Non-targeted analysis and toxicity prediction for evaluation of photocatalytic membrane distillation removing organic contaminants from hypersaline oil and gas field-produced water.

Membrane distillation (MD) has received ample recognition for treating complex wastewater, including hypersaline oil and gas (O&G) produced water (PW). Rigorous water quality assessment is critical in evaluating PW treatment because PW consists of numerous contaminants beyond the targets listed in general discharge and reuse standards. This study evaluated a novel photocatalytic membrane distillation (PMD) process, with and without a UV light source, against a standard vacuum membrane distillation (VMD) process for treating PW, utilizing targeted analyses and a non-targeted chemical identification workflow coupled with toxicity predictions. PMD with UV light resulted in better removals of dissolved organic carbon, ammoniacal nitrogen, and conductivity. Targeted organic analyses identified only trace amounts of acetone and 2-butanone in distillates. According to non-targeted analysis, the number of suspects reduced from 65 in feed to 25-30 across all distillate samples. Certain physicochemical properties of compounds influenced contaminant rejection in different MD configurations. According to preliminary toxicity predictions, VMD, PMD with and without UV distillate samples, respectively contained 21, 22, and 23 suspects associated with critical toxicity concerns. Overall, non-targeted analysis together with toxicity prediction provides a competent supportive tool to assess treatment efficiency and potential impacts on public health and the environment during PW reuse.

Water, Water Everywhere, but Every Drop Unique: Challenges in the Science to Understand the Role of Contaminants of Emerging Concern in the Management of Drinking Water Supplies.

The protection and management of water resources continues to be challenged by multiple and ongoing factors such as shifts in demographic, social, economic, and public health requirements. Physical limitations placed on access to potable supplies include natural and human-caused factors such as aquifer depletion, aging infrastructure, saltwater intrusion, floods, and drought. These factors, although varying in magnitude, spatial extent, and timing, can exacerbate the potential for contaminants of concern (CECs) to be present in sources of drinking water, infrastructure, premise plumbing and associated tap water. This monograph examines how current and emerging scientific efforts and technologies increase our understanding of the range of CECs and drinking water issues facing current and future populations. It is not intended to be read in one sitting, but is instead a starting point for scientists wanting to learn more about the issues surrounding CECs. This text discusses the topical evolution CECs over time (Section 1), improvements in measuring chemical and microbial CECs, through both analysis of concentration and toxicity (Section 2) and modeling CEC exposure and fate (Section 3), forms of treatment effective at removing chemical and microbial CECs (Section 4), and potential for human health impacts from exposure to CECs (Section 5). The paper concludes with how changes to water quantity, both scarcity and surpluses, could affect water quality (Section 6). Taken together, these sections document the past 25 years of CEC research and the regulatory response to these contaminants, the current work to identify and monitor CECs and mitigate exposure, and the challenges facing the future.

Onsite Nonpotable Water Systems Pathogen Treatment Targets: A Comparison of Infection and Disability-Adjusted Life Years (DALYs) Risk Benchmark Approaches.

Pathogen log10 reduction targets for onsite nonpotable water systems were calculated using both annual infection (LRTINF) and disability-adjusted life year (LRTDALY) benchmarks. The DALY is a measure of the health burden of a disease, accounting for both the severity and duration of illness. Results were evaluated to identify if treatment requirements change when accounting for the likelihood, duration, and severity of illness in addition to the likelihood of infection. The benchmarks of 10-4 infections per person per year (ppy) and 10-6 DALYs ppy were adopted along with multilevel dose-response models for Norovirus and Campylobacter jejuni, which characterize the probability of illness given infection (Pill|inf) as dose-dependent using challenge or outbreak data. We found differences between treatment requirements, LRTINF - LRTDALY, for some pathogens, driven by the likelihood of illness, rather than the severity of illness. For pathogens with dose-independent Pill|inf characterizations, such as Cryptosporidium spp., Giardia, and Salmonella enterica, the difference, LRTINF - LRTDALY, was identical across reuse scenarios (

Enteric pathogen reduction targets for onsite non-potable water systems: A critical evaluation.

Onsite non-potable water systems (ONWS) collect and treat local source waters for non-potable end uses such as toilet flushing and irrigation. Quantitative microbial risk assessment (QMRA) has been used to set pathogen log10-reduction targets (LRTs) for ONWS to achieve the risk benchmark of 10-4 infections per person per year (ppy) in a series of two efforts completed in 2017 and 2021. In this work, we compare and synthesize the ONWS LRT efforts to inform the selection of pathogen LRTs. For onsite wastewater, greywater, and stormwater, LRTs for human enteric viruses and parasitic protozoa were within 1.5-log10 units between 2017 and 2021 efforts, despite differences in approaches used to characterize pathogens in these waters. For onsite wastewater and greywater, the 2017 effort used an epidemiology-based model to simulate pathogen concentrations contributed exclusively from onsite waste and selected Norovirus as the viral reference pathogen; the 2021 effort used municipal wastewater pathogen data and cultivable adenoviruses as the reference viral pathogen. Across source waters, the greatest differences occurred for viruses in stormwater, given the newly available municipal wastewater characterizations used for modeling sewage contributions in 2021 and the different selection of reference pathogens (Norovirus vs. adenoviruses). The roof runoff LRTs support the need for protozoa treatment, but these remain difficult to characterize due to the pathogen variability in roof runoff across space and time. The comparison highlights adaptability of the risk-based approach, allowing for updated LRTs as site specific or improved information becomes available. Future research efforts should focus on data collection of onsite water sources.

Geospatial Patterns of Antimicrobial Resistance Genes in the US EPA National Rivers and Streams Assessment Survey.

Antimicrobial resistance (AR) is a serious global problem due to the overuse of antimicrobials in human, animal, and agriculture sectors. There is intense research to control the dissemination of AR, but little is known regarding the environmental drivers influencing its spread. Although AR genes (ARGs) are detected in many different environments, the risk associated with the spread of these genes to microbial pathogens is unknown. Recreational microbial exposure risks are likely to be greater in water bodies receiving discharge from human and animal waste in comparison to less disturbed aquatic environments. Given this scenario, research practitioners are encouraged to consider an ecological context to assess the effect of environmental ARGs on public health. Here, we use a stratified, probabilistic survey of nearly 2000 sites to determine national patterns of the anthropogenic indicator class I integron Integrase gene (intI1) and several ARGs in 1.2 million kilometers of United States (US) rivers and streams. Gene concentrations were greater in eastern than in western regions and in rivers and streams in poor condition. These first of their kind findings on the national distribution of intI1 and ARGs provide new information to aid risk assessment and implement mitigation strategies to protect public health.

Quantitative Microbial Risk Assessment of Antimicrobial Resistant and Susceptible Staphylococcus aureus in Reclaimed Wastewaters.

The annual risks of colonization, skin infection, bloodstream infection (BSI), and disease burden from exposures to antibiotic-resistant and susceptible Staphylococcus aureus (S. aureus) were estimated using quantitative microbial risk assessment (QMRA). We estimated the probability of nasal colonization after immersion in wastewater (WW) or greywater (GW) treated across a range of treatment alternatives and subsequent infection. Horizontal gene transfer was incorporated into the treatment model but had little effect on the predicted risk. The cumulative annual probability of infection (resulting from self-inoculation) was most sensitive to the treatment log10 reduction value (LRV), S. aureus concentration, and the newly calculated morbidity ratios and was below the health benchmark of 10-4 infections per person per year (ppy) given a treatment LRV of roughly 3.0. The predicted annual disability-adjusted life years (DALYs), which were dominated by BSI, were below the health benchmark of 10-6 DALYs ppy for resistant and susceptible S. aureus, given LRVs of 4.5 and 3.5, respectively. Thus, the estimated infection risks and disease burdens resulting from nasal colonization are below the relevant health benchmarks for risk-based, nonpotable, or potable reuse systems but possibly above for immersion in minimally treated GW or WW. Strain-specific data to characterize dose-response and concentration in WW are needed to substantiate the QMRA.

Standardizing data reporting in the research community to enhance the utility of open data for SARS-CoV-2 wastewater surveillance.

SARS-CoV-2 RNA detection in wastewater is being rapidly developed and adopted as a public health monitoring tool worldwide. With wastewater surveillance programs being implemented across many different scales and by many different stakeholders, it is critical that data collected and shared are accompanied by an appropriate minimal amount of metainformation to enable meaningful interpretation and use of this new information source and intercomparison across datasets. While some databases are being developed for specific surveillance programs locally, regionally, nationally, and internationally, common globally-adopted data standards have not yet been established within the research community. Establishing such standards will require national and international consensus on what metainformation should accompany SARS-CoV-2 wastewater measurements. To establish a recommendation on minimum information to accompany reporting of SARS-CoV-2 occurrence in wastewater for the research community, the United States National Science Foundation (NSF) Research Coordination Network on Wastewater Surveillance for SARS-CoV-2 hosted a workshop in February 2021 with participants from academia, government agencies, private companies, wastewater utilities, public health laboratories, and research institutes. This report presents the primary two outcomes of the workshop: (i) a recommendation on the set of minimum meta-information that is needed to confidently interpret wastewater SARS-CoV-2 data, and (ii) insights from workshop discussions on how to improve standardization of data reporting.

A risk-based evaluation of onsite, non-potable reuse systems developed in compliance with conventional water quality measures.

Water quality standards (WQSs) based on water quality measures (e.g., fecal indicator bacteria (FIB)) have been used by regulatory agencies to assess onsite, non-potable water reuse systems. A risk-based approach, based on quantitative microbial risk assessment, was developed to define treatment requirements that achieve benchmark levels of risk. This work compared these approaches using the predicted annual infection risks for non-potable reuse systems that comply with WQSs along with the benchmark risk levels achieved by the risk-based systems. The systems include a recirculating synthetic sand filter or an aerobic membrane bioreactor (MBR) combined with disinfection. The greywater MBR system had predicted risks in the range of the selected benchmark levels. However, wastewater reuse with systems that comply with WQSs had uncertain and potentially high predicted risks (i.e., >10-2 infections per person per year) in residential applications, due to exposures to viruses and protozoa. The predicted risks illustrate that WQSs based on FIB treatment performance do not ensure adequate treatment removal of viruses and protozoa. We present risk-based log10 pathogen reduction targets for intermediate-sized non-potable systems, which are 0.5 log10 less than those previously proposed for district-sized systems. Still, pathogen treatment performance data are required to better manage non-potable reuse risk.

Enteric Pathogen Treatment Requirements for Nonpotable Water Reuse Despite Limited Exposure Data.

Exposure factors (e.g., ingestion volume and frequency) are required to establish risk-based treatment requirements (i.e., log10 reduction targets (LRTs)) for enteric pathogens using quantitative microbial risk assessment (QMRA). However, data to Wastewater characterize nonpotable exposure factors are sparse. We calculated graywater and wastewater nonpotable LRTs (corresponding to 10-4 infections per person per year) for uses missing detailed exposure data (including showering and decorative fountain) and across a range of exposure factors. The LRTs decreased linearly toward zero as the log10 transformed volume or the frequency of reuse decreased. When nonroutine exposure was included, representing either accidental ingestion from misuse or cross-connection between potable and nonpotable waters, the LRTs remained high, even as the routine ingestion volume decreased. Therefore, uses with small anticipated routine ingestion volumes (i.e., roughly <10-5 L), e.g., domestic indoor or decorative fountain uses, share common LRTs, and further refinement of the routine exposure is of limited value. Additional data to characterize nonroutine exposures and uses with high routine ingestion, e.g., showering, remain valuable to better estimate LRTs. These results will assist regulators in the selection of LRTs for nonpotable uses that lack detailed exposure factor characterizations.

Droplet digital PCR quantification of norovirus and adenovirus in decentralized wastewater and graywater collections: Implications for onsite reuse.

Risk-based treatment of onsite wastewaters for decentralized reuse requires information on the occurrence and density of pathogens in source waters, which differ from municipal wastewater due to scaling and dilution effects in addition to variable source contributions. In this first quantitative report of viral enteric pathogens in onsite-collected graywater and wastewater, untreated graywater (n = 50 samples) and combined wastewater (i.e., including blackwater; n = 28) from three decentralized collection systems were analyzed for two norovirus genogroups (GI/GII) and human adenoviruses using droplet digital polymerase chain reaction (ddPCR). Compared to traditional quantitative PCR (qPCR), which had insufficient sensitivity to quantify viruses in graywater, ddPCR allowed quantification of norovirus GII and adenovirus in 4% and 14% of graywater samples, respectively (none quantifiable for norovirus GI). Norovirus GII was routinely quantifiable in combined wastewater by either PCR method (96% of samples), with well-correlated results between the analyses (R2 = 0.96) indicating a density range of 5.2-7.9 log10 genome copies/L. These concentrations are greater than typically reported in centralized municipal wastewater, yet agree well with an epidemiology-based model previously used to develop pathogen log-reduction targets (LRTs) for decentralized non-potable water systems. Results emphasize the unique quality of onsite wastewaters, supporting the previous LRTs and further quantitative microbial risk assessment (QMRA) of decentralized water reuse.

Human health impact of non-potable reuse of distributed wastewater and greywater treated by membrane bioreactors.

We assessed the annual probability of infection resulting from non-potable exposures to distributed greywater and domestic wastewater treated by an aerobic membrane bioreactor (MBR) followed by chlorination. A probabilistic quantitative microbial risk assessment was conducted for both residential and office buildings and a residential district using Norovirus, Rotavirus, Campylobacter jejuni, and Cryptosporidium spp. as reference pathogens. A Monte Carlo approach captured variation in pathogen concentration in the collected water and pathogen (or microbial surrogate) treatment performance, when available, for various source water and collection scale combinations. Uncertain inputs such as dose-response relationships and the volume ingested were treated deterministically and explored through sensitivity analysis. The predicted 95th percentile annual risks for non-potable indoor reuse of distributed greywater and domestic wastewater at district and building scales were less than the selected health benchmark of 10-4 infections per person per year (ppy) for all pathogens except Cryptosporidium spp., given the selected exposure (which included occasional, accidental ingestion), dose-response, and treatment performance assumptions. For Cryptosporidium spp., the 95th percentile annual risks for reuse of domestic wastewater (for all selected collection scenarios) and district-collected greywater were greater than the selected health benchmark when using the limited, available MBR treatment performance data; this finding is counterintuitive given the large size of Cryptosporidium spp. relative to the MBR pores. Therefore, additional data on MBR removal of protozoa is required to evaluate the proposed MBR treatment process for non-potable reuse. Although the predicted Norovirus annual risks were small across scenarios (less than 10-7 infections ppy), the risks for Norovirus remain uncertain, in part because the treatment performance is difficult to interpret given that the ratio of total to infectious viruses in the raw and treated effluents remains unknown. Overall, the differences in pathogen characterization between collection type (i.e., office vs. residential) and scale (i.e., district vs. building) drove the differences in predicted risk; and, the accidental ingestion event (although modeled as rare) determined the annual probability of infection. The predicted risks resulting from treatment malfunction scenarios indicated that online, real-time monitoring of both the MBR and disinfection processes remains important for non-potable reuse at distributed scales. The resulting predicted health risks provide insight on the suitability of MBR treatment for distributed, non-potable reuse at different collection scales and the potential to reduce health risks for non-potable reuse.

Human Health Impact of Cross-Connections in Non-Potable Reuse Systems.

We used quantitative microbial risk assessment (QMRA) to estimate the microbial risks from two contamination pathways in onsite non-potable water systems (ONWS): contamination of potable water by (treated) reclaimed, non-potable water and contamination of reclaimed, non-potable water by wastewater or greywater. A range of system sizes, event durations, fraction of users exposed, and intrusion dilutions were considered (chlorine residual disinfection was not included). The predicted annual microbial infection risk from domestic, non-potable reuse remained below the selected benchmark given isolated, short-duration intrusion (i.e., 5-day) events of reclaimed water in potable water. Whereas, intrusions of wastewater into reclaimed, non-potable water resulted in unacceptable annual risk without large dilutions or pathogen inactivation. We predicted that 1 user out of 10,000 could be exposed to a 5-day contamination event of undiluted wastewater in the reclaimed, non-potable water system each year to meet the annual benchmark risk of 10-4 infections per person per year; whereas, 1 user out of 1000 could be exposed to a 5-day contamination event of undiluted reclaimed water in the potable water each year. Overall, the predicted annual risks support the use of previously derived non-potable reuse treatment requirements for a variety of ONWS sizes and support the prioritization of protective measures to prevent the intrusion of wastewater into domestic ONWS.

Risk-based enteric pathogen reduction targets for non-potable and direct potable use of roof runoff, stormwater, and greywater.

This paper presents risk-based enteric pathogen log reduction targets for non-potable and potable uses of a variety of alternative source waters (i.e., locally-collected greywater, roof runoff, and stormwater). A probabilistic Quantitative Microbial Risk Assessment (QMRA) was used to derive the pathogen log10 reduction targets (LRTs) that corresponded with an infection risk of either 10-4 per person per year (ppy) or 10-2 ppy. The QMRA accounted for variation in pathogen concentration and sporadic pathogen occurrence (when data were available) in source waters for reference pathogens in the genera Rotavirus, Mastadenovirus(human adenoviruses), Norovirus, Campylobacter, Salmonella, Giardia and Cryptosporidium. Non-potable uses included indoor use (for toilet flushing and clothes washing) with occasional accidental ingestion of treated non-potable water (or cross-connection with potable water), and unrestricted irrigation for outdoor use. Various exposure scenarios captured the uncertainty from key inputs, i.e., the pathogen concentration in source water; the volume of water ingested; and for the indoor use, the frequency of and the fraction of the population exposed to accidental ingestion. Both potable and non-potable uses required pathogen treatment for the selected waters and the LRT was generally greater for potable use than non-potable indoor use and unrestricted irrigation. The difference in treatment requirements among source waters was driven by the microbial quality of the water - both the density and occurrence of reference pathogens. Greywater from collection systems with 1000 people had the highest LRTs; however, those for greywater collected from a smaller population (~ 5 people), which have less frequent pathogen occurrences, were lower. Stormwater had highly variable microbial quality, which resulted in a range of possible treatment requirements. The microbial quality of roof runoff, and thus the resulting LRTs, remains uncertain due to lack of relevant pathogen data.

Simulation of enteric pathogen concentrations in locally-collected greywater and wastewater for microbial risk assessments.

As decentralized water reuse continues to gain popularity, risk-based treatment guidance is increasingly sought for the protection of public health. However, effort s to evaluate pathogen risks and log-reduction requirements have been hindered by an incomplete understanding of pathogen occurrence and densities in locally-collected wastewaters (i.e., from decentralized collection systems). Of particular interest is the potentially high enteric pathogen concentration in small systems with an active infected excreter, but generally lower frequency of pathogen occurrences in smaller systems compared to those with several hundred contributors. Such variability, coupled with low concentrations in many source streams (e.g., sink, shower/bath, and laundry waters), has limited direct measurement of pathogens. This study presents an approach to modeling pathogen concentrations in variously sized greywater and combined wastewater collection systems based on epidemiological pathogen incidence rates, user population size, and fecal loadings to various residential wastewater sources. Pathogen infections were modeled within various population sizes (5-, 100-, and 1,000-person) for seven reference pathogens (viruses: adenoviruses, Norovirus, and Rotavirus; bacteria: Campylobacter and Salmonella spp.; and protozoa: Cryptosporidium and Giardia spp.) on each day of 10,000 possible years, accounting for intermittent infection and overlap of infection periods within the population. Fecal contamination of fresh greywaters from bathroom sinks, showers/baths, and laundry, as well as combined greywater and local combined wastewater (i.e., including toilets), was modeled based on reported fecal indicators in the various sources. Simulated daily infections and models of fecal contamination were coupled with pathogen shedding characteristics to generate distributions of pathogen densities in the various waters. The predicted frequency of pathogen occurrences in local wastewaters was generally low due to low infection incidence within small cohort groups, but increased with collection scale (population size) and infection incidence rate (e.g., Norovirus). When pathogens did occur, a decrease in concentrations from 5- to 100- and from 100- to 1,000-person systems was observed; nonetheless, overall mean concentrations (i.e., including non-occurrences) remained the same due to the increased number of occurrences. This highlights value of the model for characterizing scaling effects over averaging methods, which overestimate the frequency of pathogen occurrence in small systems while underestimating concentration peaks that likely drive risk periods. Results of this work will inform development of risk-based pathogen reduction requirements for decentralized water reuse.

Bioaerosol Deposition to Food Crops near Manure Application: Quantitative Microbial Risk Assessment.

Production of both livestock and food crops are central priorities of agriculture; however, food safety concerns arise where these practices intersect. In this study, we investigated the public health risks associated with potential bioaerosol deposition to crops grown in the vicinity of manure application sites. A field sampling campaign at dairy manure application sites supported the emission, transport, and deposition modeling of bioaerosols emitted from these lands following application activities. Results were coupled with a quantitative microbial risk assessment model to estimate the infection risk due to consumption of leafy green vegetable crops grown at various distances downwind from the application area. Inactivation of pathogens ( spp., spp., and O157:H7) on both the manure-amended field and on crops was considered to determine the maximum loading of pathogens to plants with time following application. Overall median one-time infection risks at the time of maximum loading decreased from 1:1300 at 0 m directly downwind from the field to 1:6700 at 100 m and 1:92,000 at 1000 m; peak risks (95th percentiles) were considerably greater (1:18, 1:89, and 1:1200, respectively). Median risk was below 1:10,000 at >160 m downwind. As such, it is recommended that a 160-m setback distance is provided between manure application and nearby leafy green crop production. Additional distance or delay before harvest will provide further protection of public health.

Emission and Dispersion of Bioaerosols from Dairy Manure Application Sites: Human Health Risk Assessment.

In this study, we report the human health risk of gastrointestinal infection associated with inhalation exposure to airborne zoonotic pathogens emitted following application of dairy cattle manure to land. Inverse dispersion modeling with the USEPA's AERMOD dispersion model was used to determine bioaerosol emission rates based on edge-of-field bioaerosol and source material samples analyzed by real-time quantitative polymerase chain reaction (qPCR). Bioaerosol emissions and transport simulated with AERMOD, previously reported viable manure pathogen contents, relevant exposure pathways, and pathogen-specific dose-response relationships were then used to estimate potential downwind risks with a quantitative microbial risk assessment (QMRA) approach. Median 8-h infection risks decreased exponentially with distance from a median of 1:2700 at edge-of-field to 1:13 000 at 100 m and 1:200 000 at 1000 m; peak risks were considerably greater (1:33, 1:170, and 1:2500, respectively). These results indicate that bioaerosols emitted from manure application sites following manure application may present significant public health risks to downwind receptors. Manure management practices should consider improved controls for bioaerosols in order to reduce the risk of disease transmission.

Hierarchal clustering yields insight into multidrug-resistant bacteria isolated from a cattle feedlot wastewater treatment system.

Forty-two percent of Escherichia coli and 58% of Enterococcus spp. isolated from cattle feedlot runoff and associated infiltration basin and constructed wetland treatment system were resistant to at least one antibiotic of clinical importance; a high level of multidrug resistance (22% of E. coli and 37% of Enterococcus spp.) was observed. Hierarchical clustering revealed a closely associated resistance cluster among drug-resistant E. coli isolates that included cephalosporins (ceftiofur, cefoxitin, and ceftriaxone), aminoglycosides (gentamycin, kanamycin, and amikacin), and quinolone nalidixic acid; antibiotics from these classes were used at the study site, and cross-resistance may be associated with transferrable multiple-resistance elements. For Enterococcus spp., co-resistance among vancomycin, linezolid, and daptomycin was common; these antibiotics are reserved for complicated clinical infections and have not been approved for animal use. Vancomycin resistance (n = 49) only occurred when isolates were resistant to linezolid, daptomycin, and all four of the MLSB (macrolide-lincosamide-streptogramin B) antibiotics tested (tylosin, erythromycin, lincomycin, and quinipristin/dalfopristin). This suggests that developing co-resistance to MLSB antibiotics along with cyclic lipopeptides and oxazolidinones may result in resistance to vancomycin as well. Effects of the treatment system on antibiotic resistance were pronounced during periods of no rainfall and low flow (long residence time). Increased hydraulic loading (short residence time) under the influence of rain caused antibiotic-resistant bacteria to be flushed through the treatment system. This presents concern for environmental discharge of multidrug-resistant organisms relevant to public health.