Monitoring Contaminants of Emerging Concern in Global Wastewater Using Sewage Epidemiology

This dissertation applies wastewater-based epidemiology (WBE) to aqueous process flows to gauge the public health status concerning exposure and potential abuse of pharmaceuticals, antimicrobials, and narcotics. The masses of emerging contaminants emitted into Indian aquatic and terrestrial environments were the highest for open defecation (17 ± 12 mt/d), with non-steroidal anti-inflammatory drugs dominating environmental loading (14 ± 10 mt/d), followed by antibiotics, antimicrobials, phthalates and miscellaneous pharmaceuticals (Chapter 2). Fourteen wastewater treatment plants sampled across the U.S. had a combined average mass loading of 71 ± 12 µg/d/capita for the antimicrobials triclosan and triclocarban, with paraben compounds contributing 19 ± 5 µg/d/US capita. Risk models showed unfavorable hazard quotients (HQ>1) for sensitive aquatic organisms (algae, zebra fish and rainbow trout) from predicted exposures to antimicrobials of alternative use, i.e., chlorhexidine and benzalkonium chloride (Chapter 3). Substances subject to licit and illicit use, monitored by WBE in a medium-sized southwestern U.S. city before and during COVID-19-related lockdowns, showed the highest mass loads for cocaine and its major metabolite benzoylecgonine (2,207 total), methadone and its major metabolite 2-Ethylidene-1,5-dimethyl-3,3-diphenylpyrrolidine (197), parent mitragynine (60), oxycodone and its major metabolite noroxycodone (48), heroin and its major metabolite 6-acetylmorphine (45), and parent codeine (37) in mg/1,000 capita/day. Heroin use during the lockdown increased ~10-fold relative to the pre-lockdown baseline, whereas oxycodone and codeine mass loading decreased 5-fold and 2.5-fold, respectively (Chapter 4). Experiments elucidating the stability of stress hormones and their metabolites as a function of temperature and in-sewer residence time revealed a rapid degradation to completion over 24 hours at 35°C, whereas lower temperatures of 25°C and 15°C were found to allow for successful tracking of indicators of stress at the population level; statistically significant differences in stress hormone decay rates were observed due to geographic locations at 25°C (p=0.009) but not due to redox conditions in the sewer pipe (Chapter 5). This thesis demonstrated the successful application of WBE for studying population health frequently and inexpensively, with the limitation that a lack of centralized wastewater infrastructure in developing countries may create barriers for at-risk populations to access and utilize this novel technology (Chapter 6).