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Acute Toxicity of Para-Nonylphenol to Saltwater Animals

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Acute Toxicity of Para-Nonylphenol to Saltwater Animals Environmental Toxicology and Chemistry, Vol. 19, No. 3, pp. 617±621, 2000 Printed in the USA 0730-7268/00 $9.00 1 .00 ACUTE TOXICITY OF PARA-NONYLPHENOL TO SALTWATER ANIMALS SUZANNE M. LUSSIER,*² DENISE CHAMPLIN,² JOSEPH LIVOLSI,² SHERRY POUCHER,³ and RICHARD J. PRUELL² ²U.S. Environmental Protection Agency, Atlantic Ecology Division, 27 Tarzwell Drive, Narragansett, Rhode Island 02882 ³Science Applications International Corporation, 221 Third Street, Admiral's Gate, Newport, Rhode Island 02840, USA (Received 25 November 1998; Accepted 14 June 1999) AbstractÐpara-Nonylphenol (PNP), a mixture of alkylphenols used in producing nonionic surfactants, is distributed widely in surface waters and aquatic sediments, where it can affect saltwater species. This article describes a database for acute toxicity of PNP derived for calculating a national saltwater quality criterion. Using a ¯ow-through exposure system with measured concen- trations, we tested early life stages of four species of saltwater invertebrates and two species of ®sh. Static 96-h tests were also conducted on zoeal Homarus americanus, embryo-larval Mulinia lateralis, and larval Pleuronectes americanus. The number of organisms surviving the ¯ow-through test was measured at 2, 4, 8, and 12 h and daily through day 7. Mortality for most species plateaued by 96 h. The ranked sensitivities (96-h 50% lethal concentrations, measured in micrograms per liter) for the species tested were 17 for Pleuronectes americanus, 37.9 (48-h 50% effective concentration) for Mulinia lateralis, 59.4 for Paleomonetes vulgaris, 60.6 for Americamysis bahia (formerly Mysidopsis bahia), 61.6 for Leptocheirus plumulosos, 70 for Menidia beryllina, 71 for Homarus americanus, 142 for Cyprinodon variegatus, and .195 for Dyspanopius sayii. Values for the seven most sensitive of these species ranged over a factor of only 4.2. The narrow range of responses for PNP implies that exceeding a threshold concentration would endanger a large proportion of the aquatic community. KeywordsÐpara-Nonylphenol 4-Nonylphenol Acute toxicity Saltwater INTRODUCTION during sewage treatment [9]. Their persistence in sewage ef- para-Nonylphenol (4-nonylphenol, or PNP) is a mixture of ¯uent and industrial wastewater has been recognized for de- alkylphenols that is used in producing nonionic surfactants for cades [10]. Degradation of nonylphenol concentration varies detergents, emulsi®ers, lubricants, and oil additives. Most non- with conditions; biodegradation of free NP is only about 0.06% ylphenols (NPs) are used as intermediates in producing non- per day, especially in the absence of sediments [11]. ylphenol ethoxylates (NPEs) for oil-soluble detergents and for Because NPs are ubiquitous, resist degradation, and bioac- emulsi®ers that can be further re®ned to produce anionic de- cumulate, their ability to produce physiological effects has tergents, lubricants, textile scouring or antistatic agents, emul- been the subject of considerable recent attention [4,12]. For si®ers for agrichemicals, antioxidants in rubber and plastics, example, previous studies have shown that nonylphenol is di- and oil additives [1]. Because NPs are also breakdown products rectly toxic to ®sh and other aquatic animals [13,14]. The goal of alkylphenol polyethoxylates used in detergents, pesticides, of this study was to measure acute toxicity of PNP to organisms herbicides, and toiletries, they are found widely in surface representative of a saltwater community. The species, repre- waters and aquatic sediments [2]. Considerable research has senting early life stages of nine different taxonomic families, indicated that PNP is bioaccumulated [3], estrogenic [4], and were chosen according to the guidelines for deriving numerical highly toxic [5,6]. Consequently, the use of NP polyethoxy- national water quality criteria [15]. Documents for water qual- lates has been banned in several European countries. ity criteria (also called aquatic-life or chemical criteria) for From 1980 to 1988, production of nonylphenol in the Unit- individual substances have been developed to protect fresh- ed States increased by 37% [6]. A 1989 and 1990 study of water and saltwater aquatic life and their uses. The history of river reaches in the continental United States detected non- the development, derivation, and use of water quality criteria ylphenol in 30% of water samples and 71% of sediment sam- has been summarized by Hansen [16]. ples. Its concentrations in water ranged from 0.20 to 0.64 mg/ MATERIALS AND METHODS L and in sediments from 10 to 3,000 mg/kg [2]. Concentrations up to 1,600 mg/L of PNP have been found in water from Biological methods industrial sources [7]. Concentrations in river water down- We determined the acute toxicity of PNP to early life-stages stream from a discharge ranged from 2 to 3,000 mg/L [8]. of four species of saltwater invertebrates (Paleomonetes vul- Nonylphenol and its ethoxylates have also been found in treat- garis, Americamysis bahia, Leptocheirus plumulosos, and ment-plant wastewaters and sewage sludges, where they have Dyspanopeus sayii) and two species of ®sh (Menidia beryllina been produced by microbial breakdown of nonionic surfactants and Cyprinodon variegatus) by using a 7-d ¯ow-through ex- * To whom correspondence may be addressed posure with measured concentrations. The second of these spe- ([email protected]). cies, Americamysis bahia, was formerly known as Mysidopsis Contribution NHEERL-NAR-1992. Although this manuscript was bahia and has been redescribed [17]. All species were cultured reviewed in accordance with of®cial U.S. Environmental Protection on site except L. plumulosos, which was cultured at the SAIC Agency procedures, its content does not necessarily re¯ect U.S. EPA policy. Mentioning of commercial products or facilities does not nec- Environmental Testing Center, Narragansett, Rhode Island, essarily mean that U.S. EPA or the U.S. federal government endorses USA [18±20]. Nauplii of Artemia sp. were fed to cultured and them. test organisms. In accordance with ASTM recommendations 617 618 Environ. Toxicol. Chem. 19, 2000 S.M. Lussier et al. [21], only reference Artemia sp. were fed to organisms during testing. Organisms were exposed simultaneously in duplicate ¯ow- through exposure chambers. Each species was placed into sep- Mulinia lateralis arate containers with glass petri dish bottoms and walls of jars None Nitext screen (mesh size 320 mm, Aquatic Eco-Systems, 3, 8-oz. glass Apopka, FL, USA). Stock solutions were delivered to exposure chambers at each of seven concentrations by a ¯ow-through Ar- diluter exposure system [22]. The surviving organisms were sp. counted at hours 2, 4, 8, 12, and 24 and daily through day 7. Homarus temia To obtain data for lower-temperature species, static tests jars americanus were conducted with zoeal Homarus americanus (96 h, un- 10, 8-oz. glass measured concentrations), larval Pleuronectes americanus (96 h, measured concentrations), and embryo-larval Mulinia lat- eralis (48 h, unmeasured concentrations) [23]. The inhibition of fertilization, rather than survival, was the acute measure of toxicity in the M. lateralis test. Static tests were monitored ter glass dish- es americanus daily. All ¯ow-through and static tests used ®ltered (15 mm) Pleuronectes None Reference 2, 19-cm-diame- seawater at pH levels of 7.8 to 8.2 and salinity of 30 to 31 g/ kg from Narragansett Bay, Rhode Island, following ASTM procedures [24]. The salinity of the M. lateralis test was 32 Ar- g/kg. Exposure conditions for ¯ow-through and static tests are sp. summarized in Table 1. Data on survival were analyzed sta- vulgaris static unmeasured, no renewal. temia tistically using the Trimmed Spearman±Karber method of es- jars Palaemonetes 5 Reference timation with Abbott's correction formula and pooled controls 4, 8-oz. glass [25,26]. Analytical methods Ar- sp. We used 90% para-C9 phenols (CAS 84852-15-3) for all bahia temia tests. The carrier solvent was a solution of 20% acetone and jars Americamysis 80% triethylene glycol. Controls for seawater and for seawater 4, 8-oz. glass with solvent were used in all tests. Final mean concentrations in the ¯ow-through test were 20.2, 21, 29.5, 67.3, 70.5, 117, -nonylphenol multispecies test exposure and 195 mg/L. For the static-measured test with P. americanus, para ®nal mean concentrations were 3.7, 6.9, 16.3, 19.1, 32.3, 73.2, 125, and 163 mg/L. In the static-unmeasured test with H. amer- jars plumulosus Leptocheirus Isochrysis sp. Reference icanus, concentrations were 16, 26, 43, 72, 120, 200, and 330 4, 8-oz. glass static unmeasured, renewed daily; SUN mg/L; and in the M. lateralis test, they were 2.4, 8, 24, 80, 5 240, and 800 mg/L. Before adding organisms, we measured the concentration Ar- of test material in the ¯ow-through diluter and in one exposure sp. chamber per treatment to verify that they were the same. On Menidia beryllina temia netted cups day 4 of the test, we measured the duplicate of each treatment. Table 1. Test conditions for Reference In the static test with P. americanus, we also sampled at the 4, 9-cm-diameter beginning and end of the exposure. The sampling procedure consisted of siphoning 1-L samples Ar- from the ¯ow-through tests into separatory funnels prerinsed sp. with solvent. After internal standards were added, the samples temia netted cups were extracted three times with 50 ml of methylene chloride variegatus static measured, no renewal; SUR Cyprinodon Reference Juvenile Juvenile Adult Postlarvae 1-day Larvae 2-day Larvae 2-day Zoea ®rst stage Embryo 4, 9-cm-diameter and dried with anhydrous sodium sulfate. Each sample was 5 then reduced in volume, exchanged to heptane, and brought to a ®nal volume of 1 ml. The samples were stored in 1.8-ml vials until they were analyzed. Ar- The PNP in samples was measured by using a DB-5 cap- sp. illary fused-silica column in a Hewlett-Packard 5890 gas chro- sayi stage temia jars 2222222103 Dyspanopeus FTM4, 8-oz.
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