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    Science of the Total Environment 329 (2004) 99113

    0048-9697/04/$ - see front matter 2004 Elsevier B.V. All rights reserved.doi:10.1016/j.scitotenv.2004.03.015

    Persistence of pharmaceutical compounds and other organicwastewater contaminants in a conventional drinking-water-

    treatment plant

    Paul E. Stackelberg *, Edward T. Furlong , Michael T. Meyer , Steven D. Zaugg ,a, b c b

    Alden K. Henderson , Dori B. Reissmand d

    US Geological Survey, 810 Bear Tavern Road, West Trenton, NJ 08628, USAa

    US Geological Survey, Box 25046, MS 407, Denver, CO 80225-0046, USAb

    US Geological Survey, 4500 SW 40th Avenue, Ocala, FL 34474, USAc

    Centers for Disease Control and Prevention, 1600 Clifton Road, MS E23, Atlanta, GA 30333, USAd

    Accepted 18 March 2004

    Abstract

    In a study conducted by the US Geological Survey and the Centers for Disease Control and Prevention, 24 water

    samples were collected at selected locations within a drinking-water-treatment (DWT) facility and from the twostreams that serve the facility to evaluate the potential for wastewater-related organic contaminants to survive aconventional treatment process and persist in potable-water supplies. Stream-water samples as well as samples of raw,settled, filtered, and finished water were collected during low-flow conditions, when the discharge of effluent fromupstream municipal sewage-treatment plants accounted for 3767% of flow in stream 1 and 1020% of flow instream 2. Each sample was analyzed for 106 organic wastewater-related contaminants (OWCs) that represent adiverse group of extensively used chemicals. Forty OWCs were detected in one or more samples of stream water orraw-water supplies in the treatment plant; 34 were detected in more than 10% of these samples. Several of thesecompounds also were frequently detected in samples of finished water; these compounds include selected prescriptionand non-prescription drugs and their metabolites, fragrance compounds, flame retardants and plasticizers, cosmeticcompounds, and a solvent. The detection of these compounds suggests that they resist removal through conventionalwater-treatment processes. Other compounds that also were frequently detected in samples of stream water and raw-water supplies were not detected in samples of finished water; these include selected prescription and non-prescriptiondrugs and their metabolites, disinfectants, detergent metabolites, and plant and animal steroids. The non-detection ofthese compounds indicates that their concentrations are reduced to levels less than analytical detection limits or thatthey are transformed to degradates through conventional DWT processes. Concentrations of OWCs detected infinished water generally were low and did not exceed Federal drinking-water standards or lifetime health advisories,although such standards or advisories have not been established for most of these compounds. Also, at least 11 andas many as 17 OWCs were detected in samples of finished water. Drinking-water criteria currently are based on thetoxicity of individual compounds and not combinations of compounds. Little is known about potential human-healtheffects associated with chronic exposure to trace levels of multiple OWCs through routes such as drinking water. Theoccurrence in drinking-water supplies of many of the OWCs analyzed for during this study is unregulated and most

    *Corresponding author. Tel.: q1-609-771-3951; fax: q1-609-771-3915. E-mail address: pestack@usgs.gov (P.E. Stackelberg).

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    100 P.E. Stackelberg et al. / Science of the Total Environment 329 (2004) 99113

    of these compounds have not been routinely monitored for in the Nations source- or potable-water supplies. Thisstudy provides the first documentation that many of these compounds can survive conventional water-treatmentprocesses and occur in potable-water supplies. It thereby provides information that can be used in setting research

    and regulatory priorities and in designing future monitoring programs. The results of this study also indicate thatimprovements in water-treatment processes may benefit from consideration of the response of OWCs and other traceorganic contaminants to specific physical and chemical treatments. 2004 Elsevier B.V. All rights reserved.

    Keywords: Pharmaceuticals; Wastewater contaminants; Water treatment

    1. Introduction

    During the 1990s, pharmaceutically active com-pounds such as lipid-regulating drugs, analgesics,

    antibiotics, antiseptics, hormones, and chemother-apy and beta-blocking heart drugs were detectedin wastewaters, streams, and ground-waterresources across Europe (Heberer and Stan, 1997;Buser et al., 1998a,b, 1999). Although pharmaceu-tically active compounds had been detected pre-viously in effluent from landfills (Turner et al.,1993; Holm et al., 1995) and sewage-treatmentplants (STPs) (Hignite and Azarnoff, 1977), thesemore recent investigations indicated that somepharmaceutically active compounds are nearly

    ubiquitous at low concentrations in water bodiesthat receive STP effluent. Reviews of the occur-rence, fate, and effects of pharmaceutically activecompounds in the environment are available (Rich-ardson et al., 1985; Halling-Sorensen et al., 1998;Daughton, 2001; Ternes, 2001).

    During 19992000, Kolpin et al. (2002) con-ducted a reconnaissance of pharmaceuticals andother wastewater-related contaminants in suscepti-ble streams across the United States, expandingthe scope of previous investigations and providing

    the first nationwide data set of this type. Resultsof this reconnaissance survey document that awide variety of organic compounds are frequentlydetected in streams that receive agricultural,domestic, and (or) industrial wastewater effluent.These contaminants include antibiotics, other pre-scription drugs, non-prescription drugs, animal andplant steroids, reproductive hormones, personal-care products, detergent metabolites, flame retar-dants, products of oil use and combustion, andother extensively used chemicals, collectively

    referred to as organic wastewater contaminants(OWCs).

    Measures to conserve and reuse water common-ly are initiated in areas with growing urban popu-lations and constraints on the development of newwater sources. These measures include the use oftreated municipal wastewater to augment raw-water suppliesa process referred to as indirectpotable water reuse (IPWR) (National ResearchCouncil, 1998). The presence of OWCs in waste-water effluent is one of the most challengingaspects of IPWR because of the large number ofcompounds that may be present, the inability todetermine all of these compounds, and the lack oftoxicity information and drinking-water standardsfor many of them (National Research Council,

    1998). The frequent occurrence of these com-pounds in streams (Kolpin et al., 2002), some ofwhich are used as sources of drinking water, givesrise to concern over the potential for these com-pounds to occur in drinking water and, thus, toaffect human health through chronic exposure.

    To date, few studies have been published con-cerning the occurrence of OWCs in drinking-watersupplies (Kummerer, 2001). Notable exceptions

    include the detection of the pharmaceuticals phen-azone and propiphenazone and the drug metabo-

    lites clofibric acid and 1-acetyl-1-methyl-2-dimethyl-oxamoyl-2-phenylhydrazide in samplesof potable water collected in the vicinity of Berlin,Germany (Heberer and Stan, 1997; Reddersen etal., 2002), and the detection of three widely usednon-prescription drugscaffeine, cotinine, andacetaminophenin samples of potable water col-lected near Atlanta, Georgia (Frick et al., 2001).

    The objective of this study, conducted by theUS Geological Survey (USGS) and the Centersfor Disease Control and Prevention, was to build

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    101P.E. Stackelberg et al. / Science of the Total Environment 329 (2004) 99113

    on the above-mentioned investigations by exam-ining a wider variety of OWCs in order to furtherassess the potential for these compounds to survive

    conventional water treatment and occur in fin-ished-water supplies. The occurrence of many ofthese compounds in drinking water is unregulatedand most of them have not been routinely moni-tored for in the Nations source- and potable-watersupplies. By documenting the occurrence of abroad suite of OWCs in source- and potable-watersupplies, results of this study can be used in settingmonitoring, research, and regulatory priorities, andin designing appropriate chemical and toxicologi-cal studies and risk assessments to address more

    fully the potential health effects associated withIPWR.

    This paper documents the occurrence of selectOWCs in 24 samples of stream, raw, settled,filtered, and finished water associated with a drink-ing-water-treatment (DWT) facility. Althoughthese OWCs represent a diverse group of chemi-cals with a wide variety of uses, they account foronly a fraction of the thousands of organic com-pounds that currently are manufactured and usedfor therapeutic purposes or that occur in various

    consumer and household, industrial and commer-cial, or agricultural products. This study, therefore,does not provide information on all of the OWCsthat may occur in source- or potable-water sup-plies; rather, it documents the occurrence of select-ed organic contaminants representing a widevariety of uses and origins in environmental watersand in potable-water supplies.

    2. Description of site and sampling methods

    The DWT facility from which samples werecollected during this study is in a heavily populat-ed, highly urbanized drainage basin. More than 50STPs discharge effluent to the two streams fromwhich the DWT facility withdraws its raw-watersuppl