Zerovalent Iron/Cu Combined Degradation of Halogenated Disinfection Byproducts and Quantitative Structure-Activity Relationship Modeling.

Previous studies have reported that zerovalent iron (ZVI) can reduce several aliphatic groups of disinfection byproducts (DBPs) (e.g., haloacetic acids and haloacetamides) effectively, and the removal efficiency can be significantly improved by metallic copper. Information regarding ZVI/Cu combined degradation of different types of halogenated DBPs can help understand the fate of overall DBPs in drinking water distribution and storage systems consisting of unlined cast iron/copper pipes and related potential control strategies. In this study, we found that, besides aliphatic DBPs, many groups of new emerging aromatic DBPs formed in chlorinated and chloraminated drinking water can be effectively degraded by ZVI/Cu; meanwhile, total organic halogen and total ion intensity were reduced significantly after treatment. Moreover, a robust quantitative structure-activity relationship model was developed and validated based on the ZVI/Cu combined degradation rate constants of 14 typical aromatic DBPs; it can predict the degradation rate constants of other aromatic DBPs for screening and comparative purposes, and the optimized descriptors indicate that DBPs possessing a lower value of the lowest unoccupied molecular orbital energy and a higher value of dipole moment tend to present higher degradation rate constants. In addition, toxicity data of 47 DBPs (belonging to 18 groups) were predicted by two previously established toxicity models, demonstrating that, although most DBPs exhibit higher toxicity than their dehalogenated products, some DBPs show lower toxicity than their lowly halogenated analogs.

Current and future perspectives for wastewater-based epidemiology as a monitoring tool for pharmaceutical use.

The medical and societal consequences of the misuse of pharmaceuticals clearly justify the need for comprehensive drug utilization research (DUR). Wastewater-based epidemiology (WBE) employs the analysis of human metabolic excretion products in wastewater to monitor consumption patterns of xenobiotics at the population level. Recently, WBE has demonstrated its potential to evaluate lifestyle factors such as illicit drug, alcohol and tobacco consumption at the population level, in near real-time and with high spatial and temporal resolution. Up until now there have been fewer WBE studies investigating health biomarkers such as pharmaceuticals. WBE publications monitoring the consumption of pharmaceuticals were systematically reviewed from three databases (PubMed, Web of Science and Google Scholar). 64 publications that reported population-normalised mass loads or defined daily doses of pharmaceuticals were selected. We document that WBE could be employed as a complementary information source for DUR. Interest in using WBE approaches for monitoring pharmaceutical use is growing but more foundation research (e.g. compound-specific uncertainties) is required to link WBE data to routine pharmacoepidemiologic information sources and workflows. WBE offers the possibility of i) estimating consumption of pharmaceuticals through the analysis of human metabolic excretion products in wastewater; ii) monitoring spatial and temporal consumption patterns of pharmaceuticals continuously and in near real-time; and iii) triangulating data with other DUR information sources to assess the impacts of strategies or interventions to reduce inappropriate use of pharmaceuticals.

Long-term trends in tobacco use assessed by wastewater-based epidemiology and its relationship with consumption of nicotine containing products.

Measurement of population tobacco use via wastewater-based epidemiology (WBE) provides objective data to evaluate the efficacy of tobacco control strategies. However, current WBE tobacco-use estimates based on nicotine metabolites (cotinine and hydroxycotinine) can be masked by use of non-tobacco nicotine-containing products. To better understand nicotine and tobacco use, we analysed tobacco-specific biomarkers, anabasine and anatabine, as well as nicotine metabolites, cotinine and hydroxycotinine, in wastewater samples collected for 6 weeks per year over 6 years (2012-2017) from an Australian wastewater treatment plant serving approximately 100,000 people. Population-normalised mass loads were used to estimate tobacco and nicotine use trends and were compared with surveys and taxation statistics. Significant annual declines were observed for anabasine, anatabine, cotinine and hydroxycotinine of -3.0%, -2.7%, -2.4%, and -2.1%, respectively. The results corresponded with the annual declining trends reported from surveys (-5%) and taxation statistics (-4%). Significant annual decreases in the ratios of anabasine to cotinine (-1.2%) and anatabine to cotinine (-1.0%) suggested a relative increase in the use of non-tobacco nicotine products at the same time that tobacco use was declining. Monitoring tobacco use with anabasine and anatabine removed influence from nicotine-containing products, showing larger reductions in this Australian city than via nicotine biomarkers, whilst also demonstrating their suitability for monitoring long-term trends.

Using wastewater-based epidemiology to estimate consumption of alcohol and nicotine in major cities of China in 2014 and 2016.

Monitoring the use of alcohol and tobacco in the population is important for public health planning and evaluating the efficacy of intervention strategies. The aim of this study was to use wastewater-based epidemiology (WBE) to estimate alcohol and tobacco consumption in a number of major cities across China and compare WBE estimates with other data sources. Daily composite influent wastewater samples were collected from wastewater treatment plants (WWTPs) across China in 2014 (n = 53) and 2016 (n = 45). The population-normalized daily consumption estimated by WBE were compared with other data sources where available. The average consumption of alcohol was 8.1 ± 7.0 mL ethanol/person aged 15+/day (EPD) in the investigated cities of 2016 while those involved in 2014 had an average consumption of 4.7 ± 3.0 EPD. The average tobacco consumption was estimated to be 3.7 ± 2.2 cigarettes/person aged 15+/day (CPD) in 2016 and 3.1 ± 1.9 CPD in 2014. The changes in the average consumption in those cities from 2014 to 2016 were supported by the results from a limited number of WWTPs where samples were collected in both years. Consumption of alcohol and tobacco in urban China is at a medium level compared with other countries on a per capita basis. WBE estimates of tobacco consumption were relatively comparable with results of traditional surveys and sales statistics. WBE estimates of alcohol consumption were lower than WHO survey results, probably due to EtS degradation and uncertainty in the EtS excretion factor.

Stability of alcohol and tobacco consumption biomarkers in a real rising main sewer.

Since alcohol and tobacco consumption are among the leading causes of population health harm, it is very important to understand the consumption behaviour to develop effective harm reduction strategies. Wastewater-based epidemiology (WBE) is a potential tool for estimating their consumption, but there are several uncertainties that need to be determined, including the stability of biomarkers in the sewer. Utilizing a real rising main sewer, this study investigated the stability of alcohol and tobacco consumption biomarkers. Rhodamine and acesulfame were used as flow tracer and benchmarker to understand the transportation of wastewater in the sewer with a hydraulic retention time between 2.7 and 5.0 h. Ethyl sulphate (EtS) and ethyl glucuronide (EtG), two biomarkers of alcohol consumption, were found to have different in-sewer stability, with EtS much more stable than EtG. The degradation rate of EtS is approximately 8% per hour, while EtG has a half-life of 1.9 h. Formation of nicotine, cotinine and trans-3'-hydroxycotinine, three biomarkers for tobacco consumption, was observed during the experiment, probably due to deconjugation of their glucuronide chemicals. The deconjugation process has prevented the determination of actual stability of the three chemicals. However, it is suggested that cotinine is relatively stable, while nicotine and trans-3'-hydroxycotinine degrade to a certain degree in the sewer system. According to our findings, the in-sewer degradation is more important during the interpretation of alcohol consumption estimation than for tobacco consumption estimation.