review with the primary removal secondary processes successfully reduced up to 80% the mechanisms of most pollutants occurring commonly in estrogenic, anti-androgenic, anti-progesteronic, and anti- primary or secondary treatment processes which provide thyroidic activities of the wastewater (Li, et al., 2010c), sorption, biodegradation and chemical transformation of Alahmad and Alawi (2010) measured concentrations of constituents. The review presents a discussion of key drugs in wastewaters from WWTPs and hospital runoff in

WWTP operational factors with guidelines to enhance the Jordan, where the technologies at the three WWTPs removal of micropollutants. Tambosi, et al. (2010b) also sampled were not adequate to completely remove all provided a detailed review of the sources, occurrence, and pharmaceutically active compounds. Maximum treatability of PPCPs in conventional WWTPs. concentrations for methotrexate, caffeine, glimepiride,

Factors that can improve the removal of ibuprofen and diclofenac were reported along with pollutants in conventional WWTPs include acclimatization treatment efficiencies which ranged from 25 to 100%, of microbial communities to target compounds, such as depending upon the treatment facility. In another study, reported by Khardenavis, et al. (2010); also increased solids Kusk, et al. (2010) investigated the endocrine potency of retention times (SRT) as demonstrated by Gros, et al. wastewater and the removal efficiency of two typical urban

(2010) can improve treatment. In the long term study of Danish sewage WWTPs, using chemical analysis and over 3 years, with total number of 84 samples from seven bioassays. The presence of EDCs was reduced in the

WWTP in the main cities along the Ebro river Basin (North WWTPs but not completely eliminated, suggesting that the

East of Spain), as well as receiving river waters researchers conventional wastewater treatment processes alone are not found that longer retention times at the WWTPs could efficient enough to prevent contamination of environmental result in additional pharmaceutical removals. However, this surface waters. This was confirmed by Kern, et al. (2010) is not the case for every compound. Stasinakis, et al. (2010) who screened for potential biotransformation products of reported on the fate of three EDCs, 4-n-nonylphenol, seven pharmaceuticals (atenolol, bezafibrate, ketoprofen, triclosan and bisphenol A and reported that the removal of metoprolol, ranitidine, valsartan, and venlafaxine) and one these compounds in activated sludge process as a function biocide (carbendazim) in sludge-seeded batch reactors. The

1925 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation 12 transformation products found to form in the batch compound as the sole organic carbon source and each experiments were then found in the effluents of 2 full-scale, compound at a lower concentration (250 μg/L) and municipal WWTPs. cellulose serving as the primary organic carbon source. The

The sorption of hydrophobic micropollutants in change in pharmaceutical concentration was determined sludge is one of the major mechanisms which drive their following 7, 28, 56, and 112 days of anaerobic incubation fate within wastewater treatment systems. The objective of at 37°C. And, while estrogen-degrading microorganisms

Barret, et al. (2010) was to investigate the influence of both have been isolated in WWTPs, their kinetics and sludge and micropollutant characteristics on the equilibria effectiveness are still largely unknown; Roh and Chu of sorption to particles and to dissolved and colloidal (2010) have determined the maximum specific substrate matter (DCM). For this purpose, the equilibrium constants utilization rates and half-velocity constants Shingomonas were measured for 13 polycyclic aromatic hydrocarbons, 5 Strain KC8 growth on 17β-estradiol, estrone and polychlorobiphenyls and the nonylphenol, and five testosterone in WWTPs. different sludge types encountered in treatment systems: a While there is still much to be documented on primary sludge, a secondary sludge, the same secondary microorganisms and their kinetics, there is already data on sludge after thermal treatment, after anaerobic digestion, interactions between toxicity removals and kemicetine and and after both treatments. While the compounds evaluated chemical oxygen demand (COD) removals. Sponza and are not necessarily considered emerging pollutants because Demirden, (2010) evaluated a sequential anaerobic baffled they are all regulated in various environmental media, the reactor/aerobic completely stirred tank reactor system for information regarding their behavior after thermal total COD and kemicetine removal efficiencies. In the treatment, i.e., no more sorption to DCM was observed, is anaerobic ABR reactor, kemicetin was converted to relevant to the behavior of other compounds that are intermediate metabolites and a substantial part of the COD emerging pollutants. Further, in this study, anaerobic was removed. In the aerobic continuously stirred tank biological treatment was shown to enhance micropollutant reactor, the intermetabolites produced in the anaerobic sorption to particles and to DCM of one logarithmic unit, reactor were completely removed and the COD remaining due to matter transformation. from the anaerobic reactor was biodegraded.

Researchers have examined the anaerobic Because biological treatment processes are degradation of 17α-ethynylestradiol, acetaminophen, effective at reducing the concentrations of some emerging acetylsalicylic acid, ibuprofen, metoprolol tartrate, and pollutants, researchers have also conducted studies to progesterone by methanogenic bacteria (Musson, et al., isolate and identify the microorganisms responsible for the

2010). Using direct sample analysis and respirometric degradation of these compounds. Chen, et al. (2010b) testing, anaerobic degradation was examined with each isolated a Gram-negative organism from WWTP sludge

1926 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation capable of using tetrahydrofuran and its intermediate as the approximately two times more oseltamivir was removed in sole carbon and energy source. The strain Pseudomonas bioremediated wastewater than controls. oleovorans DT4 mineralized tetrahydrofuran, which was Membrane Biological Reactors (MBRs). The toxic at concentrations of 200 millimolar. Madukaski, et al. use of membrane bioreactors (MBRs) continues to grow

(2010) identified as Rhodobacter spheaeroides z08, a wild because of the ability of this process to address emerging strain of purple non-sulfur bacteria that was able to degrade contaminants. As an introduction to the advances in this micropollutants in a pharmaceutical plant effluent. Optimal technology, Sipma, et al. (2010) presented a short overview conditions for the anaerobic photoautothrophic bacteria was on the current knowledge of removal of pharmaceuticals in supplementation with 5% ammonium sulfate, 0.1% yeast MBRs compared to conventional activated sludge treatment extract at a pH between 6.6 - 7.0 while incubated for 5 days systems. In general, for slowly degradable pharmaceuticals without shaking. Other researchers (Gauthier, et al., 2010) the removal in MBRs is better due to the relatively long investigated the possible fate of pharmaceuticals in the sludge ages, which leads to the development of distinct environment that are known to be resistant to microbial communities in MBRs compared to activated biodegradation and applied a cometabolism approach, sludge plants. Similar information was summarized in adding a readily degradable carbon source, to study the another review on the fate of metals in wastewater biodegradation of some pharmaceuticals. Rhodococcus treatment by conventional activated sludge processes and rhodochrous, known to co-metabolize difficult to degrade MBRs by Santos and Judd (2010) who reported a slightly hydrocarbons, and Aspergillus niger demonstrated that greater removal was obtained by the MBR process relative cometabolism of carbamazepine, sulfamethizole and to activated sludge processes. sulfamethoxazole could occur and as much as 20% of these There is a great deal of recent research that has compounds could be removed. Accinelli, et al. (2010) documented the overall performance of MBRs compared to evaluated the efficiency of a granular bioplastic other technologies with respect to the removal efficiency formulation entrapping propagules of Pseudomonas for various emerging pollutants. For example, Lamoree et chrysosporium for removal of four selected al. (2010) investigated the removal of natural estrogenic pharmaceuticals from wastewater samples. Addition of hormones for a number of Dutch WWTPs. An important inoculated granules to samples from a WWTP significantly conclusion of this study is that the effluents of conventional increased the removal of the antiviral drug oseltamivir, and treatment only still show a considerable estrogenic activity; the antibiotics, erythromycin, sulfamethoxazol, and to achieve a decrease of the concentrations of the EDCs, ciprofloxacin. Oseltamivir was the most persistent of the MBRs and active coal filtration were shown to be effective. four active substances, but after 30 days of incubation, Xue, et al. (2010) evaluated the occurrence and elimination

of 19 emerging pollutants including EDCs and PPCPs in a

1927 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation full scale anaerobic/anoxic/aerobic-MBR process; the inside of the hollow fibers through the manifold at the base, process achieved over 70% removal of the target EDCs and and the oxygen pressure for both reactors was 13 kiloPascal

50 - 100% removal of most of the PPCPs, with influent (kPa). The decomposition ratio of pharmaceuticals concentration ranging from ng/L to mg/L. Three PPCPs, (sulfamethazine and sulfathiazole) using oxygen based carbamazepine, diclofenac and sulpiride were not well membrane biofilm reactor was: sulfamethazine (77 ± 2%), removed, with the removal efficiency below 20%. And, and sulfathiazole (87 ± 2%). while the treatment of pharmaceutical wastewater is not the While MBR is an excellent treatment technology specific focus of this review, it is worth noting that Shariati, for removal of emerging contaminants, there are et al. has evaluated MBR for treatment of pharmaceutical operational challenges associated with this technology that wastewater containing acetaminophen. impact MBR performance. Dudziak and Bodzek (2010)

Researchers continue to report that the high studied effects of fouling and scaling of membranes on the removal efficiencies in MBRs are a function of the high removal of phytoestrogens—biochanin A, daidzein,

SRT and solids concentrations as shown in a study by Le- genistein, and coumestrol. The decrease in membrane

Minh, et al (2010) where concentrations of several efficiency associated with fouling or scaling brought about micropollutants were assessed in a bench-scale MBR and an increase in the retention coefficient of phytoestrogens conventional activated sludge even though influent during both reverse osmosis and nanofiltration. concentrations were highly variable and the diurnal Phytoestrogen retention was greater for the nanofiltraion samples showed the importance of mixing and dilution in membrane which was more susceptible to fouling that the sewer systems before entering a plant. However, it is also osmotic,c filter. In efforts to understand these challenges, important to note that some investigators that have Avella et al. (2010) evaluated the effect of the evaluated the impact of hydraulic retention time (HRT) and cyclophosphamide and its mean metabolites on influent concentration on MBR performance found that no extracellular polymeric substances (EPS) formation in benefit existed for operating an HRT beyond 15 hours to laboratory MBRs. The presence of CPs induced an increase remove some compounds such as cephalosporin and its in EPS concentration in the biological sludge, especially of intermediates from pharmaceutical wastewater soluble substances, mainly polysaccharides and proteins.

(Sundararman, et al. 2010). More importantly, membrane fouling with CPs was related

Other researchers have investigated specialized to the retention of an increased amount of soluble

MBR systems including Kim, et al. (2010b) who substances. Delgado, et al. (2010) confirmed this with investigated the decomposition of pharmaceuticals results of an investigation on the effect of cytostatic drugs

(sulfamethazine and sulfathiazole) using an oxygen-based on sludge and on mixed liquor characteristics of a cross- membrane biofilm reactor. Pure oxygen was supplied to the flow MBR. They showed that when cyclophosphamide was

1928 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation present the physicochemical properties of the mixed liquor levels of treatment. Beier, et al. (2010) investigated the first were characterized by additional soluble extracellular full scale MBR for separate treatment of hospital polymeric substances, which accumulated on the wastewater in Germany. A nanofiltration (NF) as well as a membrane and increased fouling. reverse osmosis (RO) module for further treatment of the

While membrane fouling can be a challenge, MBR filtrate were tested and results confirmed that MBR

Kluepfel and Frimmel (2010) investigated the retention and technology followed by an advanced treatment for trace fouling behavior during filtration of surface water (River pollutant removal is an adequate approach for specific

Alb, Germany) by nanofiltration and low pressure reverse treatment of hot spot wastewater such as hospital osmosis membranes. Rejection of four polar wastewater. In particular, it was shown that – comparing micropollutants—metamitron, clofibric acid, atrazine, and the tested NF and RO – only (a two stage) RO is terbutaline—was monitored and showed that fouling did appropriate to remove pharmaceutical residues from not affect the rejection of the compounds significantly. The hospital wastewater entirely. Further, the combination of feed matrix turned out to determine the influence of an MBRs and nanofiltration with reverse osmosis that was alkaline cleaning step on micropollutant rejection and steric used to successfully reduce the concentration of eleven and electrostatic effects were the most important factors micropollutants in hospital wastewater was enhanced by influencing retention of the organic substances. absorption, charge, and the molecular weight cut off of the

Because of advances in MBR technology, the membrane. Other research by Corvini, et al. (2010) is viability of treating high concentrations of emerging investigating methods for improving MBR performance. pollutants from wastewater is improving. For example, This research group has used low-cost industrial laccases— high-concentration antibiotic wastewater treatment by resistant oxidative enzymes—that can be immobilized by

MBR was studied using submerged flat sheet membrane covalent attachment onto the surface of nanoparticles and

(Sundararaman and Saravanane, 2010) with the objective to then retained in MBRs or perfusion basket reactors to study determine the effect of organic loading rate and hydraulic elimination of micropollutants from wastewater. Laccases retention time on the removal of a cephalosporin derivative, are metal-containing enzymes capable of oxidizing and intermediates in the MBR with enhanced numerous phenolic substrates by one electron abstraction biodegradation using bioaugmentatione. Based on these and therefore are useful biocatalysts for degrading EDCs results, the industry is looking for the alternatives of either such as bisphenol A, estradiol, ethinylestradiol, triclosan, direct disposal of 7-ADCA and phenyl acetic acid or for and nonylphenol. further degradation and disposal, which will essentially Photolysis/Photocatalysis. There is a great deal require additional cost and maintenance. Also, MBR can be of recent research on photocatalysis and photolysis; coupled with other treatment processes to provide high Gamage and Zhang (2010) have provided a review of

1929 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation widespread applications of these techniques. Evaluations of hr, compared to 80% removal in the standard reactor. applications in water and wastewater have been conducted Research by Madukasi, et al. (2010) using a suspended and include collection of data on efficiency, kinetics and growth photobioreactor was utilized to treat pharmaceutical mechanisms of reaction. There are efforts to develop new wastewater by a wild strain purple non-sulfur methods of treatment using this process including the photosynthetic bacterium isolated from the soil. Chemical collaborative effort described by Likodimos, et al. (2010) to analysis of the culture after treatment of the enriched and conduct a unique collaborative project that is aimed at non-enriched wastewater proved that photosynthetic developing innovative nanostructured UV-visible bacteria could transform complex wastewater that contains photocatalysts for water treatment and detoxification. The recalcitrant organic compounds with a resultant recovery of approach is to use anion-doped titanium dioxide (TiO2) useful products. Elmolla and Chaudhuri (2010) reported on nanomaterials and titania/carbon nanotube hybrid materials the photo-Fenton treatment of antibiotic wastewater. with enhanced photocatalytic acitivity in the UV-visible Other research has focused on characterizing the spectral range. There are researchers such as Alvarez, et al. efficiency of removal for various combinations of

(2010) who successfully prepared magnetic catalyst processes and compounds. Choina et al. (2010) studied nanoparticles that they tested for their ability to catalyze the photocatalytic degradation of tetracycline using solarium photodegradation of acetaminophen and 4 other PPCPs UV-A and black light with differently applied electric from an aqueous solution. In terms of catalytic activity, the power and catalysts. They found that photocatalytic synthesized magnetic nanoparticles were almost treatment with titantia is highly efficient at removing low comparable to a commercial TiO2 photocatalyst showing concentrations of tetracycline in drinking water. Achilleos greater than 95% removal for all target compounds tested, et al. (2010) studied solar and UV-A photocatalysis with except acetominophen. suspended TiO2 to degrade ibuprofen and carbamazepine in

Other researchers have developed a municipal aqueous matrices. Basha, et al. 2010 used integrated wastewater treatment method based on a solar AOP where photocatalytic adsorbents (IPCAs) based on TiO2-activated the photoactive layer of TiO2 was deposited on glass carbon for the photodegradation of indomethacin (IND) in spheres; Miranda-Garcia, et al. (2010) reported on this aqueous solutions. The IPCAs in dark adsorption studies method for degradation of 15 emerging contaminants. Bai, had high affinity toward IND with the amount adsorbed et al. (2010) showed that double-sided photocatalytic thin proportional to the TiO2 loading and adsorption capacity film could significantly outperform single-sided increased with increase in TiO2 content. In another study, photocatalytic thin films for removal of tetracycline in bulk photocatalytic degradation of phenol, nalidixic acid, and a wastewater; with a starting concentration of 20 parts per mixture of pesticides and other emerging contaminants in million (ppm), 96% of the tetracycline was removed after 1 water was mediated by TiO2 and iron oxide immobilized on

1930 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation functionalized polyvinyl fluoride films in a compound photodegradation. Yang, et al. (2010a) studied the parabolic collector solar photoreactor (Mazille et al., 2010). photocatalytic degradation of three beta-blockers in TiO2

Phenol was efficiently degraded and mineralized at suspensions and reported on the degradation kinetics and operational pH < 5 and nalidixic acid degradation was major degradation intermediates of this reaction. complete even at pH 7, but mineralization stopped at 35%. While photocatalytic and photolysis processes

Pesticide mixture was slowly degraded (50%) after 150 min show much promise for treatment of emerging pollutants, of irradiation. Degradation of the emerging contaminant there is potential for formation of reaction byproducts. mixture was successful for eight compounds and less Yamada, et al. (2010) subjected fenthion to UV-A efficient for six other compounds. irradiation and showed that fenthion sulfoxide and MMS

Similar to the Mazille, et al. (2010) work, the were identified as the major products and that resulting kinetics and mechanisms of photocatalytic and photolysis estrogenic activity was detected in the UVA-irradiated treatment processes are also being evaluated by various solution. They found a new and potentially significant research groups. For example, photodegradation of estrogenic active compound, S-aryl fenthion, which was boldenone and trenbolone, which have endocrine disrupting induced by the photo-irradiation showing that transformed activity, were evaluated for photolysis alone and in the products are important to consider. presence of hydrogen peroxide (H2O2) (Gryglik, et al., Ultrasonic Degradation. De Bel, et al. (2010)

2010). Photolysis of boldenone occurs very fast and is focused on the sonolytic degradation of ciprofloxacin, a independent of pH indicating possibility of its removal fluoroquinolone antibiotic. During a first experiment at during UV disinfection of drinking water; the addition of 25oC and 544 kiloHertz (kHz), degradation of a 15 mg /L

H2O2 during photolysis significantly accelerates the rate of ciprofloxacin solution showed a pseudo-first order

-1 steroids decay. Yang et al. (2010b) studied the degradation constant k1 equal to 0.0067 ± 0.0001 min (n = photocatalytic degradation kinetics of three sulfa 3). Experiments with t-butanol as a radical scavenger pharmaceuticals in TiO2 aqueous suspension and found that showed that reaction with hydroxyl radicals is the main surface reaction played an important role in the degradation degradation route for ciprofloxacin. Since the production of of sulfa pharmaceuticals. The disappearance of these three hydroxyl radicals was the highest at 544 kHz, this was also compounds follows a pseudo-first-order kinetics according the most favorable frequency for ciprofloxacin degradation

-1 to the Langmuir–Hinshelwood model. Ge, et al. (2010) in comparison with 801 (k1 = 0.0055 per minute [min ])

-1 studied the kinetics, influencing factors and mechanisms on and 1081 kHz (k1 = 0.0018 min ). the photodegradation of gatifloxacin; the reaction follows Enzymatic Treatment. Enzymatic treatment has the pseudo-first-order kinetics with in pure water and been investigated as a feasible process to degrade some undergoes direct photolysis as well as self-sensitized emerging pollutants in liquid and solid media. Majeau, et

1931 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation al. (2010) published an overview of parameters affecting WWTPs. In this study, the use of the white-rot fungus in a the biocatalysis of pollutants by laccases or lignolytic defined liquid medium was assessed. Ketoprofen was enzymes. Laccases oxidize, polymerize or transform degraded to nondetectable levels in 24 hours when it was diverse substrates such as phenols, dyes, pesticides, added at 10 mg/L; at a low concentration of 40 µg/L, endocrine disrupters and polycyclic aromatic hydrocarbons ketoprofen was almost completely removed (95%) after 5 and require only molecular oxygen as a co-substrate, and hours. Marco-Urrea, et al. (2010a) assessed the degradation no other cofactors are needed for their activity. Because of of diclofenac sodium using this species and demonstrated this property, researchers have investigated the potential for almost complete removal within the first hour of treatment. degrading tetracycline and oxytetracycline using crude In vivo and in vitro experiments suggested at least two manganese peroxidase, prepared from Phanerochaete different mechanisms of diclofenac degradation with both chrysosporium (a white rot fungi). Wen, et al. (2010) found parent compound and intermediates disappearing after 24 the degradation rate of these antibiotics was dependent on hours which also leads to decreased ecotoxicity as pH and temperature. In another similar study, Zhang and measured by the Microtox test.

Geißen (2010a) also used crude lignin peroxidase, Physical Separation, Membrane Processes. produced from the same white rot fungus species and Membranes are commonly used for filtration of drinking studied degradation of diclofenac and carbamazepine in the water. In a study by Dixson, et al. (2010), NF was presence of H2O2 as the oxygen substrate. The H2O2 evaluated for the efficiency of removing algal toxins, concentration, pH, veratryl alcohol concentration and cylindrospermopsin, 2-methylisoborneol, and geosmin. temperature were monitored during the study; diclofenac Treatment efficiency generally exceeded 90% but was was completed degraded at pH 3.0 – 4.5 and 3 – 24 ppm of affected by the molecular weight cutoff of the membrane,

H2O2, while degradation efficiency of carbamazepine was membrane material, membrane hydrophobicity, and less than 10%. operation time. Other researchers (Ben-David, et al., 2010)

Research by Rodriguez-Rodriguez, et al. (2010a have found that modified commercial NF membranes, and b) also evaluated the ability of another white rot fungus using concentration polarization-enhanced surface graft- species, Trametes versicolor, on sewage sludge and found polymerization, showed improved rejection of EDCs by that approximately half of the naproxene and commercial. In managing the concentrates resulting from carbamazapine present in the sludge could be removed NF treatment of surface water for drinking water within 24 hours. Marco-Urrera, et al. (2010b) also production, Vigneron-Larosa, et al. (2010) investigated two investigated Trametes versicolor to degrade ketoprofen, an complementary approaches. In one approach, an additional

NSAID, that has been detected in the environment in the nanofiltration stage produced an increase in drinking water range of ng/L to ug/L due to its low degradability in some production; in a second approach, removal of

1932 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation phosphonates, micropollutants and natural organic matter secondarily individually treated effluent of a WWTP was was investigated to treat the concentrate before disposal. investigated in Spain (Boleda et al., 2010). All 3 low

Acero, et al. (2010a & 2010c) tested energy polyamide membranes removed the compounds at ultrafiltration (UF) and (nanofiltration) NF membranes for rejections ranging from 30% (nicotine in March) to 100% filtration of secondary municipal effluent. Rejection (caffeine in August). coefficients for 28 pharmaceutical compounds were Physicochemical Separation, Coagulation and determined, with eliminations higher than 75% for one of Sorption Processes. The various physico-chemical pre- the NF membranes tested showing that NF may be an treatment and biotransformation processes for wastewater excellent option for the removal of pharmaceuticals in and wastewater sludge has been reviewed by Mohapatra, et municipal wastewater. Adsorption was determined to be the al. (2010) to describe the removal of bisphenol A. Sorption main retention mechanism for UF membranes, whereas size and coagulation are two of the physical pretreatment exclusion and electrostatic repulsion of negative species at processes that could be used to pretreat these samples and a high pH were deemed responsible for micropollutant summary of chemical coagulation and sorption processes retention by NF membranes. Yangali-Quintanilla, et al. that have been investigated for removal of emerging

(2010d) also conducted work that showed promising results pollutants is provided here. for rejection of organic contaminants and proposed Chemical coagulation is a conventional treatment nanofiltration as acceptable barrier for water reuse. process commonly used for drinking water treatment as

Properties of membranes are also important in well as for enhancing phosphorus removal from wastewater determining their filtration performance. For example, effluent. Effects of aluminum flocculation on activated laboratory-fabricated hollow fiber polyethersulfone (PES) sludge performance and 17α-ethinylstradiol removal were membranes were used by Bolong, et al. (2010) to remove studied by Park, et al. (2010) using bench-scale activated more than 90% of bisphenol A from water; the highly sludge systems. Results showed that higher aluminum-fed effective removal was attributed to the negatively charged activated sludge led to better settling, dewatering, and properties of the PES membranes. Moon, et al. (2010) effluent quality with better 17α-ethinylstradiol removal. compared two types of membranes, meta-phenylene Electrocoagulation is another method of creating a metal diamine (MPD) and piperazine based polymers, for hydroxide floc by applying a current to a metal electrode to propensity to foul when removing wastewater effluent generate metal ions for the process. Deshpande, et al. organic matter for water reclamation and the MPD (2010) evaluated the efficiency of electrocoagulation for membrane had a higher propensity to foul. Finally, the treatment of a pharmaceutical containing (ranitidine) ability of reverse osmosis treatment to remove 10 illicit wastewater and monitored water quality parameters and drugs and their metabolites from seasonally generated operation conditions during the study. Electrocoagulation

1933 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation successfully reduced the biochemical oxygen demand analysis of the carbon samples after adsorption of the

(BOD) and chemical oxygen demand (COD) by 85 - 90% analgesic showed that adsorbent–adsorbate affinity is at a current density of 80 milliAmps per square meter stronger in hydrophobic carbons of basic character that

(mA/m2) in 25 minutes. Robic, et al. (2010) correlated the contain a well-developed microporosity. However, these current applied between the electrodes to the removal of characteristics are not sufficient for an overall performance phenolic compounds and protein from aqueous solutions, of a carbon in acetaminophen removal. Additionally, but the principle could also be applied to other biological removals of two pharmaceuticals, an antibiotic drug, compounds; the authors developed simple, time-dependent sulfamethoxazole and an antiparasitary drug, metronidazole models based on the complex formation between these onto activated carbon from aqueous solutions were studied biological substances and the aluminum hydroxide gel by Caliskan and Gokturk (2010). Batch adsorptions studies phase. In another coagulation process, Yang, et al. (2010d) were carried out at different pH, adsorbent concentrations, investigated the effect of microwaves on species and temperatures. Increased pH caused decreased distribution of ferric hydrolysates, as well as the effect of adsorption of sulfamethoxazole and metronidazole; and the hydrolysates speciation on the treatment efficiency of kinetics of adsorption, in light of three models, the first- organic compounds in coagulation. A ferron-complexed order Lagergren model, the pseudo-second-order model timed spectrophotometric method was used to classify the and the intraparticle diffusion model was discussed. Saha, iron speciation under different reaction conditions with et al. (2010) studied the adsorption of 17β-oestradiol and results indicating that highly polymeric ferric iron 17α-ethinylestradiol onto several granular activated carbons facilitated the net rolling-sweep action for organic and macronet polymers; they demonstrated the potential of molecules in coagulation process, which enhanced the these adsorbents for the removal of EDCs from aqueous removal efficiency of entire reaction system. solution. Serrano, et al. (2010) added granular activated

Activated carbon has been used for decades to carbon (GAC) to conventional activated sludge processes adsorb contaminants from water. The removal of an to determine the benefits to PPCP removal during analgesic drug (acetaminophen) from water was secondary treatment. The more recalcitrant compounds investigated using activated carbons prepared from (carbamazepine, diazepam and diclofenac) had the highest different residues, comparing their adsorption capacity with adsorption capacities onto GAC, which is consistent with that of commercially available carbonaceous adsorbents adsorption as the removal mechanism.

(Cabrita, et al. 2010). The samples prepared from chemical There are also other sorption methods that have activation of the biomass residues show reasonably high been tested for removal of emerging pollutants. Sorption of removal efficiencies along with fast rate of adsorption, perfluorooctane sulfonate on organo-montmorillonites which are in fact comparable to commercial carbons. The (Zhou, et al., 2010d) and sorption of perfluorooctane

1934 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation sulfonate (PFOS) and perfluorooctanoate on activated copper onto its surface, resulting in a potential sorbent for sludge were studied for their removal from water. The the removal of naproxen from water. Under alkaline

PFOS molecules first diffused into the organo- conditions, the copper-modified sorbent was more effective montmorillonites via hydrophobic interaction, and then the for removal of naproxen when compared to other sorbents rearrangement occurred through electrostatic interaction prepared. A strong base anion exchange resin, MIEX©, between the two surfactants, resulting in a microstructure having a magnetic core to assist with agglomeration and change within the organo-montmorillonites. In activated recovery, was examined by Neale, et al. (2010) for the sludge studies, the effect of pH and the zeta potential removal of the steroidal hormone estrone. The interaction measurement implied that electrostatic repulsion prevented of estrone with the resin occurs as a side effect when their sorption, but the protein composition on the natural organic matter is removed and performance of the heterogeneous surface of activated sludge was favorable for resin was influenced by solution chemistry, temperature, the sorption of PFOS and PFOA. Additionally, active and the presence of competing anions. sorption on living microorganisms was also observed. The influence of adsorption and coprecipitation

Whelehan, et al. (2010) investigated the agents for the removal of PPCPs in three activated sludge feasibility, kinetics and efficiency of using liquid-core systems was examined by Serrano, et al. (2010). A microcapsules as a novel methodology, termed capsular conventional activated sludge (CAS) reactor was compared perstraction, to remove seven pharmaceuticals commonly to a CAS unit continuously fed with FeCl3, and to a reactor found in the aqueous environment. Results indicate that this in which granular activated carbon was fed directly into the approach is a viable method for removal of the target mixed liquor. Acidic pharmaceuticals (naproxen and compounds, rapidly but with a variable efficiency; the main ibuprofen) were almost completely removed (> 90%) in all rate-limiting step to mass transfer was due to the stagnant three reactors; more hydrophobic organic compounds organic film within the core of the microcapsules. Cychosz (musk fragrances) were removed by approximately 90% in and Matzger (2010) used powder x-ray diffraction to study all reactors; more recalcitrant compounds like diazepam the stability of a variety of microporous coordination and carbamazepine were removed by up to 40% and polymers (MCPs) and found that some MCPs were diclofenac up to 85%. Zhou, et al. (2010c) also evaluated novel completely water stable and were able to adsorb furosemide magnetic dendritic materials for adsorption of drugs. and sulfasalazine with large uptakes achievable at low Other research exploiting sorption as a removal concentrations, indicating that the adsorption of wastewater process for emerging pollutants has been conducted with contaminants may be a feasible application for these new nanomaterials. Saad, et al. (2010) used a nanostructed materials. Mesoporous silica, prepared by Rivera-Jimenez silica-based material as a possible adsorbent for

(2010) and modified by incorporation of cobalt, nickel, or trinitroglycerin removal and found that steady state was

1935 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation reached rapidly, within 1 hour and sorption kinetics matrices. Quintana, et al. (2010) evaluated nine acidic followed a pseudo second order equation based on the pharmaceuticals and their reaction with hypochlorous acid;

Langmuir model. Ji, et al. (2010a) evaluated the factors the effect of pH, chlorine and bromide concentrations were controlling adsorption of antibiotics tylosin, tetracycline relevant in the degradation of the parent compounds and and sulfamethoxazole to single walled carbon nanotubes, formation of byproducts, where chlorine plays the most micro and meso carbon nanotubes and graphite nanotubes. important role, but bromide also is an important factor

The results showed that adsorption varied by antibiotic and leading to brominated byproducts. Additionally, pore size was not important for the activated carbon halogenated by-products of salicylic acid have been

(meso/micro). Additional work by Ji, et al. (2010b) showed detected in all analyzed wastewater samples and that compound K-OH etching of carbon nanotubes (chlorinated) drinking water samples but not in surface improved the absorption affinity of the carbon nanotubes water, confirming that these compounds are produced for monoaromatic (phenol and nitrobenzene) as well as during chlorination. antibiotics (sulfamethoxazole, tetracycline and tylosin). Research has also been conducted using the

Wang, et al. (2010) evaluated the removal of cycling of reduced and oxidized metals to oxidize emerging carbamazepine in spiked laboratory and lake waters was pollutnants. Guan et al., provided a mini-review on the measured using silica nanoparticles and 5 different application of permanganate in the oxidation of hydroxapatite beads and was compared to removal via micropollutants. Further, in manganese [Mn(VII)] batch powdered activated carbon, which outperformed other oxidation experiments, Hu, et al. (2010) studied sorption alternatives. cirprofloxacin, lincomycin, and trimethoprim and indicated

Chemical and Electrochemical Oxidation. One that oxidation reaction rates were first order with respect to of the most common methods of chemical oxidation is Mn(VII) concentration. Temperature dependence was chlorination which is often applied in both water and consistent with the Arrhenius equation; however, pH wastewater treatment as a disinfectant, as a result impacts on reaction rate were compound specific. researchers have investigated this process for its impact on Lincomycin reaction rates increased significantly with the elimination of emerging pollutants. Acero, et al. increasing pH whereas trimethoprim reaction rates

(2010b) evaluated the elimination of four pharmaceutical decreased with increasing pH. In another study, Collado, et compounds in several water matrices, showing that al. (2010) investigated catalytic oxidation of phenol and increased organic and inorganic matter increased chlorine phenol-derivates present in pharmaceutical wastewaters demand, leaving less chlorine available for the oxidation of using hydrated iron sulfate (FeSO4 ·7H2O) as a these compounds. Half-life times and oxidant exposures homogeneous catalyst. The catalytic effect of iron [Fe]

99% removal of the pharmaceuticals were reported in these during the wet oxidation of phenol was only observed at pH

1936 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation values ranging between 2 and 3, due to the establishment of PPCPs from reverse osmosis brine as well as WWTP the Fe(III)/Fe(II) redox cycle. The best results for the effluent and found that electrical current density in the catalytic oxidation of salicylic acid were obtained for pH range 20–100 A/m2 did not have an impact on removal, values below 2, and they were related to the formation of likely due to the mass transfer resistance developed in the an Fe(II)-salicylic acid complex; conversely, the presence process when the oxidized solutes are present in such low of Fe(II) had a prejudicial effect on the degradation of p- concentrations. The mineralization of ketoprofen by anodic hydroxybenzoic and 5-hydroxyisophthalic acids. oxidation was studied by Murugananthan, et al., 2010)

Klamerth, et al. (2010a, 2010b) studied employing boron doped diamond and platinum electrodes. degradation of 15 emerging contaminants at low The redox behavior of the ketoprofen molecule, fouling of concentrations in simulated effluent and WWTP effluent in electrodes, generation of oxygen and active chlorine a pilot scale solar photo-Fenton reactor. The degradation of species were studied by cyclic voltammetry. The effect of these compounds, each with an initial concentration of 100 electrolyte, pH of aqueous medium and applied current

μg/L, was found to be dependent on the presence of density was evaluated with respect to the mineralization carbonate and bicarbonate and on the type of water behavior of ketoprofen. The physisorbed hydroxyl radical

(simulated water, simulated effluent wastewater and real impact on the boron doped diamond electrode was effluent wastewater), but is relatively independent of pH, observed to trigger the mineralization of ketoprofen; poor the type of acid used for release of hydroxyl radicals mineralization at both the boron doped diamond and scavengers and the initial H2O2 concentration used. They platinum anodes in the presence of sodium chloride as also studied solar photo-Fenton as a tertiary treatment supporting electrolyte was ascribed to the formation of process and showed successful degradation of the same chlorinated organic compounds which are refractory, contaminants in the effluents from different municipal however, complete mineralization of ketoprofen was

WWTPs at low iron concentration (5 mg/L). Results achieved using sodium sulfate as the supporting electrolyte. showed that although most degradation took place during Ozone and Advanced Oxidation Processes the Fenton process, photo-Fenton was necessary to degrade (AOPs). The ability of ozone to significantly reduce low the target compounds below their limit of detection. Su, et level concentrations of trace organic compounds, including al. (2010) also conducted a study on the photo-Fenton EDCs, PPCPs, and other emerging contaminants have oxidation process for treatment of acetylspiramycin increased interest in applying ozone in potable water and pharmaceutical wastewater. wastewater treatment (Oneby, et al., 2010). A recent

Electro-oxidation is another oxidation process American Water Works Research Foundation report that has been evaluated for treatment of emerging indicated high removals of many EDCs and PPCPs at pollutants. Perez, et al. (2010) investigated removal of ten typical disinfection doses. Utilities are using ozone in a

1937 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation variety of ways: as a primary disinfectant, for treatment of filtration), but five of the nine target pollutants plummeted microconstituents, and in combination with other processes to concentrations below the method detection limits

(e.g., membranes and UV) to produce high quality water following AOP, which provided higher removal for all nine for indirect potable reuse and this review paper highlights compounds, compared to conventional treatment. the different applications, treatment goals and basis of Nanaboina et al. (2010) examined the evolution process selection. Further, because of its high reduction- of absorbance spectra of wastewater ozonated using oxidation potential ozone is a good process candidate for varying initial ozone concentrations or treatment times; treatment of complex organics which is why researchers concomitant changes of concentrations of trace-level continue to publish information on removal of emerging pharmaceuticals were also quantified. Gharbani, et al. pollutants in both water and wastewater using this (2010) studied degradation of 4-chloro-2-nitro phenol in technology. In fact, Lundstroem, et al. (2010) showed aqueous solution by ozonation; the main intermediate through investigation of different types of wastewater product was chlorophenol and that ozonation was more retreatment for efficacy at removing pharmaceuticals, effective at alkaline than acidic conditions. Coelho, et al. hormones and endocrine disruptors that of conventional (2010) studied the biodegradability and toxicity of 3 with and without sand filtration, moving bed biofilm NSAIDs (diclofenac, ibuprofen and naproxen) treated by reactor, ozone, moving bed biofilm reactor combined with ozonation. The results show that the total removal of 200 ozone, and MBR, ozone had the highest efficacy of mg/L of diclofenac and 100 mg/L of naproxen is possible treatment but sometimes resulted in ecotoxilogical effects. using an ozone dose of 0.20 and 0.04 g/L, respectively. For

A similar review was conducted by Oulton, et al. (2010) 200 mg/L of ibuprofen, 90% removal is achieved using an who reviewed published data and commented on the most ozone dose of 2.3 g/L. According to the Microtox test, the cost effective series of treatment technologies for PPCP treatment with ozone removes the toxicity of the naproxen removal; at best, 90% removal was observed for primary solution. and secondary treatment with AOPs affording significantly Other researchers have evaluated options for higher removal efficiency, sometimes to below laboratory enhancing ozone treatment of emerging pollutants by using detection limits. These conclusions were further confirmed catalysis. Beltrán et al. (2010) studied the ozonation of by Rahman, et al. (2010), who studied the occurrence of diclofenac and synthetic 17α-ethinylstradiol in laboratory selected EDCs and PPCPs in Lake Huron Water by spiking prepared water and domestic wastewater, in the presence of raw Lake Huron water with 9 target compounds and perovskite catalysts; they showed that both compounds are treating in a dual train pilot scale treatment plant. None of removed by direct ozonation and reported the apparent rate the target chemicals showed significant removal following constants of the heterogeneous reaction between ozone and conventional treatment (coagulation, sedimentation and total organic carbon (TOC) on the experimental catalyst

1938 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation surface. Yang, et al. (2010a) investigated catalytic respectively. Both diclofinac and naproxen exhibited a two- ozonation of pharmaceutically active compounds aqueous stage biodegradability reaction wherein the ozonation solution. Using attenuated total reflection-Fourier transform products produced in stage 1 were biodegradable than the infrared (ATR-FTIR) spectroscopy the researchers verified products produced in stage 2. The toxicity of ozonated that the Lewis acid sites of several catalysts were the ibuprofen and naproxen solution decreased after treatment reactive centers for the catalytic ozonation of ciprofloxacin and remained unchanged for diclofenac solutions and ibuprofen in water. There are instances when ozonation as an

Although ozonation is a useful treatment oxidation reaction alone is not sufficient to remove some technology for the removal of micropollutants, some compounds and AOPs are taking on greater importance for micropollunts are ozone refractory and are partially treatment of emerging pollutants. A great deal of research degraded due to hydroxyl radicals generated via oxidation is ongoing with regard to documenting the removal rates, of dissolved organic matter by ozone. Tri-n-butyl efficiencies and mechanisms for various AOP. Tuerk et al., phosphate and tris-2-chloroisopropyl phosphate 2010 has evaluated different AOPs for the treatment of degradation by ozone followed first order kinetics and their highly loaded wastewater streams evaluated optimization of concentrations were halved at ozone to DOC ratios of 0.25 removals and improvement of efficiency in the laboratory and 1.0, respectively (Pocostales et al., 2010). Because of and in pilot plants. The persistent cytostatic drug this, toxicity can be a concern and Stalter, et al. (2010) has cyclophosphamide was selected as a reference substance conducted toxicity evaluations of different treated regarding elimination for evaluation of the various wastewater effluents treated with an ozonation step and an oxidation processes. In another study, Can et al. (2010) activated carbon treatment step in parallel subsequent to evaluated dissolved organic carbon (DOC), COD, UV conventional activated sludge treatment. Estrogenicity absorbance at 254 nanometers (UV254), total coliform, removal by ozonation and activated carbon treatment was dissolved ozone and 6 EDCs were during ozone and confirmed toxicity and genotoxicity were observed ozone/H2O2 treatment of tertiary WWTP effluent. The following ozonation possibly resulting from formation of optimum ozone:H2O2 ratio was 0.5; at a ratio of 2, the toxic oxidation byproducts; in these cases, biologically efficiency of the AOP was diminished due to consumption active sand filtration obviously is suggested as an effective of the ozone by H2O2. barrier to such compounds. Coelho, et al., (2010) have also Researchers also report on kinetics of AOP. An, evaluated the toxicity and biodegradability of ibuprofen, et al. (2010), studied three fluoroquinolone pharmaceutical diclofenac and naproxen with water following ozonation. compounds and reported on the absolute rate constants for

Biodegrability measured as BOD/COD value was 0.20, 0.3, hydroxyl radical and the hydrated electron. For norfloxacin, and 0.21 for diclofinac, ibuprofen and naproxen, levofloxacin, and lomefloxacin, the bimolecular reaction

1939 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation rate constants with hydroxyl radical were determined and to also correlated with ultraviolet absorbance at 254 nm provide insights into the chemistry of destruction of these (UV254). three target pharmaceuticals, transient spectra were Research into innovative AOPs include work by obtained for the reaction of hydroxyl radicals with the three Gerrity, et al. (2010) who evaluated a pilot-scale compounds. Also, Gunagi, et al., 2010 studied the nonthermal plasma AOP for degradation of advanced oxidation kinetics of 6-aminopenicillanic acid pharmaceuticals and potential EDCs. Degradation of seven oxidation by diperiodatoargentate(III); researchers reported indicator compounds was monitored in tertiary-treated the reaction order and mechanism of reaction with reaction wastewater and spiked surface water to evaluate the effects constants and thermodynamic quantities. Tuerk, et al. of differing water qualities on process efficiency; results

(2010) evaluated three AOP strategies (low pressure indicated that NTP may be a viable alternative due to its mercury lamps and H2O2, high pressure mercury lamps comparable energy requirements and ability to operate with H2O2 and ozone) that efficiently reduced the toxicity without any additional feed chemicals. Dominguez, et al. of wastewater containing cyclophosphamide, (2010) investigated electrochemical anodic oxidation as an carbamazepine, chloramphenicol, and sulfamethoxazole, at AOPs for destruction of carbamazepine by varying pH, treatment times ranging from 17 to 285 minutes. Although current, concentration of supporting electrolyte sodium efficient for these compounds, the strategies are not sulfate, and solution flow rate; optimum degradation was recommended for diagnostic compounds because found at pH 9; other operational parameters were also transformation rather than degradation occurs. reported for flow, and current density.

Mechanisms of AOP are also elucidated by While effective for a wide range of treatment researchers such as Fernandez, et al. (2010) who studied goals, use of AOP for drinking water treatment can have different AOPs for cyclophosphamide oxidative challenges associated with formation of halogenated degradation in aqueous media showing that the radical disinfection by-products. Dotson, et al. (2010) followed a mechanism acting in the AOPs rapidly degrades UV/H2O2 AOP with chlorination which resulted in a slight cyclophosphamide. Rosario-Ortiz, et al. (2010) evaluated increase in total trihalomethane (TTHM) formation.

AOP for the oxidation of six pharmaceuticals in three Addition of H2O2 resulted in an up to 37 ug/mg-C increase wastewater effluents. The role of the water quality on in TTHMs in the case of 10 ppm H2O2 addition. hydroxyl radicals was used to explain differences in Because of its application, AOP performance removals between wastewaters. Results indicated that the monitoring is of significant interest and there is a renewed efficacy of this process was a function of EfOM and its interest in predicting the ratio between hydroxyl radical and reactivity towards hydroxyl radicals; the removals were ozone exposures (RCT), following growing evidence that

AOP is effective against many emerging contaminants.

1940 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Vincent, et al. (2010) investigated five surface waters for constants for Fenton's reagent. Kim and Tanaka (2010) hydroxyl radical activity using the RCT concept, to predict compared ozone, ozone/H2O2 and ozone/UV effectiveness

RCT using traditional water quality characteristics and in the removal of antibiotics, analgesics, insect repellants, contaminant removal by ozonation and peroxone. They and other PPCPs. A detention time of 10 minutes and showed that RCT was dependent on water quality ozone concentration of 6 mg/L was effective in removing characteristics and could be modeled using water 90% of the pharmaceuticals; however, UV or H2O2 are characteristics and treatment conditions. In addition to needed to remove caffeine, DEET, and cyclophosphamide. performance monitoring, treatment costs for AOPs is In another study, ozone, ozone/UV and H2O2/UV presented by Carlesi Jara and Fino (2010); they present the successfully reduced the concentration of diclofenac, derivation and application of an expression to determine the clofibric acid, carbamazepine and diazepam following optimal current density in order to carry out the direct conventional biological wastewater treatment (Jose, et al. electroxidation of pharmaceutical-compound containing 2010); however, oxidation degradation products of aqueous solutions. carbamazepine were observed in ozone treated waters. Giri,

There are numerous methods of implementing et al. (2010) evaluated seven AOPs and for sixteen PPCPs.

AOP and as such, much research has focused on comparing The removal profiles exhibited four distinct patterns: a) the cost and efficiency of these processes. Bertanza et al. easily degradable by all seven techniques, b) not easily

(2010) showed that to implement advanced oxidation degradable by all seven techniques, c) easily degradable by

(UV/H2O2 and ozonation) at WWTPs for destruction of ozone-based techniques, but not by ultraviolet radiation-

EDCs and PPCPs, treatment efficiency and cost must based techniques and d) easily degradable by ultraviolet justify the inclusion of this technology for trace compound radiation-based techniques, but not by ozone-based removal. To achieve 70 % reduction of the following techniques. Lee and von Gunten (2010) investigated the representative compounds nonylphenol and bis-phenol A at ability of chlorine, chlorine dioxide, ferrate, ozone, and

1 µg/L, the treatment costs are 9 Eurocents/m3 and 2-4 hydroxyl radical to degrade micropollutants. Hydroxyl

3 Eurocents/m for UV/H2O2 and ozonation, respectively, radicals were non selective and reacted with any inorganic with the higher UV operating costs is due to the UV lamp moieties whereas the other oxidants were more selective in energy consumption. treating with electron rich moieties. Organic matter, amines

Real, et al. 2010 evaluated hydrochlorothiazide, a and ammonia competed with the micropollutants for the thiazidic diuretic very frequently used in the treatment of oxidants and the competition was oxidant specific. hypertension, oxidation by means of UV radiation, In applying ozonation and AOP, there are often

Fenton’s reagent and ozone. In this work, competition benefits of evaluating these processes in combination with kinetics were used to determine second order kinetic other treatment processes to provide perspective on

1941 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation application. For example, Rivera-Utrilla, et al. (2010) when Ruel, et al. (2010) evaluated eight municipal WWTPs examined treatment of tinidazole, an antibiotic, with ozone that had conventional and advanced secondary processes; and activated carbon; this combination into a single process the removal efficiency of sixty organic substances in may be an attractive alternative to advanced oxidation wastewater and sludge was about 70% by the activated systems. Results of this study showed increased removal sludge process. MBRs increased efficiency for about one rates, reduced oxidation by-product toxicity, and reduced third of the substances, although five of the substances concentrations of dissolved organic matter. Flyborg, et al. were measured at concentrations exceeding target quality

(2010) evaluated the benefits of the combination of standards at the plant outlets. nanofiltration and ozone to remove micropollutants in Gabet-Giraud, et al. (2010) also examined the wastewater for potential reuse conditions. Order was not removal efficiencies of eight biological treatment processes significant as either approach resulted in 99% removal of for the removal of estrogens and beta blockers. Biological the micropollutants. Liu, et al. (2010) evaluated the treatment was efficient for removal of estrogens from the efficiency of ozone, UV and UV/ozone to treat dissolved phase, with removal rate around 90%. For beta microcystein, a hepatoxin excreted by cyanobacteria in blockers, acebutolol and nadolol were efficiently removed contaminated water. Sequential treatment with UV and (mean removal rate of 80%), whereas sotalol and ozone outperformed treatment by UV or ozone individually propranolol were hardly impacted by biological treatments and, in some instances, natural organic matter improved (removal rate below 20%). Ozonation, reverse osmosis and treatment efficiency (UV) and in other cases hindered activated carbon filtration provided high removal efficiency performance (ozone). for beta blockers (above 80%), but on the contrary, high

Comparison of Treatment Technologies. With speed chemical settler, sand filtration, silex filtration, respect to water treatment processes, Kegel, et al. (2010) microfiltration and UV generally provided removal rates evaluated the effectiveness of reverse osmosis and below 30% for all beta blockers. The polishing pond activated carbon filtration to remove micropollutants from presented variable removal performances depending on the source water. Reverse osmosis treatment effectiveness was molecules (up to 75% for propranolol). In another study of more negatively impacted by hydrophobicity and less biological treatment processes, Dagnino, et al. (2010) impacted by water permeability and salt rejection while examined three different treatment technologies, waste activated carbon was effective even at low hydraulic stabilization ponds, trickling filters and activated sludge residence times. supplemented with a biofilter system; for estrogenic and

In wastewater, many researchers have evaluated aryl hydrocarbon receptor, the waste stabilization ponds more than a single process to determine the most efficient showed greater or similar removal efficiency than activated method for removal of emerging pollutants. For example, sludge with biofilters, and both were much more efficient

1942 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation than the trickling filter, which had the lowest removal treatment, a MBR, an ozonation. The efficiency of removal efficiency. by the MBR treatment improved from 20% to 60% when

Balabanic, et al. (2010) investigated the removal ozonation was added. Schaar, et al. (2010) reported that the of endocrine disruptors from paper mill waste using upgrade of an Austrian municipal WWTP for nitrogen anaerobic and aerobic biological treatment, MBR, ultra- removal also reduced the concentrations of many filtration, reverse osmosis, and AOPs. The AOPs were micropollutants, but was not sufficient to completely found to remove 70 - 100% of the endocrine disruptors. eliminate them. Subsequently, application of ozonation to

Combinations of Treatment Technologies. additionally treat the effluent increased removal of

Researchers have clearly determined that a multibarrier micropollutants, but authors noted that iodated contrast approach to treatment of emerging pollutants is an media were not removed by this combination of treatment appropriate means to provide excellent removal of a wide processes. Rosal, et al. (2010) reported on the occurrence of range of compounds. A conceptual and integrated analysis emerging pollutants in an urban WWTP and their removal of the upflow anaerobic sludge blanket/polishing pond by biological treatment followed by ozonation. Results

(UASB/PP) system was presented in relation to the removal showed that paraxanthine, caffeine and acetaminophen of specific constituents not normally covered in literature, were the primary pollutants found at concentrations over 20 namely surfactants, the micropollutants including phthalate parts per billion (ppb); N-formyl-4-amino- antipiryne and and bisphenol A, and sulfide (Chernicharo, et al., 2010). galaxolide were also detected at ppb concentrations. A

Experimental studies on a small full-scale UASB/PP group of compounds including beta-blockers, lipid system have shown limited overall removal efficiencies for regulators, antibiotics, antiinflammatories, an antiepileptic, some constituents (53% to 70% for phthalates and 50% for and an anti-acid exhibited removal efficiencies below 20%

LAS), but excellent removal levels for bisphenol A (around in the WWTP. Ozonation improved the removal of many of

99%) and sulfide (no trace concentrations were detected in these pollutants that were refractory to biological treatment. the second and third ponds of the series). Avila, et al. Reungoat, et al. (2010a, 2010b) studied the biological and

(2010) reported on performance of an anaerobic reactor chemical quality of water produced based on the followed by parallel constucted wetlands. Sorbtion of combination of ozonation and activated carbon filtration at

PPCPs to particulate matter and biodegradation in wetlands a full-scale reclamation plant. Analysis for the detection of result in high TSS removal and selected PPCPs pathogens, quantification of pharmaceutical and pesticide

In many studies, ozonation was applied following micropollutants, and bioassays to evaluate the level of treatment and significantly improved removal of target various adverse biological effects were performed. Results compounds. Mascolo, et al. (2010) investigated the removal suggested that reclaimed water comparable to the quality of 28 organic compounds in water using conventional produced by reverse osmosis was produced by the

1943 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation combination of ozonation and activated carbon treatments. a factor of up to 1.8. The authors believed the discrepancy

Macova, et al. (2010) used a battery of bioassays to could be relieved by improving eliminating strategies in evaluate the toxicity effects of treated effluent from various natural aquatic environment and WWTP (photolysis and wastewater processes; results of the work showed that biodegradation). Letzel, et al. (2010) investigated activated carbon filtration provided significant removal of occurrence and fate of ritalinic acid in wastewater, surface the toxic effects of micropollutants with ozonation resulting water and bank filtrate. They found low removal rates in in complete removal as measured by the bioassays. WWTPs resulted in ritalinic acid being detected in German

rivers at concentrations of 4–23 ng/L and in bank filtrate. A

Fate and Transport of Emerging Pollutants comparison to available sales data shows that a significant

Methods for tracking wastewater-derived amount of methylphenidate applied can be found as the contaminants to the environment continue to improve. stable metabolite, ritalinic acid, in the environment.

Lawrence and Bariel (2010) and Lawrence (2010) Schirmer, et al. (2010) also provided a summary of studies monitored the discharge of the conservative wastewater on transport and fate of xenobiotics in the urban water tracer anthropogenic gadolinium which is used as an MRI cycle in Halle/Saale and Leipzig (Germany). contrast agent. They examined the transport of gadolinium Metcalfe, et al. (2010b) evaluated the occurrence from a WWTP in Toowoomba, Queensland, Australia, into of 6 antidepressants of 5 of their metabolites in wastewater, a creek and finally into a river which is a source for sewer water, and drinking water and caged flathead drinking water. A detectable wastewater contribution minnows. Although concentrations of the compounds were within the drinking water supply was reported and up to 3% present in the river water and raw drinking water, the wastewater was detected up to 100 kilometers away from compounds were not detected in the final drinking water. the point source. The technique was also used to study the Further, venlafaxine and its metabotes did not estuarine mixing of wastewater in Moreton Bay, bioaccumulate in the minnows despite high concentrations

Queensland; Lawrence (2010) further demonstrated the of these compounds in the sewer water and the authors applicability of this technique for wastewater effluent questioned if metabolite presence was due to uptake or tracking in marine samples. These kinds of tools as well as invivo metabolism. In another study, however, in which more conventional methods are useful for evaluating Ashauer, et al. (2010) evaluated the uptake and elimination environmental fate and transport of emerging pollutants. rate constants, bioaccumulation factors, and elimination

In aqueous samples, Alder, et al. (2010) times in the freshwater arthropod Gammarus pulex for 14 compared modeled β-blocker concentrations in a watershed organic micropollutants covering a wide range of to measured values and found the model (greatly) over- hydrophobicity, several compounds showed unexpectedly predicted the actual β-blocker concentrations measured by long elimination times. Kallio, et al. (2010) evalutated the

1944 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation metabolites of diclofenac in fish bile and their findings control on the concentrations of both pharmaceuticals and suggested that fish living downstream of WWTPs are biodegradation is less important. chronically exposed to the drug; both the drug and its In biosolids, Maoz and Chefetz (2010) evaluated metabolites may accumulate in the fish bile. Vernouillet, et the role and mechanism of interaction of the al. (2010) evaluated several organisms from different tropic pharmaceuticals naproxen and carbamazepine with levels to determine the toxic effects of carbamazepine and structural fractions of biosolids-derived organic matter, documented bioaccumulation in the test organisms. demonstrating that hydrophobic fractions were more

“Statin” drugs inhibit the liver enzyme efficient at sorbing naproxen and carbamazepine, and controlling cholesterol synthesis, are exclusively used for probably other pharmaceutical compounds, than the more human use and are not extensively metabolized by the polar hydrophilic fractions at a pH near the pKa of the body. Therefore, Ottmar, et al. (2010b) evaluated statin analytes. Lahnsteiner and Vranitzky (2010) have evaluated absorption affecting its fate in environmental systems and the use of ozone for treatment of organic micropollutants in found a linear relationship between pharmaceutical sewage sludge. Because biosolids are often applied to soils, distribution for several sorbents and organic matter researchers have investigated the fate and transport of concentration in wastewater. Siemens, et al. (2010) emerging contaminants between these media. Kwon, et al. conducted leaching studies and effects of naproxen, (2010) evaluated the adsorption and in-situ biological ibuprofen, benzafibrate, diclofenac, gemfibrocil, treamtent of antibacterial agents in soil with and without clarithromycin, trimethroprim, clindamycin, erythromycin, biosolids amendment. The target compounds were and metaprolol in column experiments showing that there is susceptible to biological transformation, but the presence of considerable risk that all of these are leached to biosolids slowed the transformation of both compounds. groundwater and that these compounds can contribute to Karnjanapiboonwong, et al. (2010) assessed the sorption of increased soil carbon dioxide emissions by 50% one day estrone, 17β-estradiol, estriol, 17α-ethynylestradiol, after application. Einsiedl, et al. (2010) investigated triclosan, and caffeine to two loam soils and Ottawa sand ibuprofen and diclofenac in a karst groundwater system. was assessed. Xu, et al. (2010) also evaluated the impact of

Both pharmaceuticals were detected in effluent water of the dissolved organic matter, polyacrylanides and salinity on

WWTPs and diclofenac was detected in most springs NSAID leaching and no significant difference in leaching discharging the groundwater to rivers while ibuprofen was was observed compared to the distilled water control. rarely detected in groundwater. Both pharmaceuticals are However, the loss of NSAIDs from soil was mainly due to thought move into the fractured system of the karst system degradation rather than leaching. Peterson, et al. (2010) and into storage; dilution processes are the dominant conducted experiments with ampicillin and α-alumina

particles at different pH conditions to evaluate transport in

1945 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation soil–water systems; results showed that transport is hydroponic conditions showing that plants that are controlled in part by adsorption to nanometer-size particles consumed by humans can bioaccumulate pharmaceutical with weak electrostatic forces dominating at low pH and compounds. al-Ansari et al., (2010) reported that 17α- stronger attachment mechanisms at higher pH. Gibson, et ethynylestradiol concentrations were measured in shorthead al. (2010) investigated the impact of irrigation with redhorse suckers collected from a WWTP outfall and untreated wastewater and how it introduces PPCPs to the downstream of the outfall in the St. Clair River in Canada. terrestrial environment. Acidic pharmaceuticals and The compound was detected in 50% of the samples from endocrine disruptors did not accumulate in the soil, but the WWTP site and none from the downstream reference carbamazepine was present at a number of soil horizons, site and mean wert weight 17α-ethynylestradiol suggesting its mobility in the environment. Al-Rajab, et al. concentrations in male and female were 1.64 and 1.43

(2010b) evaluated the environmental fate of diclofenac nanograms per gram (ng/g), respectively. through the application of municipal biosolids or While much research on the fate of emerging wastewater in the laboratory with findings indicating that pollutants has focused on specific media, trends toward diclofenac is readily biodegradable in agricultural soils. disposal of various PPCPs and other emerging

Other researchers have determined the degradation rate and contaminants in landfills have prompted research on the half-lives of twelve micropollutants in biosolids under fate of these compounds in landfills. Reinhart, et al. (2010) thermophilic composting conditions (Poulsen and Bester, conducted an assessment and reported on the fate of

2010). In this study, the half-lives of compounds ranged nanomaterials within landfills. from 20 to 110 days and degradation was not observed for triphenyl phosphate. Also, in other solid media, sorption Microorganisms and Antibiotic Resistance kinetics and exchangeable value of carbamazepine was In addition to chemical compounds, there are assessed for river sediment and river sediment amended emerging concerns regarding the presence of newly with charcoal, showing that the isotopic exchangeability identified microorganisms as well as antibiotic resistant could be used as a measure of the available fraction of microorganisms in the environment. Riner, et al. (2010) carbamazepine (Williams and Kookana, 2010). identified Cyclospora cayetanensis as a protozoan of

Ultimately, emerging pollutants may end up in emerging concern. It causes self-limiting gastroenteritis in plants and other organisms. Jones-Lepp, et al. (2010) immune-competent hosts and transmission via drinking or developed a method and applied it to demonstrate the recreational water has been reported in the US. Fuentefria, potential plant uptake of antibiotics and other drugs in et al. (2010) evaluated the contribution of untreated irrigated crops. Herklotz, et al. (2010) evaluated the uptake hospital wastewater to the dissemination of resistant of human pharmaceuticals by plants grown under Pseudomonas aeruginosa strains in aquatic environments

1946 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation through the analysis of their antibiotic susceptibility profile identify the partitioning of various compounds into and genetic similarity. The antibiotic resistance was higher compartments. A one-year, multi-compartment water among the hospital wastewater strains; no genetic similarity monitoring program was conducted with statistical analyses among the Pseudomonas aeruginosa strains from the indicating that compartmental correlations existed for the hospital wastewater and superficial water samples were antibiotics evaluated in the study (Musolff, et al., 2010). In found and genetically distinct populations were established another study, Trapp, et al. (2010) developed a system of in these different environments indicating that some other equations, based on activity and analogous to the fugacity contamination source could be contributing to the presence approach, to describe the fate of organic ionics, including of resistant strains in these water bodies. Pignato, et al. pesticides, pharmaceuticals, and personal care products.

(2010) conducted a molecular epidemiology study at local Understanding overall environmental partitioning scale in Sicily, Italy of ampicillin resistance in Salmonella of these compounds, including potential loading to spp. isolates from municipal wastewater and clinical treatment facilities is important. Ottmar, et al. (2010a) specimens with previously examined Escherichia coli developed a mass balance model to estimate prescription isolates from wastewater. Analysis of isolates from pharmaceutical loadings to municipal WWTPs; model wastewater were demonstrated to be a useful epidemiologic results were consistent with measured results within about tool to monitor the prevalence of antibiotic resistance and an order of magnitude for 90% of compounds evaluated. genetic elements related to antibiotic resistance in Rowsell, et al. (2010) estimated micropollutant levels in

Salmonella clones circulating in the human population. WWTP influents and reported accuracy between 77 and

Also, to determine if wastewater effluent inputs result in 100%. Based on data for more than 600 WWTPs in detectable and stable changes in antibiotic resistances England, the authors demonstrated that compounds such as downstream WWTPs, Akiyama, et al. (2010) studied the di(2-ethylhexyl) phthalate, lead, and linear alkyl- antibiotic resistance of Escherichia coli and total coliform benzenesulfonates could reach influent levels that are bacteria in stream water and sediment using a culture-based challenging for conventional wastewater treatment. Mullot, method. Their results indicated that antibiotic resistant et al. (2010) conducted a study three French hospitals in bacteria are entering the stream, but resistances change order to assess and model the pharmaceutical load in within a short distance of effluent inputs, more quickly than hospital wastewater and its impact in WWTPs. Comparison indicated based on chemical water properties. of measured and calculated concentrations, a satisfactory

correlation could be observed for some pharmaceuticals,

Modeling mainly those with short elimination half-lifes and weak

With regard to understanding emerging pollutants human metabolism, however, for other compounds, the in the environment, researchers have developed models to authors determined that modeling should take into account

1947 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation factors such as outpatient use, pharmacokinetic data and their models predicted the carbon loading of most solutes molecule stability in wastewater. Modeling has also been within 0.5 log unit deviation from measured values. conducted to estimate the potential for treatment of these Electrocoagulation is a technique gaining attention for compounds. Plosz, et al. (2010) developed a model to removal of emerging pollutants from water and wastewater; predict the removal of the antibiotic micropollutants, Robic and Miranda (2010) correlated current applied sulfamethoxazole, tetracycline, and ciprofloxacin, in an between the electrodes to the removal of phenolic activated sludge treatment system. Their evaluation of compounds or protein from aqueous solutions; they measured and simulation results suggested that, robust developed a model that showed good agreement with model prediction can be achieved by approximating the experimental data and that pH had the most significant influent load of chemicals biodegrading via a given parent effect on the efficiency of removal. compound, e.g., human conjugates, as an antibiotic mass For membrane treatment, Yangali-Quintanilla, et that is proportional to the parent compound load. To assist al., (2010a, 2010b) conducted principal component analysis with the elucidation of biological transformation products to find a quantitative structure-activity relationship (QSAR) produced during microbially-mediated reactions, Helbling, model equation that combines interactions between et al. (2010) developed an integrated experimental, membrane characteristics and solute properties for analytical and post-acquisition data processing procedure predicting rejection of emerging contaminants by NF which was used to identify 26 transformations products, of membranes. Membrane characteristics related to which many were previously unidentified. With regard to hydrophobicity, salt rejection, and surface charge, treatment using sorption processes, Worch (2010) used two compound properties describing hydrophobicity, polarity, user-oriented model approaches to overcome the size (molar volume, molecular length, molecular depth, difficulties in modeling the competitive adsorption in equivalent width, molecular weight), and membrane multi-component systems. These model approaches, as well operating conditions (flux, pressure, cross flow velocity) as a simplified model for batch processes, are compared for were identified and evaluated as candidate variables for the adsorption of atrazine and diuron, from Elbe River rejection prediction. Nothe, et al. (2010) developed a model water onto activated carbon. A multivariate linear to simulate the kinetics of the reaction of ozone with regression model was developed by de Ridder, et al. (2010) degradation of micropollutants; the authors found that to predict equilibrium carbon loading on activated carbon reaction kinetics can generally be adequately described by for a variety of solutes. Solute hydrophobicity, two components and their respective rate constants. polarizability, aromaticity and the presence of hydrogen- Diclofenac, which is degraded fast, and bezafibrate, which bond donor/acceptor groups were examined as properties is degraded moderately fast, this model describes their that affect activated carbon sorption. They determined that measured elimination well.

1948 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Other researchers, including Papa, et al. (2010) zone designation, classification, grading and scheduling to have worked to develop models to characterize the aid in managing estuarine ecosystem health. environmental and toxicological profiles of new and emerging pollutants with endocrine disruption behavior Toxicity such as brominated flame retardants. The QSAR models The environmental impact with regard to toxicity were developed in an effort to improve the regulatory and other ecological effects is a topic of much research acceptance of QSARs as a simple tool for the screening and including studies on methods for evaluating toxic effects. characterization of brominated flame retardants. Diniz, et Constantine and Huggett (2010) conducted a comparison of al. (2010) reported on the assessment of estrogenic potency the chronic effects of human pharmaceuticals on Daphnia in a Portuguese WWTP using an integrated approach magna and Ceriodaphnia dubia, showing that C. dubia may

A model for prediction of the removal of be a more sensitive invertebrate species when assessing the micropollutants in stormwater treatment systems was potential risks associated with the toxicity of human presented by Vezzaro, et al. (2010). Based on the most pharmaceuticals. The issue of toxicity is complicated by relevant removal processes—settling, volatilization, properties of emerging pollutants such as chiral drugs, sorption, biodegradation, and abiotic degradation—the which can exist in the form of enantiomers, which have model allows dynamic simulation of micropollutant similar physicochemical properties but differ in their behavior in different treatment systems. De Keyser, et al. biological properties such as distribution, metabolism and

(2010) combined a multimedia fate and transport model excretion. Due to stereospecific interactions of enantiomers with an integrated urban water system model to simulate with biological systems, these processes usually favor one the fate of bis(2-ethylhexyl) phthalate (DEHP) with and enantiomer over the other (Kasprzyk-Hordern, 2010). And, without stormwater infiltration ponds indicating that degradation of chiral drugs during wastewater treatment inclusion of infiltration ponds decreased mass fluxes to and in the environment can be stereoselective and can lead downstream water bodies and soil, and increased to chiral products of varied toxicity. groundwater and air compartment DEHP concentrations Racz and Goel (2010) provided a discussion of and fate of micropollutants was based on their properties. the physiological effects of estrogens, the degree of

In an effort to develop a pragmatic approach to problems they pose, the fate of estrogens in wastewater managing drainage basin scale ecosystem health, Meng, et treatment systems and how they may reach drinking water al. (2010) presents some points of view on the approach of sources and they also discussed treatment technologies and estuarine ecosystem health scientific research based project future research trends. Toxicity testing for a number of experience of the Chinese Research Academy of emerging pollutants has indicated relatively low acute

Environmental Sciences using information about functional toxicity to fish species, but no information is available on

1949 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation possible sublethal effects. Thus, Hampel, et al. (2010) present. The toxicological impacts of untreated, treated and studied the physiological pathways involved in the blended pulp and paper mill effluents have been assessed exposure of Atlantic salmon as representative test species using egg production, somatic parameters, and gene to acetaminophen, carbamazepine, and atenolol and found expression of flathead minnows (Werner et al., 2010). that 5 day exposure produced differences in the expression Toxicity can result in interruption of normal of 659, 700, and 480 candidate genes. Song, et al. (2010) metabolic and reproductive activity in some organisms. evaluated the cellular transmembrane distribution and Sole, et al. (2010) studied the exposure of marine mussels toxicological effects of kanamycin and chloramphenicol in to propranolol and acetaminophen and they examined the efforts to gain insight into cytotoxicity of antibacterial responses of Mytilus galloprovincialis as a sentinel species drugs. The new method that the researchers developed to test the effects on a behavior parameter, xenobiotic could be useful for evaluating the interactions of toxins metabolism and oxidative stress. Some enzymatic activities with cellular membranes and elucidating the mechanisms in liver were reduced after propranolol exposure whereas of cytotoxicity in aquatic organisms. acetaminophen enhanced them. Nishi, et al. (2010)

Nassef, et al. (2010) examined the toxicity of measured the in vitro cyclooxygenase (COX)-inhibiting three PPCPs – triclosan, diclofenac, and carbamazepine – activity of the surface water and domestic wastewater in the on embryonic development of Japanese medaka (Oryzias Tone Canal, Japan. A dose–response relationship between latipes) using in ovo nanoinjection. They concluded that the inhibiting activity and sample volume were observed in the nanoinjection medaka embryos model is a valuable tool the wastewater sample. The higher COX-inhibiting for analyzing the effects of chemicals on the development activities were observed in the wastewater sample, as of fish embryos and feasibility of nanoinjecting PPCPs into compared with the samples of the surface water in the small fish eggs perhaps mimicking early exposure resulting canal. Xenoestrogen exposure and toxicological effects from oocyte uptake of contaminants from maternal extra were studied in the Reedy River Basin of Greenville, South gonadal tissues. Vermeirssen, et al. (2010) sampled 21 final Carolina, by Truman and van den Hurk (2010) who effluents with POCISs. They investigated whether an examined bluegill (Lepomis macrochirus) for association could be found between data from biological xenoestrogenic exposure and vitellogenin production in and chemical analyses of photosystem II (PS-II) inhibitors, juvenile fish. Results were compared to the hepatosomatic and between data from an algal and a bacterial assay for index as a general health parameter and showed that fish baseline toxicity. The authors determined that six collected downstream of the Greenville WWTP had a 4- chemically analyzed PS-II inhibitors explained 65% of the fold induction in bile estrogenic activity as well as a 10- absolute toxicity effect; however, the algal test did not fold induction in plasma vitellogenin relative to a reference identify sites in which nonspecific toxicity was evidently site. Allner, et al. (2010) studied the effect of EDCs in

1950 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation water on the reproductive ability of the two dominant fish transcriptional responses from biofilm microorganisms and species in German surface waters perch (Perca fluviatilis that low concentrations of small molecules can induce

L.) and roach (Rutilus rutilus L.). A statistically significant transcriptional changes in a complex microbial community. elevated proportion of males were observed in fish obtained Rocco, et al. (2010) also showed how the deoxyribonucleic from a tributyl tin contaminated marina and suppression of acid (DNA) of zebrafish can be damaged after exposure to gonadal ripening was observed in females caught in a furosemide, ranitidine, bezafibrate, and ibuprofen at sewage-contaminated brook. Both effects appear to be due concentrations consistent with WWTP effluent. to chemical contamination. Mennigen, et al. (2010) In higher vertebrates, studies also showed investigated the effect of two doses of fluoxetine at potential concerns regarding effects of exposure to environmental concentrations and 100-times this emerging pollutants. Pregnant ewes were maintained on concentration, on feeding and key metabolic parameters in pastures fertilized, twice yearly, with sewage sludge. After goldfish. Fish were exposed for a period of 28 days and 8 months, Lind, et al. (2010) reported that adult ewe femurs changes in food intake and body mass were assessed. exhibited a significantly reduced bone cross sectional area,

Significant decreases in food intake and weight gain were mineral content and mineral density when compared with recorded in goldfish exposed to the high concentration and control animals. In fetal bones, there was a reduction in a significant decrease occurred in circulating glucose levels circumference and marrow cavity area in the female fetuses in the group exposed to the lower concentration. compared with female control fetuses. Wang, et al. (2010)

Bringolf, et al. (2010) evaluated the occurrence, studied whether or not exposure to persistent organic distribution, and bioaccumulation of fluoxetine in water pollutants was related to developing diabetes; results were samples and freshwater mussels downstream of municipal inconclusive and further study was recommended.

WWTPs. Fluoxetine was shown to disrupt reproductive With respect to biosolids, Prado, et al. (2010) chemistry in mussels at high levels (ug/l). Environmentally conducted an evaluation of the toxicity of veterinary relevant levels (ng/l) may result in reproductive disorders antibiotics in activated sludge using modified Sturm Tests. over extended periods of exposure. To test if transcriptional Application of these tests showed a higher tetracycline responses could be observed in complex river microbial biodegradability, which may be related to the molecular communities, biofilm reactors were inoculated with water conformation of tetracycline and tylosine antibiotics, the from two rivers of differing trophic statuses and treated former is constituted of four benzoic cycles hardly with environmentally relevant doses of erythromycin, breakable, while tylosine is constituted of a central gemfibrozil, sulfamethazine, and sulfamethoxazole. structure with attached glycosidic-like fragments which

Yergeau, et al., (2010) demonstrated that pharmaceutical might easily be biologically degraded. treatments induced both positive and negative

1951 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Risk Assessment endocrine disrupting chemicals including estrone, 17β-

Caldwell, et al. (2010), using the Pharmaceutical estradiol, and 17α-ethynylestradiol in an Australian

Assessment and Transport Evaluation model showed that reservoir receiving recycled wastewater. The health risk consistently large margins of exposure and margins of assessment showed that simulated concentrations were safety strongly suggest that prescribed and total estrogens below fish exposure threshold values and human public that may potentially be present in drinking water in the health standards, but the human equivalent dose of

United States are not causing adverse effects in US endocrine disrupting chemicals was about 10 times higher residents, including sensitive subpopulations. O’Brien and than from drinking water consumption.

Cummins (2010) confirmed this finding for nanomaterial There was also research published in 2010 that surface water concentrations and population ingestional developed a quantitative pharmaceutical risk assessment exposure through drinking water resulting from these framework for meprobamate, carbamazepine, and products. They reported high removal efficiencies were for phenytoin during accidental exposures of stream water and

Irish WWTPs and WTP with predicted surface and fish consumption and direct ingestion of finished drinking drinking water concentrations being unlikely to pose any water for children and adults Kumar and Xagoraraki ecotoxicological or human health risk, although nano-scale (2010a, 2010b). The authors also showed that acceptable

TiO2 and silver may warrant monitoring. Munoz, et al. daily intake was the primary contributor in overall

(2010) also reported on the potential health risks derived uncertainties of hazard quotient estimates, followed by fish from wastewater reuse in agriculture; in a case study consumptions and pharmaceutical concentrations in water involving the effluents of two Spanish WWTPs, the overall and also highlighted identified some of the key issues and results showed that risks are lower for the WWTP applying challenges associated with evaluating human health risks. tertiary treatment, especially concerning microbiological While there is growing evidence that there is little parameters. Camacho-Munoz, et al., (2010b) conducted a concern regarding human health risks, other researchers one-year monitoring study to investigate the presence of 16 have documents that there are important considerations for pharmaceuticals in 7 therapeutic groups in wastewater other species. Oakes, et al. (2010) reported that the discharges, rivers and streams affecting Donana Park. serotonin re-uptake inhibitor fluoxetine was selected for an

Fourteen pharmaceuticals were detected in wastewater environmental risk assessment, using the most recent effluent and 13 were detected in surface water; risk European guideline (EMEA 2006) within the EU-funded quotient values in surface water were lower than 1 so no Environmental Risk Assessment of Pharmaceuticals project toxicological effect is suspected to occur. Contrary to other due to its environmental persistence, acute toxicity to studies, Cao, et al. (2010) developed a fugacity based nontarget organisms, and unique pharmacokinetics model and applied it to simulate distribution of three associated with a readily ionizable compound. They

1952 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation reported that current monitoring techniques are flawed by states and the District of Columbia, were analyzed and an over-reliance on partition coefficients that are not thirty-eight (54%) of the 72 analytes were detected in at applicable at environmental pH values. Zhou, et al. (2010b) least one composite sample. Langdon, et al. (2010) reported on 9 pharmaceutical compounds in WWTP presented a screening-level assessment to determine the effluent and their receiving waters; target pharmaceuticals relative hazard posed to aquatic ecosystems by PPCPs and and caffeine were detected in all WWTP and river samples. EDCs in biosolids. This involved estimating maximum

Authors calculated the quotients and found the risk possible runoff water concentrations of compounds, using quotients of carbamazepine, erythromycin, and an equilibrium partitioning approach and then comparing trimethropim were greater than 1 in wastewater influent these with the lowest available aquatic toxicity data, using and effluent, suggesting a chronic aquatic environmental the hazard quotient (HQ) approach. risk that is not decreased by treatment (Zhou et al. 2010a).

Kar and Roy (2010) reported on interspecies toxicity Regulation correlations for estimating contaminant sensitivity with Bottini, et al. (2010) conducted a review of known levels of uncertainty for a diversity of wildlife emerging contaminants and based on the information species. In this context, the authors have developed toxicity presented made specific recommendations that the correlations between Daphnia magna (zooplankton) and inclusion of emerging pharmaceuticals in the revision of fish by assessing the ecotoxicological hazard potential of EU List of Priority Substances under the Water Framework

77 diverse pharmaceuticals. Ginebrida, et al. (2010) also Directive 2000/60/EC should be implemented as well as the reported on relationships between Hazard Indexes and definition of respective environmental quality standards. aquatic macroinvertebrate diversity indexes in the Perazzolo, et al. (2010) developed a framework to identify

Llobregat River (Spain) through risk assessment analysis. priority micropollutants, which included prediction of

With respect to risks from exposure to pollutants environmental concentrations. Thus, the researchers in biosolids, the U.S. National Academies called for a identified potential drugs due to manufacturing patterns, better assessment of chemical pollutants contained in the predicted environmental concentration, predicted approximately 7 million dry tons of digested municipal environmental consumption including excretion, predicted sludge produced annually in the US. The mean the impacts of degradation in WWTP, and the impacts of concentrations of 72 PPCPs were determined in 110 environmental dilution on pollutant presence and biosolids samples collected by the US Environmental concentration. However, the framework needs information

Protection Agency in its 2001 National Sewage Sludge regarding consumption and that information is considered

Survey (McClellan and Halden, 2010). Composite samples confidential data as wells as physicochemical, metabolic, of archived biosolids, collected at 94 US WWTPs from 32 and ecotoxicological data for the constituents identified.

1953 Water Environment Research, Volume 83, Number 10—Copyright © 2011 Water Environment Federation Schriks, et al. (2010) derived provisional drinking Ultrafiltration and Nanofiltration. Chem. Eng. J. water guideline values for a selection of 50 emerging (Amsterdam, Neth.), 163 (3), 264–272. contaminants based upon toxicological literature data. Achilleos, A.; Hapeshi, E.; Xekoukoulotakis, N. P.;

Comparing the maximum concentration levels reported in Mantzavinos, D.; Fatta-Kassinos, D. (2010) UV- surface waters, groundwater and/or drinking water were A and Solar Photodegradation of Ibuprofen and using data in the downstream parts of the Rhine and Meuse Carbamazepine Catalyzed TiO2. Sep. Sci. river basins showed that, the majority of the compounds Technol., 45 (11), 1564–1570. evaluated pose individually no appreciable concern to Akiyama, T.; Savin, M. C. (2010) Populations of human health. Antibiotic-Resistant Coliform Bacteria Change

Rapidly in a Wastewater Effluent Dominated

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their Removal through Biological Treatment Technol, 62 (12), 2862–2871.

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