Skip to main content

Pharmaceuticals in the Surface Water of the USA: A Review

Abstract

This review investigates the occurrence of pharmaceuticals in the surface waters (including rivers, lakes, oceans, and aquifers) of the USA, discusses various pathways of pharmaceutical contamination from different point sources, assesses the potential risk of pharmaceutical contamination for aquatic organisms, and provides a discussion on the opportunities for a sustainable management of pharmaceutical contamination. We found a total of 93 pharmaceuticals that have been reported to contaminate the surface water, including: 27 antibiotics; 15 antidepressants; 9 antihypertensives; 7 analgesics; 7 anticonvulsants; 6 antilipidemics; 3 contraceptives; 3 stimulants; and 2 each of antihistamines, blood thinners, disinfectants, antacids, antitussives, anti-anxiety, anti-inflammatory, and diuretic agents. The pharmaceuticals that are assessed to be at high risk (risk quotient RQ ≥1.0) include acetaminophen (analgesic), caffeine (stimulant), sulfadimethoxine (antibiotic), as well as triclocarban and triclosan (both used in disinfectants). Such drugs require detailed evaluation as to the frequency of their occurrence and the risks for aquatic organisms and humans. Opportunities for sustainable control of pharmaceutical contamination include source control (proper disposal of leftover pharmaceuticals; careful monitoring of hospital wastes), and improvements to treatment facilities for the efficient removal and safe transformation of pharmaceutical contaminants.

Introduction

A significant volume of pharmaceuticals are used by humans for the treatment of diseases, injuries, or illnesses, in addition to their use as personal care products [1]. At the consumer level, we are mostly concerned about the use of pharmaceuticals and personal care products (PPCPs) in making our lives healthier, and are less concerned about the fate of PPCPs after consumption. However, the occurrence of PPCPs in our water environment [25, 6•, 7] opens up new discussions on the fate of PPCPs post-consumption, and the repercussions of their presence in water.

A number of studies have investigated the impact of pharmaceutical contamination of the water environment on aquatic organisms [813]. For example, Gelsleichter and Szabo [8] in a recent study found that synthetic estrogens used as human contraceptives (17α-ethynylestradiol), as well as six of the selective serotonin/norepinephrine reuptake inhibitors (citalopram, fluoxetine, fluvoxamine, paroxetine, sertraline, venlafaxine) used as human antidepressants, were observed at detectable levels in the plasma of neonate bull sharks (Carcharhinus leucas) residing in the wastewater-impacted Caloosahatchee River in Florida. In another study, Fair et al. [10] reported detectable levels of anthropogenic triclosan (a chemical commonly found in household disinfectants) in blood plasma of wild bottlenose dolphins (Tursiops truncatus).

Such unwanted exposure and accumulation may pose potential health risks for aquatic organisms, as has been documented in a number of reports [1425]. Fent et al. [16] reviewed the ecotoxicity of human pharmaceuticals and suggested that, while acute effects on aquatic organisms are most unlikely (except for large volume spills), very little is however known about the long-term effects of these pharmaceuticals on aquatic organisms. Oliveira et al. [25] investigated the effects of oxytetracycline and amoxicillin on the development and biomarker activities of zebrafish, and indicated that short-term effects on physiological impairment in the zebrafish population is unlikely to occur, but suggested that chronic long-term exposures from low doses must also be investigated. In another study, Nietch et al. [17] suggested that the effects of chronic lower range exposure of triclosan may play an important role towards a shift in the stream mesocosm community, including bacteria and macro-invertebrates.

Since chronic (long-term) pharmaceutical toxicity data is limited, a common method of assessing environmental risk is by calculating a risk quotient (RQ). This is a ratio of the measured or predicted pharmaceutical environmental concentration (PEC), and the predicted no-effect concentration (PNEC), the environmental concentration at which no adverse effect on aquatic ecosystem function is to be expected [23, 24, 2628]. The PNEC values are estimated on the basis of available acute or chronic toxicity data for several aquatic organisms: bacteria, algae, invertebrates, and fish; where the toxicity data is adjusted with an appropriate assessment factor [23, 29•]. The calculated RQ value is then used to prioritize pharmaceuticals that are likely to pose a high risk (RQ ≥ 1.0); medium risk (1.0 > RQ ≥ 0.1); or low risk (RQ < 0.1); to the aquatic ecosystem [21, 29•, 30].

The unwanted exposure to pharmaceuticals may also pose health risks for humans, either indirectly through bioaccumulation in the food chain, or directly through consumption of drinking water tainted with pharmaceutical contaminants (measured or estimated) [15, 20, 3133]. For example, Leung et al. [33] investigated the occurrence of pharmaceuticals in tap water and assessed the health risks to humans at different life stages. They concluded that the risk to humans from exposure to pharmaceutical contaminants is low based on current toxicity data, although a long-term monitoring framework is proposed [33]. Similarly, other studies have concluded that, based on current knowledge, the presence of trace levels of pharmaceuticals poses negligible or only minor risks to humans [15, 20, 31, 32].

Given the significance of pharmaceutical contamination in the water environment, this review examines the maximum levels of pharmaceuticals reported in the surface waters (exclusively of the USA), discusses various pathways of pharmaceutical contamination from different point sources, assesses the potential risk of pharmaceuticals contamination for aquatic organisms, and identifies opportunities for sustainable management of pharmaceutical contamination. In this review, ‘pharmaceuticals’ are defined as prescription and non-prescription drugs that are either ingested, inhaled, or topically applied for prevention and/or cure of diseases, illnesses, and injuries. Thus, two of the antimicrobial compounds (triclosan and triclocarban) commonly used in household disinfectants are included; however, all of the naturally occurring hormones, as well as synthetic flavors and fragrances, cosmetics, and personal care products were excluded. Where maximum or highest levels of pharmaceuticals were not available, average or mean values were used as maximum levels. The literature search was conducted using the Web of Science database, using the keyword “pharmaceutical(s)” in natural or surface water, which includes rivers, lakes, oceans, and aquifers. The database was searched for all the years up to January 2014, but only those references that reported maximum concentrations of the same pharmaceutical were included.

Fate of Pharmaceuticals Post-consumption

Figure 1 shows a schematic of the various pathways by which pharmaceuticals can enter the surface water, which includes rivers, lakes, oceans, and aquifers. The major point sources of pharmaceuticals are: (1) industry (mainly from manufacture of pharmaceuticals) [34]; (2) household [35, 36]; and (3) hospitals [37]. The contribution from household and hospitals is mainly the result of the excretion of un-metabolized or metabolized consumed (ingested, injected, inhaled) pharmaceuticals; the washing away of topically applied personal care products [36, 38]; and the disposal (flushed down the toilet or solid waste) of expired and unwanted (leftover) pharmaceuticals [39, 40]. A significant volume of pharmaceutical waste also ends up as solid waste, including waste from Concentrated Animal Feeding Operations (CAFO).

Fig. 1
figure 1

Schematic showing various pathways by which pharmaceuticals enter surface water, and distribution of the types of pharmaceuticals found in surface water of the USA. WW (wastewater); DW (drinking water); CAFO (Concentrated Animal Feeding Operation); WWTP (wastewater treatment plant); DWTP (drinking water treatment plant)

Pharmaceutical wastewater from the aforementioned point sources, including other liquid waste from industry, hospitals, and household (washing, bathing, showering, and kitchen use), form a complex mixture of raw wastewater (Raw WW), which is treated in wastewater treatment plants (WWTP). Although the primary goal of a WWTP is to treat wastewater through a combination of physical, biological and chemical treatment [35]; the ability to treat pharmaceuticals and personal care products (PPCPs) is widely evaluated [41], particularly the persistence of pharmaceuticals post-WWTP, in the treated wastewater (Treated WW) [20], and Biosolids [42]. The latter is an unwanted byproduct of WWTP that results from municipal wastewater residuals or sewage sludge after additional treatment processes, including aerobic and/or anaerobic digestion, lime stabilization, and dewatering [43].

Persistent pharmaceuticals in Treated WW is either discharged into surface waters (especially in coastal settings) or reclaimed for land irrigation and farming [44], which may also enter surface water via direct leaching or surface runoffs [2, 45]. Biosolids, on the other hand, are applied on land as fertilizer or soil conditioner. However, persistent pharmaceuticals in biosolids, including pharmaceuticals from solid waste, may also enter surface water through leaching or surface runoffs [46]. Additional pathways by which pharmaceutical contaminants can enter surface water are from sewer overflow or the leakage of sewer distribution lines [4749].

Pharmaceutical contaminants may also enter groundwater via infiltration from surface water, or leachate of solid waste, or pharmaceutical-tainted irrigation water. The occurrence of pharmaceuticals in groundwater is problematic, especially since groundwater may be used for drinking water, especially in rural settings where remote treatment facilities are limited [50], thus posing potential health risks for humans. In contrast, human exposure to pharmaceutical contaminants in surface water is mostly indirect, including accidental ingestion, topical exposure, and biomagnification through the food chain. Surface water drawn in for raw drinking water (Raw DW) is subject to extreme treatment before distribution as drinking water. However, pharmaceutical contaminants in surface water may pose potential health risks for aquatic organisms [46].

Occurrence and Risk Assessment of Pharmaceuticals in Surface Water

Figure 1 (inset) also shows the number of pharmaceuticals (per pharmaceutical type) reported to occur in the surface water of the USA. A total of 93 pharmaceuticals have been reported to be present and contaminate the surface water, including: 27 antibiotics; 15 antidepressants; 9 antihypertensives; 7 analgesics; 7 anticonvulsants; 6 antilipidemics; 3 contraceptives; 3 stimulants; and 2 each of antihistamines, blood thinners, disinfectants, antacids, antitussives, anti-anxiety, anti-inflammatory, and diuretic agents. Table 1 groups the pharmaceuticals included in this study by type and identity (CAS #), with a brief description on the uses of the different types, and also indicates metabolites of the original pharmaceuticals used. Only one veterinary medicine, tylosin (CAS# 1401-69-0) categorized under antibiotics, was included in this study. Additionally, the occurrence of cotinine (CAS# 486-56-6), which is a metabolite of nicotine, is most likely linked to exposure from cigarette smoke. A recent study by Levine et al. showed elevated levels of cotinine in urine samples of smokers compared to nonsmokers (through passive smoking) [51]. The suggested pathway for cotinine contamination is from urine samples to Raw WW to Treated WW to surface water.

Table 1 List of pharmaceuticals, categorized as per their usage, included in this study

It is important to note here that the total number of 93 pharmaceuticals is only a fraction of the total number of pharmaceuticals used by humans and by animal farms. Thus, more pharmaceuticals are expected to occur in the surface water, given the physical-chemical properties of pharmaceuticals favoring persistence, and the inefficiency of the WWTPs. Furthermore, data on more pharmaceuticals occurring in surface waters of the USA could perhaps be found with different search keywords, such as naturally occurring hormones, synthetic flavors and fragrances, cosmetics, personal care products, and the aforementioned specific types of pharmaceuticals (e.g., antibiotics).

In order to assess the risks posed by the pharmaceuticals detected in surface water to living organisms, we calculated the risk quotient (RQ) values, a ratio of the highest concentrations of pharmaceuticals detected in surface water and predicted no-effect concentration (PNEC) values. The PNEC values were estimated by dividing the pharmaceutical’s chronic toxicity values towards fish (obtained from PBT Profiler [52]) with an assessment factor of 100 [27], which is required to extend the chronic toxicity values for fish to other aquatic organisms [30, 53, 54]. Table 2 shows highest concentrations of pharmaceuticals detected in surface water, their estimated PNEC, and calculated RQ values. We sub-categorized the RQ values into low risk (RQ < 0.1); medium risk (0.1 ≤ RQ < 1); and high risk (RQ ≥ 1.0) [21, 29•, 30, 55]. The levels of pharmaceuticals at medium risk are: azithromycin; carbamazepine; cimetidine; citalopram; codeine; cotinine; diltiazem; diphenhydramine; 17-α-ethinylestradiol; fluoxetine; mestranol; paraxanthine; sertraline; sulfamethoxazole; thiabendazole; and venlafaxine. The occurrence of these pharmaceuticals in surface water needs further monitoring. Acetaminophen (analgesic), caffeine (stimulant), sulfadimethoxine (antibiotic), triclocarban (used in disinfectants), and triclosan (used in disinfectants) levels in surface water are at high risk, which suggests detailed evaluation of their potential risk for aquatic organisms [21].

Table 2 Maximum concentrations of pharmaceuticals detected in surface water (SW), their predicted no-effect concentration (PNEC), and their calculated risk quotient (RQ)

Opportunities for Sustainable Management of Pharmaceuticals

A total of 93 pharmaceuticals have been reported to occur in the surface water of the USA. It is important to evaluate the potential health risks of prioritized pharmaceuticals for humans and aquatic organisms, to design strategies for their removal from surface water, evaluate the pathways by which these pharmaceuticals enter surface water, and highlight their point sources. Such a comprehensive undertaking will give us an opportunity to explore sustainable strategies for managing and controlling pharmaceutical contamination in the environment.

The aforementioned text on “Fate of pharmaceuticals post-consumption” discusses the pathways by which pharmaceuticals enter the surface water. The first opportunity for minimizing pharmaceutical contamination is at the consumer level [39, 40, 56•, 57, 58], especially with respect to disposal of unwanted or leftover pharmaceuticals through the sink, toilet, or garbage. Wieczorkiewics et al. recently investigated the use, storage, and disposal of prescription and nonprescription medications by the residents of Cook County, Illinois. The study revealed that 59 % of respondents reported disposing of medications in the household garbage, and 31 % flushed them down the toilet or sink. More interestingly, over 80 % of respondents stated that they had never received information about proper medication disposal [56•]. It is evident from this study that public education on proper disposal of pharmaceuticals is lacking or not “prescribed” at the drug stores. Viable solutions for minimizing pharmaceutical contamination at consumer level include: (1) state or federal-funded collection bins at the local grocery or drug stores for collecting leftover (unwanted, unused or expired) pharmaceuticals; (2) public education on proper disposal of leftover drugs through schools, flyers, and television advertisements.

Another opportunity for controlling pharmaceuticals at the source would be to address waste from pharmaceutical industries [34] and hospitals [26, 29•, 37, 59, 60]. In a recent study Verlicchi et al. found consistent differences in the levels of some antibiotics, analgesics and lipid regulators in the effluent directly from the hospital with that mixed with the local urban effluent, thereby suggesting that hospital effluents represent one of the main sources of pollutants, in particular antibiotics, receptor antagonists and lipid regulators [29•]. Thus, wastewater from the pharmaceutical industry and hospitals should be more carefully monitored for elevated levels of pharmaceuticals and perhaps have their own treatment units; further, the pharmaceutical industries could invest in manufacturing greener pharmaceuticals [61] that are more conducive to degradation post-consumption and safe for the environment [46].

Furthermore, wastewater treatment facilities should be more carefully evaluated for the efficiency of their treatment of pharmaceutical contaminants [38, 6265]. Progress has been made towards the more efficient removal and transformation of pharmaceuticals using advanced treatments, employing processes of physical [66, 67], chemical [62, 6871], and biological nature [7275]. In addition to evaluating the treatment efficiency, it is also important to investigate whether pharmaceuticals are transformed into safer metabolites [46].

Conclusions

Given the significance of pharmaceutical contamination in the water environment, this review assessed the occurrence and risk of pharmaceuticals in the surface waters of the USA. A total of 93 pharmaceuticals have been reported to occur in the surface water, the most common being of the type antibiotic (total of 27) and antidepressant (total of 15). The pharmaceuticals that are assessed to be at high risk (RQ ≥ 1.0) include acetaminophen (analgesic); caffeine (stimulant); sulfadimethoxine (antibiotic); triclocarban (used in disinfectants); and triclosan (used in disinfectants). Given the high ecological risk, these pharmaceuticals require detailed evaluation, which means that their levels in surface water must be continuously monitored, and the risks for aquatic organisms must be carefully evaluated (both for chronic and acute toxicity), and any opportunities for their removal from the surface water and sustainable management opportunities must be explored. The following recommendations can be used as a guide for sustainable management of pharmaceutical contaminants:

  1. (1)

    State or federal-funded collection bins at the local grocery or drug stores for collecting leftover (unwanted, unused or expired) pharmaceuticals;

  2. (2)

    Public education on proper disposal of leftover drugs through schools, flyers, or television advertisements;

  3. (3)

    Stringent monitoring of pharmaceutical contaminants in the wastewater from pharmaceutical industry and hospitals;

  4. (4)

    Investment in manufacture of greener pharmaceuticals more conducive to degradation post-consumption;

  5. (5)

    Careful evaluation of WWTPs for efficiency of pharmaceutical contaminant removal;

  6. (6)

    Regulation of the use of biosolids as fertilizer or soil conditioner;

  7. (7)

    Regulation of the use of Treated WW for recreational use;

  8. (8)

    Conduct research on chronic (long-terms) effects of pharmaceuticals (and their metabolites) on aquatic organisms.

References

Papers of particular interest, published recently, have been highlighted as: • Of importance

  1. Ruhoy IS, Daughton CG. Beyond the medicine cabinet: an analysis of where and why medications accumulate. Environ Int. 2008;34:1157–69.

    PubMed  Article  CAS  Google Scholar 

  2. Karnjanapiboonwong A, Suski JG, Shah AA, Cai QS, Morse AN, Anderson TA. Occurrence of PPCPs at a wastewater treatment plant and in soil and groundwater at a land application site. Water Air Soil Pollut. 2011;216:257–73.

    Article  CAS  Google Scholar 

  3. Snyder S. Occurrence of pharmaceuticals in U.S. drinking water. In: Halden R, editor. Contaminants of emerging concern in the environment: ecological and human health considerations. Washington, D.C.: American Chemical Society; 2010. p. 69–80.

    Chapter  Google Scholar 

  4. Sengupta A, Lyons JM, Smith DJ, Drewes JE, Snyder SA, Heil A, et al. The occurrence and fate of chemicals of emerging concern in coastal urban rivers receiving discharge of treated municipal wastewater effluent. Environ Toxicol Chem. 2014;33:350–8.

    PubMed  Article  CAS  Google Scholar 

  5. Daughton C. Pharmaceutical ingredients in drinking water: overview of occurrence and significance of human health considerations. In: Rolf UH, editor. Contaminants of emerging concern in the environment: ecological and human health considerations. Washington, D.C.: American Chemical Society; 2010. p. 9–68.

    Chapter  Google Scholar 

  6. Kaplan S. Review: pharmacological pollution in water. Crit Rev Environ Sci Technol. 2013;43:1074–116. This study highlights research developments on pharmacological pollution in water, including pollution characterization, analytical methods, removal via wastewater treatment plants, and potential environmental impacts.

    Article  CAS  Google Scholar 

  7. Boxall ABA, Rudd MA, Brooks BW, Caldwell DJ, Choi K, Hickmann S, et al. Pharmaceuticals and personal care products in the environment: what are the big questions? Environ Health Perspect. 2012;120:1221–9.

    PubMed Central  PubMed  Article  Google Scholar 

  8. Gelsleichter J, Szabo NJ. Uptake of human pharmaceuticals in bull sharks (Carcharhinus leucas) inhabiting a wastewater-impacted river. Sci Total Environ. 2013;456:196–201.

    PubMed  Article  CAS  Google Scholar 

  9. Brodin T, Fick J, Jonsson M, Klaminder J. Dilute concentrations of a psychiatric drug alter behavior of fish from natural populations. Science. 2013;339:814–5.

    PubMed  Article  CAS  Google Scholar 

  10. Fair PA, Lee HB, Adams J, Darling C, Pacepavicius G, Alaee M, et al. Occurrence of triclosan in plasma of wild Atlantic bottlenose dolphins (Tursiops truncatus) and in their environment. Environ Pollut. 2009;157:2248–54.

    PubMed  Article  CAS  Google Scholar 

  11. Owen SF, Huggett DB, Hutchinson TH, Hetheridge MJ, Kinter LB, Ericson JF, et al. Uptake of propranolol, a cardiovascular pharmaceutical, from water into fish plasma and its effects on growth and organ biometry. Aquat Toxicol. 2009;93:217–24.

    PubMed  Article  CAS  Google Scholar 

  12. Christenson T. Fish on morphine: protecting Wisconsin's natural resources through a comprehensive plan for proper disposal of pharmaceuticals. Wis Law Rev. 2008;1:141–79.

    Google Scholar 

  13. Brozinski J-M, Lahti M, Meierjohann A, Oikari A, Kronberg L. The anti-inflammatory drugs diclofenac, naproxen and ibuprofen are found in the bile of wild fish caught downstream of a wastewater treatment plant. Environ Sci Technol. 2013;47:342–8.

    PubMed  Article  CAS  Google Scholar 

  14. Cunningham VL, Constable DJC, Hannah RE. Environmental risk assessment of paroxetine. Environ Sci Technol. 2004;38:3351–9.

    PubMed  Article  CAS  Google Scholar 

  15. Cunningham VL, Binks SP, Olson MJ. Human health risk assessment from the presence of human pharmaceuticals in the aquatic environment. Regul Toxicol Pharmacol. 2009;53:39–45.

    PubMed  Article  CAS  Google Scholar 

  16. Fent K, Weston AA, Caminada D. Ecotoxicology of human pharmaceuticals. Aquat Toxicol. 2006;76:122–59.

    PubMed  Article  CAS  Google Scholar 

  17. Nietch CT, Quinlan EL, Lazorchak JM, Impellitteri CA, Raikow D, Walters D. Effects of a chronic lower range of triclosan exposure on a stream mesocosm community. Environ Toxicol Chem. 2013;32:2874–87.

    PubMed  Article  CAS  Google Scholar 

  18. Cleuvers M. Mixture toxicity of the anti-inflammatory drugs diclofenac, ibuprofen, naproxen, and acetylsalicylic acid. Ecotoxicol Environ Saf. 2004;59:309–15.

    PubMed  Article  CAS  Google Scholar 

  19. Cleuvers M. Aquatic ecotoxicity of pharmaceuticals including the assessment of combination effects. Toxicol Lett. 2003;142:185–94.

    PubMed  Article  CAS  Google Scholar 

  20. Kostich MS, Batt AL, Lazorchak JM. Concentrations of prioritized pharmaceuticals in effluents from 50 large wastewater treatment plants in the USA and implications for risk estimation. Environ Pollut. 2014;184:354–9.

    PubMed  Article  CAS  Google Scholar 

  21. Komori K, Suzuki Y, Minamiyama M, Harada A. Occurrence of selected pharmaceuticals in river water in Japan and assessment of their environmental risk. Environ Monit Assess. 2013;185:4529–36.

    PubMed  Article  CAS  Google Scholar 

  22. Ortiz de Garcia S, Pinto Pinto G, Garcia-Encina PA, Irusta Mata R. Ranking of concern, based on environmental indexes, for pharmaceutical and personal care products: an application to the Spanish case. J Environ Manag. 2013;129:384–97.

    Article  Google Scholar 

  23. Ferrari B, Mons R, Vollat B, Fraysse B, Paxeus N, Lo Giudice R, et al. Environmental risk assessment of six human pharmaceuticals: are the current environmental risk assessment procedures sufficient for the protection of the aquatic environment? Environ Toxicol Chem. 2004;23:1344–54.

    PubMed  Article  CAS  Google Scholar 

  24. Carlsson C, Johansson AK, Alvan G, Bergman K, Kuhler T. Are pharmaceuticals potent environmental pollutants? Part I: environmental risk assessments of selected active pharmaceutical ingredients. Sci Total Environ. 2006;364:67–87.

    PubMed  Article  CAS  Google Scholar 

  25. Oliveira R, McDonough S, Ladewig JCL, Soares AMVM, Nogueira AJA, Domingues I. Effects of oxytetracycline and amoxicillin on development and biomarkers activities of zebrafish (Danio rerio). Environ Toxicol Pharmacol. 2013;36:903–12.

    PubMed  Article  CAS  Google Scholar 

  26. Orias F, Perrodin Y. Characterisation of the ecotoxicity of hospital effluents: a review. Sci Total Environ. 2013;454:250–76.

    PubMed  Article  CAS  Google Scholar 

  27. Carlsson C, Johansson AK, Alvan G, Bergman K, Kuhler T. Are pharmaceuticals potent environmental pollutants? Part II: environmental risk assessments of selected pharmaceutical excipients. Sci Total Environ. 2006;364:88–95.

    PubMed  Article  CAS  Google Scholar 

  28. Carlsson G, Orn S, Larsson DGJ. Effluent from bulk drug production is toxic to aquatic vertebrates. Environ Toxicol Chem. 2009;28:2656–62.

    PubMed  Article  CAS  Google Scholar 

  29. Verlicchi P, Al Aukidy M, Galletti A, Petrovic M, Barcelo D. Hospital effluent: investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Sci Total Environ. 2012;430:109–18. This study compared the chemical and ecotoxicological characteristics of hospital wastewater, for 73 pharmaceuticals compounds from 12 different therapeutic classes, with those in other influent wastewater entering wastewater treatment plant. The study found that pharmaceutical compounds found in hospital wastewater were consistently higher than those found in other influent wastewater, suggesting that hospital wastewater requires more specific treatment options.

    PubMed  Article  CAS  Google Scholar 

  30. Hernando MD, Mezcua M, Fernandez-Alba AR, Barcelo D. Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments. Talanta. 2006;69:334–42.

    PubMed  Article  CAS  Google Scholar 

  31. Kumar A, Xagoraraki I. Human health risk assessment of pharmaceuticals in water: An uncertainty analysis for meprobamate, carbamazepine, and phenytoin. Regul Toxicol Pharmacol. 2010;57:146–56.

    PubMed  Article  CAS  Google Scholar 

  32. Kumar A, Chang B, Xagoraraki I. Human health risk assessment of pharmaceuticals in water: issues and challenges ahead. Int J Environ Res Pub Health. 2010;7:3929–53.

    Article  CAS  Google Scholar 

  33. Leung HW, Jin L, Wei S, Tsui MMP, Zhou B, Jiao L, et al. Pharmaceuticals in tap water: human health risk assessment and proposed monitoring framework in China. Environ Health Perspect. 2013;121:839–46.

    PubMed Central  PubMed  Article  Google Scholar 

  34. Phillips PJ, Smith SG, Kolpin DW, Zaugg SD, Buxton HT, Furlong ET, et al. Pharmaceutical formulation facilities as sources of opioids and other pharmaceuticals to wastewater treatment plant effluents. Environ Sci Technol. 2010;44:4910–6.

    PubMed Central  PubMed  Article  CAS  Google Scholar 

  35. Daughton CG, Ternes TA. Pharmaceuticals and personal care products in the environment: agents of subtle change? Environ Health Perspect. 1999;107:907–38.

    PubMed Central  PubMed  Article  CAS  Google Scholar 

  36. Daughton CG, Ruhoy IS. Environmental footprint of pharmaceuticals: the significance of factors beyond direct excretion to sewers. Environ Toxicol Chem. 2009;28:2495–521.

    PubMed  Article  CAS  Google Scholar 

  37. Nagarnaik PM, Batt AL, Boulanger B. Healthcare facility effluents as point sources of select pharmaceuticals to municipal wastewater. Water Environ Res. 2012;84:339–45.

    PubMed  CAS  Google Scholar 

  38. Ternes TA, Joss A, Siegrist H. Scrutinizing pharmaceuticals and personal care products in wastewater treatment. Environ Sci Technol. 2004;38:392A–9A.

    PubMed  Article  CAS  Google Scholar 

  39. Ruhoy IS, Daughton CG. Types and quantities of leftover drugs entering the environment via disposal to sewage - revealed by coroner records. Sci Total Environ. 2007;388:137–48.

    PubMed  Article  CAS  Google Scholar 

  40. Glassmeyer ST, Hinchey EK, Boehme SE, Daughton CG, Ruhoy IS, Conerly O, et al. Disposal practices for unwanted residential medications in the USA. Environ Int. 2009;35:566–72.

    PubMed  Article  CAS  Google Scholar 

  41. Heidler J, Halden RU. Meta-analysis of mass balances examining chemical fate during wastewater treatment. Environ Sci Technol. 2008;42:6324–32.

    PubMed Central  PubMed  Article  CAS  Google Scholar 

  42. Venkatesan AK, Halden RU. Wastewater treatment plants as chemical observatories to forecast ecological and human health risks of manmade chemicals. Sci Rep. 2014, 4.

  43. McClellan K, Halden RU. Pharmaceuticals personal care products in archived US biosolids from the 2001 EPA national sewage sludge survey. Water Res. 2010;44:658–68.

    PubMed Central  PubMed  Article  CAS  Google Scholar 

  44. Chen W, Xu J, Lu S, Jiao W, Wu L, Chang AC. Fates and transport of PPCPs in soil receiving reclaimed water irrigation. Chemosphere. 2013;93:2621–30.

    PubMed  Article  CAS  Google Scholar 

  45. Katz BG, Griffin DW, Davis JH. Groundwater quality impacts from the land application of treated municipal wastewater in a large karstic spring basin: Chemical and microbiological indicators. Sci Total Environ. 2009;407:2872–86.

    PubMed  Article  CAS  Google Scholar 

  46. Deo RP, Halden RU. Pharmaceuticals in the built and natural water environment of the USA. Water. 2013;5:1346–65.

    Article  CAS  Google Scholar 

  47. Phillips P, Chalmers A. Wastewater effluent, combined sewer overflows, and other sources of organic compounds to Lake Champlain. J Am Water Resour Assoc. 2009;45:45–57.

    Article  CAS  Google Scholar 

  48. Shala L, Foster GD. Surface water concentrations and loading budgets of pharmaceuticals and other domestic-use chemicals in an urban watershed (Washington, DC, USA). Arch Environ Contam Toxicol. 2010;58:551–61.

    PubMed  Article  CAS  Google Scholar 

  49. Halden RU, Paull DH. Co-occurrence of triclocarban and triclosan in US water resources. Environ Sci Technol. 2005;39:1420–6.

    PubMed  Article  CAS  Google Scholar 

  50. Fram MS, Belitz K. Occurrence and concentrations of pharmaceutical compounds in groundwater used for public drinking-water supply in California. Sci Total Environ. 2011;409:3409–17.

    PubMed  Article  CAS  Google Scholar 

  51. Levine H, Berman T, Goldsmith R, Goeen T, Spungen J, Novack L, et al. Exposure to tobacco smoke based on urinary cotinine levels among Israeli smoking and nonsmoking adults: a cross-sectional analysis of the first Israeli human biomonitoring study. BMC Public Health. 2013;13:1241.

    PubMed Central  PubMed  Article  Google Scholar 

  52. USEPA PBT Profiler software. Available at http://www.pbtprofiler.net 2013.

  53. Hernando MD, Gomez MJ, Aguera A, Fernandez-Alba AR. LC-MS analysis of basic pharmaceuticals (beta-blockers and anti-ulcer agents) in wastewater and surface water. Trac-Trends Anal Chem. 2007;26:581–94.

    Article  CAS  Google Scholar 

  54. Yu Y, Wu L, Chang AC. Seasonal variation of endocrine disrupting compounds, pharmaceuticals and personal care products in wastewater treatment plants. Sci Total Environ. 2013;442:310–6.

    PubMed  Article  CAS  Google Scholar 

  55. Blair BD, Crago JP, Hedman CJ, Klaper RD. Pharmaceuticals and personal care products found in the Great Lakes above concentrations of environmental concern. Chemosphere. 2013;93:2116–23.

    PubMed  Article  CAS  Google Scholar 

  56. Wieczorkiewicz SM, Kassamali Z, Danziger LH. Behind closed doors: medication storage and disposal in the home. Ann Pharmacother. 2013;47:482–9. This study investigated the disposal of prescription and nonprescription medications, and found that 59% of consumers disposed medications in the household garbage, 31% flushed them down the toilet or sink, suggesting that most consumers are unaware of proper disposal of leftover medications.

    PubMed  Article  Google Scholar 

  57. Daughton CG, Ruhoy IS. The afterlife of drugs and the role of PharmEcovigilance. Drug Saf. 2008;31:1069–82.

    PubMed  Article  CAS  Google Scholar 

  58. Daughton CG. Cradle-to-cradle stewardship of drugs for minimizing their environmental disposition while promoting human health. I. Rationale for and avenues toward a green pharmacy. Environ Health Perspect. 2003;111:757–74.

    PubMed Central  PubMed  Article  CAS  Google Scholar 

  59. Escher BI, Baumgartner R, Koller M, Treyer K, Lienert J, McArdell CS. Environmental toxicology and risk assessment of pharmaceuticals from hospital wastewater. Water Res. 2011;45:75–92.

    PubMed  Article  CAS  Google Scholar 

  60. Aurelien BH, Sylvie B, Alain D, Jerome G, Yves P. Ecotoxicological risk assessment linked to the discharge by hospitals of bio-accumulative pharmaceuticals into aquatic media: the case of mitotane. Chemosphere. 2013;93:2365–72.

    Article  CAS  Google Scholar 

  61. Kummerer J, Hempel M. Green and sustainable pharmacy. 1st ed. Berlin: Springer-Verlag; 2010.

    Book  Google Scholar 

  62. Le-Minh N, Khan SJ, Drewes JE, Stuetz RM. Fate of antibiotics during municipal water recycling treatment processes. Water Res. 2010;44:4295–323.

    PubMed  Article  CAS  Google Scholar 

  63. Petrovic M, De Alda MJL, Diaz-Cruz S, Postigo C, Radjenovic J, Gros M, et al. Fate and removal of pharmaceuticals and illicit drugs in conventional and membrane bioreactor wastewater treatment plants and by riverbank filtration. Philos Trans R Soc A Math Phys Eng Sci. 2009;367:3979–4003.

    Article  CAS  Google Scholar 

  64. Jones OAH, Voulvoulis N, Lester JN. Human pharmaceuticals in wastewater treatment processes. Crit Rev Environ Sci Technol. 2005;35:401–27.

    Article  CAS  Google Scholar 

  65. Onesios KM, Yu JT, Bouwer EJ. Biodegradation and removal of pharmaceuticals and personal care products in treatment systems: a review. Biodegradation. 2009;20:441–66.

    PubMed  Article  CAS  Google Scholar 

  66. Chang PH, Li ZH, Yu TL, Munkhbayer S, Kuo TH, Hung YC, et al. Sorptive removal of tetracycline from water by palygorskite. J Hazard Mater. 2009;165:148–55.

    PubMed  Article  CAS  Google Scholar 

  67. Wilcox JD, Bahr JM, Hedman CJ, Hemming JDC, Barman MAE, Bradbury KR. Removal of organic wastewater contaminants in septic systems using advanced treatment technologies. J Environ Qual. 2009;38:149–56.

    PubMed  Article  CAS  Google Scholar 

  68. Werner JJ, McNeill K, Arnold WA. Photolysis of chlortetracycline on a clay surface. J Agric Food Chem. 2009;57:6932–7.

    PubMed  Article  CAS  Google Scholar 

  69. Santoke H, Song WH, Cooper WJ, Greaves J, Miller GE. Free-radical-induced oxidative and reductive degradation of fluoroquinolone pharmaceuticals: kinetic studies and degradation mechanism. J Phys Chem A. 2009;113:7846–51.

    PubMed  Article  CAS  Google Scholar 

  70. Hu L, Martin HM, Arcs-Bulted O, Sugihara MN, Keatlng KA, Strathmann TJ. Oxidation of carbamazepine by Mn(VII) and Fe(VI): reaction kinetics and mechanism. Environmental Science &amp. Technology. 2009;43:509–15.

    Article  CAS  Google Scholar 

  71. Leech DM, Snyder MT, Wetzel RG. Natural organic matter and sunlight accelerate the degradation of 17 beta-estradiol in water. Sci Total Environ. 2009;407:2087–92.

    PubMed  Article  CAS  Google Scholar 

  72. Benotti MJ, Brownawell BJ. Microbial degradation of pharmaceuticals in estuarine and coastal seawater. Environ Pollut. 2009;157:994–1002.

    PubMed  Article  CAS  Google Scholar 

  73. Yu TH, Lin AYC, Lateef SK, Lin CF, Yang PY. Removal of antibiotics and non-steroidal anti-inflammatory drugs by extended sludge age biological process. Chemosphere. 2009;77:175–81.

    PubMed  Article  CAS  Google Scholar 

  74. Wu CX, Spongberg AL, Witter JD. Sorption and biodegradation of selected antibiotics in biosolids. J Environ Sci Health Part A Toxic/Hazard Subst Environ Eng. 2009;44:454–61.

    Article  CAS  Google Scholar 

  75. Wu CX, Spongberg AL, Witter JD. Adsorption and degradation of triclosan and triclocarban in solis and biosolids-amended soils. J Agric Food Chem. 2009;57:4900–5.

    PubMed  Article  CAS  Google Scholar 

  76. Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD, Barber LB, et al. Pharmaceuticals, hormones, and other organic wastewater contaminants in US streams, 1999-2000: a national reconnaissance. Environ Sci Technol. 2002;36:1202–11.

    PubMed  Article  CAS  Google Scholar 

  77. Vanderford BJ, Snyder SA. Analysis of pharmaceuticals in water by isotope dilution liquid chromatography/tandem mass spectrometry. Environ Sci Technol. 2006;40:7312–20.

    PubMed  Article  CAS  Google Scholar 

  78. Haggard BE, Bartsch LD. Net changes in antibiotic concentrations downstream from an effluent discharge. J Environ Qual. 2009;38:343–52.

    PubMed  Article  CAS  Google Scholar 

  79. Schultz MM, Furlong ET, Kolpin DW, Werner SL, Schoenfuss HL, Barber LB, et al. Antidepressant pharmaceuticals in two US effluent-impacted streams: occurrence and fate in water and sediment, and selective uptake in fish neural tissue. Environ Sci Technol. 2010;44:1918–25.

    PubMed  Article  CAS  Google Scholar 

  80. Wu CX, Witter JD, Spongberg AL, Czajkowski KP. Occurrence of selected pharmaceuticals in an agricultural landscape, western Lake Erie basin. Water Res. 2009;43:3407–16.

    PubMed  Article  CAS  Google Scholar 

  81. Ferrer I, Thurman EM. Analysis of 100 pharmaceuticals and their degradates in water samples by liquid chromatography/quadrupole time-of-flight mass spectrometry. J Chromatogr A. 2012;1259:148–57.

    PubMed  Article  CAS  Google Scholar 

  82. Young TA, Heidler J, Matos-Perez CR, Sapkota A, Toler T, Gibson KE, et al. Ab initio and in situ comparison of caffeine, triclosan, and triclocarban as indicators of sewage-derived microbes in surface waters. Environ Sci Technol. 2008;42:3335–40.

    PubMed  Article  CAS  Google Scholar 

  83. Boyd GR, Grimm DA. In: McLachlan JA, Guillette LJ, Iguchi T, Toscano WA, editors. Occurrence of pharmaceutical contaminants and screening of treatment alternatives for southeastern Louisiana. 2001. p. 80–9.

    Google Scholar 

  84. Monteiro SC, Boxall ABA. Occurrence and fate of human pharmaceuticals in the environment. In: Whitacre DM, editor. Reviews of environmental contamination and toxicology, vol. 202. Summerfield: Springer; 2010. p. 53–154.

    Chapter  Google Scholar 

  85. Batt AL, Kostich MS, Lazorchak JM. Analysis of ecologically relevant pharmaceuticals in wastewater and surface water using selective solid-phase extraction and UPLC-MS/MS. Anal Chem. 2008;80:5021–30.

    PubMed  Article  CAS  Google Scholar 

  86. Bartelt-Hunt SL, Snow DD, Damon T, Shockley J, Hoagland K. The occurrence of illicit and therapeutic pharmaceuticals in wastewater effluent and surface waters in Nebraska. Environ Pollut. 2009;157:786–91.

    PubMed  Article  CAS  Google Scholar 

  87. Schultz MM, Furlong ET. Trace analysis of antidepressant pharmaceuticals and their select degradates in aquatic matrixes by LC/ESI/MS/MS. Anal Chem. 2008;80:1756–62.

    PubMed  Article  CAS  Google Scholar 

  88. Gibs J, Heckathorn HA, Meyer MT, Klapinski FR, Alebus M, Lippincott RL. Occurrence and partitioning of antibiotic compounds found in the water column and bottom sediments from a stream receiving two wastewater treatment plant effluents in Northern New Jersey, 2008. Sci Total Environ. 2013;458:107–16.

    PubMed  Article  CAS  Google Scholar 

  89. Boyd GR, Reemtsma H, Grimm DA, Mitra S. Pharmaceuticals and personal care products (PPCPs) in surface and treated waters of Louisiana, USA and Ontario, Canada. Sci Total Environ. 2003;311:135–49.

    PubMed  Article  CAS  Google Scholar 

  90. Lindsey ME, Meyer M, Thurman EM. Analysis of trace levels of sulfonamide and tetracycline antimicrobials, in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometry. Anal Chem. 2001;73:4640–6.

    PubMed  Article  CAS  Google Scholar 

  91. Standley LJ, Rudel RA, Swartz CH, Attfield KR, Christian J, Erickson M, et al. Wastewater-contaminated groundwater as a source of endogenous hormones and pharmaceuticals to surface water ecosystems. Environ Toxicol Chem. 2008;27:2457–68.

    PubMed  Article  CAS  Google Scholar 

  92. Guo YC, Krasner SW. Occurrence of primidone, carbamazepine, caffeine, and precursors for n-nitrosodimethylamine in drinking water sources impacted by wastewater. J Am Water Resour Assoc. 2009;45:58–67.

    Article  CAS  Google Scholar 

  93. Spongberg AL, Witter JD. Pharmaceutical compounds in the wastewater process stream in Northwest Ohio. Sci Total Environ. 2008;397:148–57.

    PubMed  Article  CAS  Google Scholar 

  94. Ferguson PJ, Bernot MJ, Doll JC, Lauer TE. Detection of pharmaceuticals and personal care products (PPCPs) in near-shore habitats of southern Lake Michigan. Sci Total Environ. 2013;458:187–96.

    PubMed  Article  CAS  Google Scholar 

  95. Halden RU, Paull DH. Analysis of triclocarban in aquatic samples by liquid chromatography electrospray ionization mass spectrometry. Environ Sci Technol. 2004;38:4849–55.

    PubMed  Article  CAS  Google Scholar 

Download references

Acknowledgments

The author acknowledges support from Grand Canyon University, and Professor Rolf Halden of Arizona State University.

Compliance with Ethics Guidelines

Conflict of Interest

Randhir P. Deo declares that he has no conflict of interest.

Human and Animal Rights and Informed Consent

This article does not contain any studies with human or animal subjects performed by any of the authors.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Randhir P. Deo.

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Deo, R.P. Pharmaceuticals in the Surface Water of the USA: A Review. Curr Envir Health Rpt 1, 113–122 (2014). https://doi.org/10.1007/s40572-014-0015-y

Download citation

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s40572-014-0015-y

Keywords

  • Risk assessment
  • Surface water
  • Biosolids
  • Pharmaceuticals
  • Review
  • Antibiotics
  • Effluents
  • Fate
  • Antibiotics
  • Antidepressants
  • Contraceptives
  • Disinfectants
  • Sustainable
  • Management