Efficiency of conventional drinking-water-treatment processes in removal of pharmaceuticals and other organic compounds
Introduction
More than 100,000 synthetic chemicals are used in a variety of domestic, industrial, and agricultural applications (Jørgensen, 2004). Numerous studies have documented that many of these compounds, including pharmaceuticals, fragrances and flavorants, flame retardants and plasticizers, detergent metabolites, components of personal care products, and products of petroleum use and combustion are incompletely degraded or removed during wastewater treatment and are persistent in the aquatic environment. Reviews of the occurrence and fate of organic compounds (OCs) in wastewaters and the aquatic environment are available (Metcalfe et al., 2004, Focazio et al., 2004, Daughton, 2001, Halling-Sørensen et al., 1998, Daughton and Ternes, 1999). Fewer studies have documented the occurrence of these OCs in drinking-water supplies. Exceptions include documentation of low-level concentrations of OCs in plant-scale studies of drinking-water supplies (Loraine and Pettigrove, 2006, Petrovic et al., 2003, Adams et al., 2002, Ternes et al., 2002, Reddersen et al., 2002, Heberer and Stan, 1997) and evaluation of their fate in laboratory-scale simulations of drinking-water-treatment (DWT) processes (Westerhoff et al., 2005, Huber et al., 2005, Pinkston and Sedlak, 2004, Zwiener and Frimmel, 2000).
In 2001, the potential for 106 OCs to survive a conventional DWT process and persist in finished, potable water was investigated (Stackelberg et al., 2004). The results provided the first documentation that a wide variety of OCs, most of which are currently unregulated in drinking-water supplies, can survive conventional DWT, but limitations in the study design precluded quantitative comparison of the degradation or removal of OCs by individual water treatments. Subsequent sampling at the same DWT plant in 2003 by the U.S. Geological Survey in cooperation with the New Jersey Department of Environmental Protection addressed these limitations by including (1) collection of multiple time-composited water samples at each treatment step to account for retention time through the DWT plant and diurnal variations in source-water quality, and (2) collection of solids samples for evaluation of the effectiveness of adsorptive processes in removing OCs. This paper uses data from the 2003 sampling to evaluate the average percent removal (concentration decreases) and fate of OCs that were detected in the DWT plant's source waters.
Section snippets
Description of DWT plant and sample collection
The DWT plant is in a heavily populated, highly urbanized drainage basin in which more than 50 STPs discharge effluent to the two streams (or their tributaries) that provide source water for the DWT plant. The DWT plant treats and provides an average of 235 million L/day to about 850,000 people. Supernatant water that is decanted from settled sludge and filter backwash sediments is recycled to the head of the plant (Fig. 1). This recycled water represents about 9% of water entering the
Analytical methods
The water samples were analyzed for 113 compounds, and the sediment samples were analyzed for 71 of these compounds, using methods developed by the USGS (Table 1A, Table 1B). Eighteen pharmaceuticals and selected degradates in water samples were measured by solid-phase extraction (SPE) and high-performance liquid chromatography/mass spectrometry positive-ion electrospray ionization [HPLC/MS–ESI(+)] (Table 1A, Table 1B) as described in Cahill et al. (2004), and 17 pharmaceuticals and selected
Quality assurance
Six field blanks and 86 laboratory blanks were analyzed for target compounds. Blank samples were derived from laboratory-grade organic-free water. Field blanks were used to indicate whether sampling procedures, sampling equipment, field conditions, or sample-shipment procedures introduced target compounds into environmental samples, and laboratory blanks were used to assess the potential for sample contamination in the laboratory. Field blanks were collected at each of the six water-sampling
Data analysis
Analysis of variance (ANOVA) on ranked concentrations was used to evaluate the null hypothesis that mean ranked concentrations were statistically similar among the six sampling points. If the null hypothesis was rejected, Tukey's multiple comparison test was used to indicate which mean ranked concentrations were similar to or significantly different from others (Helsel and Hirsch, 1992). Significance was set at the 95% confidence level for all statistical tests.
Average percent removal by each
Results
The effectiveness of a DWT plant in degrading or removing OCs depends on several factors (some of which may change through time), including the quality of the source water, the type and mode of operation of each treatment process, and physiochemical characteristics of the compounds themselves (Volk et al., 2005, Coupe and Blomquist, 2004). The flow of one of the two source streams ranged from about 6 to more than 81 m3/s during the sample collection period and the concentrations of some
Discussion
Results of this study indicate that the combined water treatments (clarification, disinfection, and GAC filtration) were effective at degrading or removing many OCs from source-water supplies to concentrations below analytical detection. Of the 32 compounds that were detected in at least 25% of the source-water samples (Fig. 2), 16 were not detected in samples of finished water (100% degradation or removal), and seven (carbamazepine, caffeine, acetaminophen, bisphenol A, triethyl citrate, TDIP,
Acknowledgements
This study was conducted cooperatively between the U.S. Geological Survey and the New Jersey Department of Environmental Protection. The authors thank the operators and staff of the drinking-water-treatment plant for allowing access to their facility and assisting our needs. We also thank Richard Coupe and Gregory Delzer of the U.S. Geological Survey and a anonymous reviewer for their helpful comments and suggestions.
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