Human and Ecological Risk Assessment: An International Journal

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Arsenic and Heavy Metal Concentrations in Drinking Water in and Risk Assessment: A Case Study

Sardar Khan, Irfan Ali Shah, Said Muhammad, Riffat Naseem Malik & Mohammad Tahir Shah

To cite this article: Sardar Khan, Irfan Ali Shah, Said Muhammad, Riffat Naseem Malik & Mohammad Tahir Shah (2015) Arsenic and Heavy Metal Concentrations in Drinking Water in Pakistan and Risk Assessment: A Case Study, Human and Ecological Risk Assessment: An International Journal, 21:4, 1020-1031, DOI: 10.1080/10807039.2014.950925 To link to this article: https://doi.org/10.1080/10807039.2014.950925

View supplementary material Accepted author version posted online: 08 Aug 2014. Published online: 06 Dec 2014.

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Arsenic and Heavy Metal Concentrations in Drinking Water in Pakistan and Risk Assessment: A Case Study

Sardar Khan,1 Irfan Ali Shah,1 Said Muhammad,2 Riffat Naseem Malik,3 and Mohammad Tahir Shah4 1Department of Environmental Sciences, University of Peshawar, Peshawar, Pakistan; 2Department of Earth Sciences, COMSATS Institute of Information Technology, Abbottabad, Pakistan; 3Environmental Biology and Ecotoxicology Laboratory, Department of Environmental Sciences, Faculty of Biological Sciences, Quaid-I-Azam University, Islamabad, Pakistan; 4National Center of Excellence in , University of Peshawar, Peshawar, Pakistan

ABSTRACT The present study was performed to assess drinking water quality and poten- tial health risk in the Nowshera District, , Pakistan. For this purpose drinking water samples were collected from local available sources and an- alyzed for physico-chemical characteristics, arsenic (As) and heavy metals. Results revealed high levels of toxic heavy metals such as chromium (Cr), nickel (Ni), lead (Pb), cadmium (Cd), and As contaminations in the drinking water. Results were evaluated for chronic risk including average daily intake (ADI) and hazard quotient (HQ). Among heavy metals the HQ values were highest for Cd (5.80) and As (2.00). Therefore, populations in the study area may be at a low level of chronic toxicity and carcinogenic risk. Statistical analyses showed that contribution of different drinking water sources to the mean contaminant levels in the study area was insignificant (p = .53). Correlation analysis further revealed that anthropogenic activities were the main sources of contamination, rather than geogenic. This study strongly recom- mends the treatment of urban and industrial wastewater in the vicinity of the study area and provision of safe drinking water. Key Words: drinking water, hazard quotient, average daily intake, cancer risk, statistical analyses, Nowshera District.

Received 8 March 2014; revised manuscript accepted 28 July 2014. Address correspondence to Sardar Khan, Department of Environmental Sciences, Univer- sity of Peshawar, Peshawar 25120, Pakistan. E-mail: [email protected]; or to Said Muhammad, Department of Earth Sciences, COMSATS Institute of Information Technology, Abbottabad 22060, Pakistan. E-mail: [email protected] Color versions of one or more of the figures in the article can be found online at www. tandfonline.com/bher.

1020 Arsenic and Heavy Health Risk Assessment via Drinking Water

INTRODUCTION Drinking water contaminations have both natural (ore deposits, rocks weather- ing, and erosion) and anthropogenic (industries, mining, agriculture activities, and wastewater) origins (Muhammad et al. 2010; Khan et al. 2013; Li et al. 2014). Among contaminants the heavy metals are of global concern, which find their ways into water and food, impairing their quality and cause toxicity (Shah et al. 2012; Spayd et al. 2012; Hu et al. 2014). Among metals, sodium (Na), calcium (Ca), magnesium (Mg), zinc (Zn), cobalt (Co), iron (Fe) and copper (Cu) are essential and required at certain concentrations for normal body function and growth. However, others such as As, Cd, Ni, and Pb are non-essentials or toxic metals and causing numerous human health risks after ingestion (Muhammad et al. 2010, 2011). Toxic effects of these metals include abdominal pain, headache, irritability, blood pressure, kidney damage, nerve damages, skeletal damage, cancer, and affects intellectual functions (Khan et al. 2013). Characteristically, heavy metals are mostly carcinogenic in na- ture but their toxicity and targeted organs vary from metal to metal and also depend on the ingested amount, body immunity of the individual, and exposure duration (Goyer et al. 2004). Heavy metals enter into the human body through several path- ways. However, oral ingestion, especially through drinking water, is one of the major sources for human exposure (Spayd et al. 2012; Khan et al. 2013). Humans need drinking water for sustaining life and social prosperity. Provision of clean water supplies is a high priority issue for safe guarding a population’s health (Simeonov et al. 2002). Clean drinking water and its adequate supply is a key factor contributing to decreased mortality and morbidity and improved economic development in the developing countries (Koc 2010). Therefore, human health risk assessment through drinking water consumption has become the prime focus of environmental researchers globally (Spayd et al. 2012). Being a developing country, Pakistan is facing a serious crisis in the supply of clean and safe portable water in its urban and rural areas. In the past, few studies have been reported on the drinking water contaminations in the northern region of Pakistan (Muhammad et al. 2010, 2011; Shah et al. 2012; Khan et al. 2013). Although, the Nowshera District hosts a population of more than 1.2 million, no research has been carried out on drinking water quality and it potential health risk. Therefore, this study aimed to identify the sources of drinking water contaminations and their potential health risk assessment in the selected district.

METHODS AND MATERIALS Study Area The Nowshera District is located along the banks of the Kabul River and lies between 33◦–41 to 34◦–10 N latitudes and 71◦–39 to 72◦–16 E longitudes, with a total area of 1748 km2 (Figure 1). It is bounded on the east by the Attock Dis- trict of Punjab Province, on the west by Peshawar and on the northwest side by Charsadda, while on the northern side by the Mardan and Swabi Districts and on the south by the Kohat District. The district is cold (4◦C) in winter and very warm (43◦C) in the summer, receiving an annual precipitation of 600 mm. Generally, depth in water tables varies from 13–50 meters. The main professions of the local

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Figure 1. Map of the study area showing locations of the sampling sites.

residents are agriculture, business and jobs in government institute, or the Aman- garh Industrial Estate (AIE). The AIE hosts a number of paper, textile, ceramics, tanneries, and ghee industries. The Kabul River enters this district at its western side and runs through the plain and joins the Indus River at a kund near Khairabad (DCR 1998).

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Water Samplings and Analyses Inhabitants of the Nowshera District are using tube wells, bore wells, dug wells, and hand pumps as sources of water for drinking purposes. The district was classified into 39 sampling sites and each site into three spots (Figure 1). From each spot, water was collected in two plastic bottles. Basic parameters such as pH and electrical conductivity (EC) were measured on the spot using water quality checker U-10 Horriba-Japan. The location of each sampling site was noted using a global positional system (GPS). Water of one bottle was acidified at each sampling spot for As and heavy metal analyses, while another bottle was non-acidified and tested for anions including nitrate (NO3), sulphate (SO4), and chloride (Cl). Collected samples were transported and stored in the dark at 4◦C for further analyses (APHA 2005).

Nitrate, SO4, and Cl were measured in non-acidified samples by the titration method adopted from the American Public Health Association (APHA 2005). Light metals (Na, K, Ca, and Mg) and heavy metals (Pb, Cu, Cr, Ni, Cd, and Zn) were measured using a graphite atomic absorption spectrophotometer (Perkin Elmer, AAS-PEA-700), while As concentrations were measured using a mercury hydride system (MHS). Analyses were performed in triplicate. Reproducibility was found to be at 95% confidence level. Therefore, mean values of samples were used for results interpre- tation. Reliability and reproducibility of analyses were checked by analyzing blank and known standards after every 10 samples. Chemicals (acids and reagents) used in samples’ analyses were of analytical grade and purchased from MERCK & Co., Inc. All analyses were performed in the laboratory of the National Centre of Excellence in Geology (NCEG), University of Peshawar, Pakistan.

Potential Risk Assessment Exposure assessment For exposure assessment of the study area, the average daily intake (ADI) of metals through drinking consumptions is calculated according to the equation adopted from the U.S. Environmental Protection Agency (USEPA 1998) and Shah et al. (2012).

ADI = CW × IR × EF × ED/BW × AT (1) where CW is the concentration of metals in water (mg/L), EF is the exposure frequency (365 days/year), IR is the ingestion rate of water (L/day), ED is expo- sure duration (30 years), BW is bodyweight (60 kg), and AT is averaging time, i.e., 365 days/year × ED for non-carcinogens and 365 days/year × 70 years for carcino- gens (ATSDR 2008; WHO 2011; Shah et al. 2012).

Risk assessment Chronic risk level was calculated using the following equation adopted from USEPA (1998) and Muhammad et al. (2011).

HQ = ADI/RfD (2) where HQ is the hazard quotient and RfD is the reference dose (mg/kg-day).

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The carcinogenic risk level was calculated using following formula: CR = ADI × CF (3) where CR is the cancer risk and CSF is the cancer slope factor (mg/kg-day–1). The CSF value of As is 1.5 mg kg–1 day–1 as adopted from USEPA (2005) and Muhammad et al. (2010).

Statistical analyses Data were analyzed statistically for means, range, standard deviation, one-way Analysis of Variance (ANOVA), and Pearson’s correlation using MS Excel (2007) and SPSS 18 (SPSS Inc., Chicago, IL, USA).

RESULTS AND DISCUSSION Physico-Chemical Parameters Summarized in Table S1 (see the online supplementary information) are the concentrations of physico-chemical parameters in drinking water of the Nowshera District. The minimum (5.7) value of pH was found in tube well water at Umaray, with maximum (7.3) in dug wells at the Nowshera cantonment and hand pump at Pabbi. The drinking water of the study area was slightly acidic. Among water quality param- eters, pH is one of the important indicators of contamination level in an aquatic system (Jonnalagadda and Mhere 2001) and affects water quality (viz., pathogens survival and metal solubility). EC values were observed lowest (276.0 µS/cm) in tube well water at Manahi, while highest (2400.0 µS/cm) in tube well water at Umaray. The values of pH and EC were observed to be within the safe drinking water guide- lines of Pak EPA (2008) and WHO (2011). However, 12% of sampling sites surpassed the safe limit of EC. Tube well water showed higher EC values as compared to other sources of drinking water. The EC qualitatively estimates the contamination level in water (viz., ionized species and inorganic dissolved solids) (Jonnalagadda and Mhere 2001). Water chemistry is subjective to bed rock and contaminant sources in the vicinity of an area (Muhammad et al. 2010; Shah et al. 2012). Dissolution of in rain water is mainly responsible for the metal contents in groundwater. These metals’ concentrations are affected by the of the aquifer and water residence time. As a result deeper groundwater can feel prominent changes in elemental composition with increasing residence time (Edmunds et al. 1987; Shah et al. 2012). Chloride concentrations were found lowermost (21.0 mg/L) in tube well water at Akora Khattak, while uppermost (200.0 mg/L) in dug well water at Risalpur.

Similarly, NO3 values were found minimum (1.5 mg/L) in hand pump water at Adamzai, while maximum (55.0 mg/L) in tube well water at Hisartang village.

This higher concentration of NO3 in tube well water may be attributed to extensive agriculture practices in Hisartang village and surrounding. SO4 concentrations were observed highest (68.0 mg/L) in bore well water at Ziarat KaKa Sahib, while lowest

(5.0) in Kheshgi, Risalpur, Shekhan, and so on. Highest SO4 concentrations in bore well water at Ziarat KaKa Sahib may be attributed to sulphide mineralization and fertilizer based agriculture practices in the vicinity. The concentrations of Cl,

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SO4,andNO3 were found to be within the drinking water guidelines suggested by domestic and international organizations such as Pak EPA (2008) and WHO (2011) (Table S1). Sodium concentrations ranged from 7.0–50.2 mg/L (Table S1). Highest (50.2 mg/L) Na concentrations were found in dug well water at Kanra Khel. Similarly, K concentrations ranged from 0.7–14.2 mg/L (Table S1). Maximum (14.2 mg/L) K concentrations were noted in bore well water at Badrashi. The concentrations of Ca ranged from 9.4–269.8 mg/L (Table S1). Uppermost Ca concentrations were noted in dug well water at Rashakai. Similarly, Mg concen- trations ranged from 3.7–74.2 mg/L (Table S1). Highest (74.2 mg/L) Mg con- centrations were observed in bore well water at the Shaidu village. Shallow water (dug wells and hand pump) sources showed higher concentrations of Na, K, Ca, and Mg as compared to deep water sources. The concentrations of Na, K, Ca, and Mg were found to be within the safe drinking water guidelines of Pak EPA (2008) and WHO (2011). However, 15% and 8% of sampling sites showed anomalies from the limits of Ca and Mg, respectively. Muhammad et al. (2010) reported that light metal such as Na, K, Ca, and Mg are essential elements required for human and their deficiency may cause health problem (e.g., low blood pressure, hypertension, depression, fatigue, dehydration, muscle weakness, bladder weakness, kidney prob- lem, and heart problems). Copper concentrations ranged from <0.01–0.03 mg/L (Table S1). Highest (0.03 mg/L) Cu concentrations were found in bore well water at Kher Abad. Cop- per is an essential metal, however, lower or higher concentrations may cause health problems (Dieter et al. 2005; Muhammad et al. 2011). Chromium concentrations ranged from <0.1–1.5 mg/L (Table S1). Uppermost Cr concentrations were noted in water at the AIE area. Like Cu, Cr is also one of the human body’s required metals needed in a specific amount. However, at high concentrations it may cause toxic effects such as kidney and liver problems and cancer (Knight et al. 1997; Loubieres et al. 1999). Nickel concentrations ranged from <0.01–0.3 mg/L (Table S1). Highest Ni concentrations were observed in dug well water at the AIE. In the study area, highest concentrations of Cr and Ni were observed in water collected from the AIE area. These higher concentrations in water may be due to untreated urban and industrial sewage. The intake of Ni compounds at high dose can cause severe health problem such as heart problems (Knight et al. 1997). Chromium and Ni concentrations of the study area were observed higher than those reported by Shah et al. (2012) in drinking water along mafic and ultramafic terrain, Mohmand Agency, Pakistan. The concentrations of Cu were observed to be within the safe drinking water guidelines set by domestic and international organizations (Pak EPA 2008; WHO 2011). However, 75% of sampling sites had surpassed these limits for Cr and Ni. Zinc concentrations ranged in different water sources of the Nowshera District from <0.01–0.5 mg/L (Table S1). Highest (0.5 mg/L) Zn concentrations were found in tube well water at the Hisartang site. Zinc is one of the most essential metals for the human body. Its low concentration may cause deficiency effects such as hair loss, depression, diarrhea, and poor wound healing (Strachan 2010). Lead concentrations in the study area ranged from <0.02–0.3 mg/L (Table S1). Maxi- mum (0.3 mg/L) Pb concentrations were observed in dug well water at the AIE

Hum. Ecol. Risk Assess. Vol. 21, No. 4, 2015 1025 S. Khan et al. area. These high concentrations of Pb in drinking water may be attributed to un- treated domestic and industrial wastewater discharges in the AIE area. Lead is one of the most hazardous metals and is number three in terms of toxicity. Children are the most sensitive to Pb toxicity; it may cause behavioral disturbances, memory problems, and anemia. Other toxic effects include abdominal pain, headache, hy- pertension, irritability, kidney damage, nerve damages, stomach cancer, and lung cancer (Steenland and Boffetta 2000; Mortada et al. 2001; Jarup 2003). Cadmium concentrations ranged from <0.01–0.1 mg/L (Table S1). Uppermost (0.1 mg/L) Cd concentrations were noted in tube wells, bore wells, and dug well water. Highest concentrations of Cd and Pb in drinking water may be due to in- dustrial effluent, domestic sewage, plumbing, and extensive agriculture practices. Groundwater may have higher Cd and Pb contaminations than surface water, as reported (DeZuane 1997; Muhammad et al. 2011). Plumbing is also one of the most important sources of Cd and Pb contaminations in drinking water (Barton et al. 2002; Barton 2005). Cadmium has toxic effects of both short-term (viz., diarrhea, vomiting, and mucous membrane destruction) and long-term (viz., itai-itai disease, bone, and kidney damage) exposure (Jarup 2003; Muhammad et al. 2011). Lead and Cd concentrations of the study area were observed higher than those reported by Muhammad et al. (2011) in drinking water from the Kohistan region, Pakistan. The concentrations of Zn were observed to be within the safe drinking water guidelines suggested by domestic and international organizations such as Pak EPA (2008) and WHO (2011). However, 40% and 90% of sampling sites crossed the limits set for Pb and Cd, respectively. Arsenic concentrations ranged from <0.01–17.58 µg/l (Table S1). Highest As concentrations were observed in tube well water at Pirsabak. Similarly, the As con- centrations were observed to be within the safe drinking water guidelines of Pak EPA (2008) and WHO (2011), except 5% of sampling sites exceeded the WHO limits. Among drinking water contaminants, As is one of the hazardous metalloids that orig- inated from both natural and anthropogenic sources (Baig et al. 2009; Muhammad et al. 2010). High concentrations of As cause toxicity (viz., hypertension and vascular disease, hyperkeratosis, skin lesion, melanosis, and cancer) (Ali and Tarafdar 2003; Fatmi et al. 2009; Rahman et al. 2009; Muhammad et al. 2010).

Potential Risk Assessment People of the study area were interviewed about age, sex, literacy rate, livelihood, health, and drinking water. It was observed that the majority of the population are living in rural areas, have low income and low literacy rate. Residents of the study area cannot afford water (bottled water), therefore, they are using bore wells, dug wells, hand pumps, and tube wells as prime sources of drinking water. That is why these drinking water sources were evaluated for potential risk assessment through exposure assessment (viz., ADI) and risk assessment (viz., HQ and CR).

Exposure Assessment In the study area, ADI values observed the highest (mean 3.3E-02 mg/kg-day) value for Cr in hand pump waters, whereas the lowest (mean 2.9E-05 mg/kg-day) value for As in tube well waters (Table S2). However, other metal ADI mean values

1026 Hum. Ecol. Risk Assess. Vol. 21, No. 4, 2015 Arsenic and Heavy Health Risk Assessment via Drinking Water were noted between the two extremes. The highest ADI values for Cr are due to its high contamination level in drinking water of the study area. This higher ADI of Cr in drinking water may be attributed to severe contamination from urban and industrial sewage and wastewater in the vicinity. These ADI values of the study area were observed much higher than those reported by Shah et al. (2012) for drinking water from the Mohmand Agency, Pakistan.

Risk Assessment Daily intake values of metals were evaluated for the risk assessment through the HQ. The highest HQ value (5.80) was noted for Cd in tube well waters, whereas the lowest (<0.01) was noted for Cu in all water sources (Table S2; Figure 2). Chronic toxicity and carcinogenic risk of metals in the drinking water depends on type, variety, consumption rate, concentration, and toxicity (Kapaj et al. 2006). The highest HQ value for Cd in the study area was due to its low RfD values and high concentration than other toxic metals. Therefore, people of the study area may be at chronic health risk due to drinking of water contaminated with metals. HQ values for the study area were noted to be higher than those reported by Muhammad et al. (2010, 2011) for drinking water in the Kohistan region, Pakistan. The CR values ranged from 1.5E-09–1.3E+06 via drinking water consumption in the study area (Table S2). According to the USEPA, CR values higher than one in a million (10–6) are considered to be significant. However, these values are changed according to the local environmental standards and national policies (USEPA 2000; WHO 2004). Results revealed that drinking water may pose a low risk, when compared with the USEPA approach (1999). In the study area, CR values were much lower than those reported by Nguyen et al. (2009) for drinking water in Vietnam.

Statistical Analyses Statistical comparison of different drinking water contamination using one-way ANOVA revealed that various sources were insignificant (p = 0.53). This showed that all these drinking water sources were contributing nearly equally to the mean contaminations. Inter-relationships of physico-chemical parameters provide inter- esting and valuable information about the sources and pathways of contaminants (Muhammad et al. 2011). Results of correlation matrices for the physico-chemical parameters revealed that selected parameter pairs that showed positive correlations = = = = were Cl-NO3 (r 0.538), Cr-Pb (r 0.574), Cd-Mg (r 0.574), Cd-Mg (r 0.529), and Cd-Ni (r = 0.899) as shown in Table S3. These correlations showed that the major sources of contamination in drinking water in the study area were anthro- pogenic in origin rather than geogenic in nature. Results of this study are consistent with those reported by Shah et al. (2012) and Khan et al. (2013) for drinking water. Pakistan is facing a severe problem in provision of clean and adequate drinking water in its urban areas (e.g., Islamabad, Peshawar, Quetta, and Karachi). The sit- uation is more critical in rural areas due to scattered populations and agriculture practices. In the Nowshera District, the majority of the local population is living in rural areas. Due to low income level and no or little awareness about drinking water the people are using groundwater sources without any pre-treatment. Results from

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Figure 2. Hazard quotient values of heavy metals in the study area.

1028 Hum. Ecol. Risk Assess. Vol. 21, No. 4, 2015 Arsenic and Heavy Health Risk Assessment via Drinking Water this study showed that all drinking water sources were highly contaminated with met- als. Shallow water sources (dug wells and hand pumps) have higher Pb, Cu, Cr, and Zn contaminations. These higher concentrations of shallow water sources may be at- tributed to easy seepage from agriculture and wastewater. However, Ni and Cd have higher concentrations in tube wells and bore wells. Higher concentrations of these contaminants result from plumbing and urban and industrial effluents released in the AIE. This study and some of the previous studies revealed that heavy metals and other chemically contaminated drinking water sources are the main cause of human health risks (Muhammad et al. 2010, 2011; Shah et al. 2012; Khan et al. 2013). Recorded or reported diseases in a field survey of reported studies regarding heavy metals were vomiting, hypertension, low blood pressure, headache, diarrhea, irri- tability, abdominal pain, gastroenteritis, liver and kidney problems, nerve damage, anemia, viral hepatitis, intellectual disabilities, heart problems, and a few cases of cancer (Muhammad et al. 2010, 2011; Shah et al. 2012; Khan et al. 2013).

CONCLUSION Physico-chemical parameters of water from the Nowshera District were to be within the safe drinking water guidelines set by Pak EPA and WHO. However, physico- chemical parameters that surpassed these safe guidelines in different sampling sites were EC (12%), Ca (15%), Mg (8%), Cr (75%), Ni (75%), Pb (40%), Cd (90%), and As (5%). Results revealed that the main contributing factors toward the drinking water contamination were plumbing, industrial wastewater, agriculture practices, and local geology to a lesser extent, as well. The values of ADI were the highest for Cr, whereas HQ values were highest for Cd. This higher intake of toxic metals in drinking water may pose chronic toxicity and carcinogenic risks to the local population. This study strongly recommends the banning of drinking water from contaminated sites and wastewater discharge and provision of safe water for domestic uses.

ACKNOWLEDGMENT We are thankful to HERA’s editor for his kind suggestion on the structure of article.

FUNDING We are thankful to the University of Peshawar, Pakistan for provision of financial support to the authors.

SUPPLEMENTAL MATERIAL Supplemental material for this article can be accessed on the publisher’s website.

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