Addressing wastewater epidemiology limitations with the use of dynamic population surrogates, complementary urinalyses and in-situ experiments Public Deposited


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  • Wastewater epidemiology is an emerging discipline that requires collaborative research involving analytical chemists, drug epidemiologists, and wastewater engineers. Wastewater epidemiology involves the sampling and quantitative analysis of raw wastewaters from communities for illicit drugs and their metabolites. Mass loads (mass per day) and per capita (mg per day per person) are then calculated from concentrations and indicate the approximate quantity of illicit drugs used and excreted by the community. Limitations to wastewater epidemiology include that the population served by wastewater treatment plants within a day and between days is not well known. In addition, biodegradation of illicit drugs during transit in sewers may affect the concentration and mass flows that reach wastewater treatment plants. This thesis describes a series of studies conducted by an international collaboration between scientists and engineers from the United States and Switzerland to answer these two limitations. The experimental approaches for these studies used included high-frequency wastewater sampling strategies, the use of creatinine as a human urinary biomarker, as well as the use of unique locations as test sites including an open community, a prison in the state of Oregon, and a 5 km section of sewer in Zürich Switzerland. In Chapter 2, the diurnal study on the mass flows of illicit drugs or metabolites was formed over four days in a municipality with a population of approximately 55,000 people. The diurnal trends in illicit substances vary by substance. The high (g/day) mass flows of caffeine, methamphetamine, and creatinine indicate that lower-frequency sampling (approximately one sample per h) may representatively capture the use and excretion of these substances. However, lower and episodic mass flows of cocaine and its primary human metabolite, benzoylecgonine, indicate that higher-frequency is needed to accurately assess the use of the cocaine within the municipality. Normalization of illicit substances to creatinine gave between-day trends in illicit and legal substances that differed from non-normalized trends. Resident use of cocaine and methamphetamine were indicated by normalized mass flows that increased during early morning hours while commuters are largely absent from the community. Chapter 3 describes a series of experiments conducted at an Oregon state prison. The prison setting provided a unique opportunity to study a nearly-fixed population of individuals and their corresponding mass flows of illicit substances, the number of doses per person consumed, as well as an opportunity to quantify the level of agreement between numbers of individuals and the measured mass flows of creatinine. Methamphetamine use was more prevalent than cocaine/benzoylecgonine in the prison over the one month study in which single daily (24 h) composite samples of wastewater were collected. The hypothesis that the mass flows of methamphetamine and cocaine would be lower on days on which random urinalysis testing (RUA) is typically conducted by the prison (Monday-Thursday) was rejected. While the mass flows (mg/d) of methamphetamine were less than those for a nearby open community, the number of estimated doses per person was higher for the prison population. A higher number of positive RUA results were obtained for methamphetamine while none were positive for cocaine, which is consistent with the data obtained from wastewater. The hourly (diurnal) trend in methamphetamine mass loads indicated continual methamphetamine use/excretion inside the prison while cocaine and benzoylecgonine were detected in five hourly composite samples. Use of methamphetamine and cocaine by inmates could not be unambiguously distinguished from that of non-inmates (employees and visitors). The observed diurnal trends in creatinine mass loads were similar to those of an open community and are indicative of the general pattern of human wakefulness/activity. Predicted creatinine mass loads based on the total prison (inmates + non-inmates) were in good agreement with the measured mass loads, which indicates the potential use of creatinine as a quantitative population indicator. Additional research on the biodegradability of creatinine is needed because the prison setting was deliberately selected to minimize the potential for creatinine biodegradation. Chapter 4 addresses the data gap that exists on illicit drug transformation during in situ transit in sewers. The rates of in situ biodegradation have not yet been determined for conditions that are relevant to sewers, which include low to variable oxygen concentrations, the presence of a biofilm, and temperatures ≤ 20 °C. For this reason, two tracer tests were conducted in a 5 km stretch of sewer located near Zürich, Switzerland. The stable-isotope forms (deuterated) of cocaine and benzoylecgonine were injected into flowing wastewater and three locations up to 5 km downstream were sampled over time. Breakthrough curves were constructed from measurements of cocaine-d3 and benzoylecgonine-d3 concentration with time. The area under the curve (mass) was determined by integrating concentration over time. Benzoylecgonine-d3 was present in the injectate that should have only contained cocaine-d3; because the benzoylecgonine-d3 formation prior to injection is not known. The injected mass of cocaine-d3 did not decline over the 5 km distance. The observed mass of cocaine-d3 at 5 km was 10% greater than at 500 m, which indicates that the transformation of cocaine was not significant over the 1.5 h experiment. At 5 km downgradient, the apparent mass of benzoylecgonine-d3 had increased by 35% over that observed at 500 m. However, the apparent increase in benzoylecgonine-d3 mass was not accompanied by a corresponding loss of cocaine-d3. While uncertainty is apparent in the increase of both cocaine-d3 and benzoylecgonine-d3, the ratio of cocaine-d3/benzoylecgonine-d3 is subject only to analytical error because any errors associated with sampling and the integration of masses cancel out. The ratio of cocaine-d3/benzoylecgonine-d3 declined from 2.98 in the injectate to 1.66 at Location 3, which indicated a greater increase in benzoylecgonine-d3 relative to cocaine over the 5 km distance. Due to the benzoylecgonine-d3 that was present in the injectate, any biodegradation of cocaine-c3 to form benzoylecgonine-d3 could not be unambiguously distinguished. During the second tracer test in which benzoylecgonine-d3 was injected, the mass of benzoylecgonine-d3 did not significantly decline, which suggests that the apparent loss of benzoylecgonine-d3 during the cocaine-d3 test cannot be attributed to in-situ biodegradation. Overall, while uncertainty exists about the integrated masses for cocaine-d3 and benzoylecgonine-d3, the 5 km distance was too short in order to observe a significant loss of cocaine-d3 and formation of benzoylecgonine-d3. Recommendations for future research include conducting analysis on the injectate solution to ensure that only cocaine-d3 is introduced so that any formation of benzoylecgonine-d3 is readily apparent and quantifiable. In addition, the tracer tests should be repeated in a longer section of sewer to increase the residence time beyond 1.5 hr and degradation products of benzoylecgonine-d3 should be monitored including ecgonine and ecgonine methyl ester.
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