Disinfection Byproducts in Rajasthan, India: Are Trihalomethanes a Sufficient Indicator of Disinfection Byproduct Exposure in Low-Income Countries?

The implementation of chlorine disinfection in low-income countries reduces the risk of waterborne illness but initiates exposure to disinfection byproducts (DBPs). Like high-income countries, low-income countries typically are adopting regulations focusing on trihalomethanes (THM4) as an indicator of overall DBP exposure. However, the use of impaired water sources can decouple the formation of THM4 from other DBP classes that are more potent toxins. The documentation of DBP species other than THM4 is rare in low-income countries, where water sources may be degraded by inadequate sanitation infrastructure and other uncontrolled wastewater discharges. We measured THM4 and 21 unregulated DBPs in tap waters and laboratory-treated source waters from two cities in northwestern India. The contribution of each DBP class to the cumulative toxicity was estimated by weighting each species by metrics of toxic potency; haloacetonitriles typically were the dominant contributor, while the contribution of THM4 was negligible. THM4 concentrations did not correlate with the total toxic potency-weighted DBP concentrations. Although THM4 rarely exceeded international guidelines, DBPs of greater toxicological concern were observed in high concentrations. The total toxic potency-weighted DBP concentrations in some waters were elevated compared to conventional drinking waters in high-income countries and more closely resembled chlorine-disinfected wastewater effluents. Artificial sweeteners confirmed widespread contamination of both surface and groundwaters by domestic sewage. The results suggest that THM4 may not be an adequate indicator of overall DBP exposure in impaired water supplies prevalent in some low-income nations.

It's getting hot in here: Effects of heat on temperature, disinfection, and opportunistic pathogens in drinking water distribution systems.

As global temperatures rise with climate change, the negative effects of heat on drinking water distribution systems (DWDS) are of increasing concern. High DWDS temperatures are associated with degradation of water quality through physical, chemical and microbial mechanisms. Perhaps the most pressing concern is proliferation of thermotolerant opportunistic pathogens (OPs) like Legionella pneumophila and Naegleria Fowleri. Many OPs can be controlled in DWDS by residual disinfectants such as chlorine or chloramine, but maintaining protective residuals can be challenging at high temperatures. This critical review evaluates the literature on DWDS temperature, residual disinfectant decay, and OP survival and growth with respect to high temperatures. The findings are synthesized to determine the state of knowledge and future research priorities regarding OP proliferation and control at high DWDS temperatures. Temperatures above 40 °C were reported from multiple DWDS, with a maximum of 52 °C. Substantial diurnal temperature swings from ∼30-50 °C occurred in one DWDS. Many OPs can survive or even replicate at these temperatures. However, most studies focused on just a few OP species, and substantial knowledge gaps remain regarding persistence, infectivity, and shifts in microbial community structure at high temperatures relative to lower water temperatures. Chlorine decay rates substantially increase with temperature in some waters but not in others, for reasons that are not well understood. Decay rates within real DWDS are difficult to accurately characterize, presenting practical limitations for application of temperature-dependent decay models at full scale. Chloramine decay is slower than chlorine except in the presence of nitrifiers, which are especially known to grow in DWDS in warmer seasons and climates, though the high temperature range for nitrification is unknown. Lack of knowledge about DWDS nitrifier communities may hinder development of solutions. Fundamental knowledge gaps remain which prevent understanding even the occurrence of high temperatures in DWDS, much less the overall effect on exposure risk. Potential solutions to minimize DWDS temperatures or mitigate the impacts of heat were identified, many which could be aided by proven models for predicting DWDS temperature. Industry leadership and collaboration is needed to generate practical knowledge for protecting DWDS water quality as temperatures rise.

Passive biomonitoring for per- and polyfluoroalkyl substances using invasive clams, C. fluminea.

Per- and polyfluoroalkyl substances (PFAS) are a class of toxic manufactured chemicals in commercial and consumer products. They are resistant to environmental degradation and mobile in soil, air, and water. This study used the introduced bivalve Corbicula fluminea as a passive biomonitor at sampling locations in a primary drinking water source in Virginia, USA. Many potential PFAS sources were identified in the region. Perfluorohexane sulfonate (PFHxS) and 6:2 fluorotelomer sulfonic acid (6:2 FTS) levels were highest downstream of an airport. The highest levels of short-chain carboxylic acids were in locations downstream of a wastewater treatment plant. Measured PFAS concentrations varied by location in C. fluminea, sediment, and surface water samples. Two compounds were detected across all three mediums. Calculated partitioning coefficients confirm bioaccumulation of PFAS in C. fluminea and sorption to sediment. C. fluminea bioaccumulated two PFAS not found in the other mediums. Perfluoroalkyl carboxylic acids and short-chain compounds dominated in clam tissue, which contrasts with findings of accumulation of longer-chain and perfluorosulfonic acids in fish. These findings suggest the potential for using bivalves to complement other organisms to better understand the bioaccumulation of PFAS and their fate and transport in a freshwater ecosystem.

Use of trihalomethanes as a surrogate for haloacetonitrile exposure introduces misclassification bias.

Epidemiologists have used trihalomethanes (THMs) as a surrogate for overall disinfection byproduct (DBP) exposure based on the assumption that THM concentrations are proportional to concentrations of other DBP classes. Toxicological evidence indicates THMs are less potent toxins than unregulated classes like haloacetonitriles (HANs). If THMs are not proportional to the DBPs driving toxicity, the use of THMs to measure exposure may introduce non-trivial exposure misclassification bias in epidemiologic studies. This study developed statistical models to evaluate the covariance and proportionality of HAN and THM concentrations in a dataset featuring over 9500 measurements from 248 public water systems. THMs only explain ∼30% of the variance in HANs, whether the data is pooled in a classic linear regression or hierarchically grouped by water system in a multilevel linear regression. The 95% prediction interval on HANs for the median THM concentration exceeds the interquartile range of HANs. Mean HAN:THM ratios range from ∼2.4% to ∼80% across water systems, and varied with source water category, season, disinfectant sequence and distribution system location. The HAN:THM ratio was 265% higher in groundwater systems than in surface water systems and declined by ∼40% between finished effluent and maximum residence times in surface water systems with chlorine-chlorine disinfection. A maximum likelihood approach was used to estimate the misclassification bias that may result from using THMs to construct risk-ratios, assuming that HANs represent the "true" DBP exposure risk. The results indicate an odds ratio of ∼2 estimated with THM concentrations could correspond to a true odds ratio of 4-5. These findings demonstrate the need for epidemiologic studies to evaluate exposure by measuring DBPs that are likely to drive toxicity.

Chlorine taste can increase simulated exposure to both fecal contamination and disinfection byproducts in water supplies.

Expanding drinking water chlorination could substantially reduce the burden of disease in low- and middle-income countries, but the taste of chlorinated water often impedes adoption. We developed a Monte Carlo simulation to estimate the effect of people's choice to accept or reject drinking water based on chlorine taste and their subsequent exposure to E. coli and trihalomethanes, a class of disinfection byproduct (DBP). The simulation used empirical data from Dhaka, Bangladesh, a megacity with endemic waterborne disease. We drew on published taste acceptability thresholds from Dhaka residents, measured residual chlorine and thermotolerant E. coli inactivation following the addition of six chlorine doses (0.25-3.0 mg/L as Cl2) to untreated piped water samples from 100 locations, and analyzed trihalomethane formation in 54 samples. A dose of 0.5 mg/L, 75% lower than the 2 mg/L dose typically recommended for household chlorination of low-turbidity waters, minimized overall exposure to E. coli. Doses of 1-2 mg/L maximized overall exposure to trihalomethanes. Accounting for chlorine taste aversion indicates that microbiological exposure increases and DBP exposure decreases above certain doses as a higher proportion of people reject chlorinated water in favor of untreated water. Taken together with findings from other modeling analyses, empirical studies, and field trials, our results suggest that taste acceptability should be a critical consideration in establishing chlorination dosing guidelines. Particularly when chlorination is first implemented in water supplies with low chlorine demand, lower doses than those generally recommended for household water treatment can help avoid taste-related objections while still meaningfully reducing contaminant exposure.

Co-occurrence of geogenic and anthropogenic contaminants in groundwater from Rajasthan, India.

Northwest India suffers from severe water scarcity issues due to a combination of over-exploitation and climate effects. Along with concerns over water availability, endemic water quality issues are critical and affect the usability of available water and potential human health risks. Here we present data from 243 groundwater wells, representing nine aquifer lithologies in 4 climate regions that were collected from the Northwestern Indian state of Rajasthan. Rajasthan is India's largest state by area, and has a significant groundwater reliant population due to a general lack of surface water accessibility. We show that the groundwater, including water that is used for drinking without any treatment, contains multiple inorganic contaminants in levels that exceed both Indian and World Health Organization (WHO) drinking water guidelines. The most egregious of these violations were for fluoride, nitrate, and uranium; 76% of all water samples in this study had contaminants levels that exceed the WHO guidelines for at least one of these species. In addition, we show that much of the groundwater contains high concentrations of dissolved organic carbon (DOC) and halides, both of which are risk factors for the formation of disinfectant byproducts in waters that are treated with chemical disinfectants such as chlorine. By using geochemical and isotopic (oxygen, hydrogen, carbon, strontium, and boron isotopes) data, we show that the water quality issues derive from both geogenic (evapotranspiration, water-rock interactions) and anthropogenic (agriculture, domestic sewage) sources, though in some cases anthropogenic activities, such as infiltration of organic- and nitrate-rich water, may contribute to the persistence and enhanced mobilization of geogenic contaminants. The processes affecting Rajasthan's groundwater quality are common in many other worldwide arid areas, and the lessons learned from evaluation of the mechanisms that affect the groundwater quality are universal and should be applied for other parts of the world.

Tradeoffs between pathogen inactivation and disinfection byproduct formation during sequential chlorine and chloramine disinfection for wastewater reuse.

Treatment of fully nitrified municipal wastewater effluents with chlorine followed by chloramines (i.e., sequential chlorine disinfection) upstream of advanced treatment trains can contribute pathogen inactivation credits for potable reuse while leaving a chloramine residual to control biofouling on membrane units in the advanced treatment train. However, free chlorine exposures must be optimized to maximize pathogen inactivation while minimizing the formation of disinfection byproducts (DBPs) that are challenging to remove in the advanced treatment train. Using a pilot-scale disinfection contactor receiving fully-nitrified, tertiary municipal wastewater effluent, this study found that a 3 mg × min/L free chlorine CT (i.e., the product of the chlorine residual "C" and the contact time "T") followed by a 140 mg × min/L chloramine CT could reliably achieve 5-log inactivation of MS2 bacteriophage and reduce median total coliform concentrations below 2.2 MPN/100 mL. Free chlorine disinfection was equally effective when chlorine was dosed to exceed the breakpoint for 1 mg/L of ammonia as N. At this free chlorine exposure, regulated trihalomethane (THM) and haloacetic acid (HAA) formation remained below their Maximum Contaminant Levels (MCLs), but NDMA concentrations of ∼30 ng/L were above the 10 ng/L California Notification Level. Increasing the free chlorine exposure to ∼30 mg × min/L increased THM and HAA formation, with regulated THMs approaching or exceeding the MCL. Although this free chlorine exposure prevented NDMA formation during chloramination, the ∼10 ng/L background NDMA formation in the tertiary effluent remained. Increasing the free chlorine exposure also increased the formation of unregulated halogenated DBP classes that may be significant contributors to the DBP-associated toxicity of the disinfected wastewater. The results indicate that sequential chlorination can be used to optimize the benefits of free chlorine (virus and NDMA control) and chloramine disinfection (THM, HAA, and coliform control).