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Total organic halogen (TOX) is widely used as a surrogate bulk parameter to measure the overall exposure of halogenated disinfection byproducts (DBPs) in drinking water. In this study, we surprisingly found that the level of TOX in chlorinated waters had been significantly underestimated under common analytical conditions. After the addition of quenching agent sodium thiosulfate, total organic chlorine and total organic bromine exhibited a two-phase decomposition pattern with increasing contact time, and a significant decomposition was observed for different types of quenching agents, quenching doses, and pH conditions. More importantly, the decomposed TOX closely correlated with the acute toxicity of quenched water against luminous bacteria, implying that the DBPs responsible for TOX decomposition could be of important toxicological significance. Based on nontarget analysis by using high-resolution mass spectrometry, molecular formulas for the decomposed TOX were determined. After re-examining the mass balance of TOX in the context of unintentional decomposition, it was found that both the level and percentage of unknown TOX in chlorinated waters were considerably higher than historically thought. Overall, this study brings new insights into the knowledge of TOX formed during chlorination, providing important clues on the identification of toxicity driver in drinking water.

Snow with large specific surface area and strong adsorption capacity can effectively adsorb atmospheric pollutants, which could/might lead to the increase of disinfection by-product (DBP) precursors in surface water. In this study, the contents and characteristics of dissolved organic matter (DOM) in meltwater were investigated, and DBP formation and the DBP-associated cytotoxicity index during chlorination of meltwater was first explored. Overall, meltwater exhibited high nitrogen contents. Meltwater-derived DOM was mainly composed of organics with low molecular weights, low aromaticity, and high unsaturated degrees. DBP formation potentials and cytotoxicity indexes in chlorinated meltwater were positively correlated with air quality index and were significantly impacted by snowfall stages. The trihalomethane and haloacetic acid yields from meltwater were relatively low, while yields of highly cytotoxic DBPs, especially halonitromethanes (6.3-10.8 μg-HNMs/mg-DOC), were significantly higher than those of surface water (1.7 μg-HNMs/mg-DOC). Notably, unsaturated nonaromatic organic nitrates in meltwater were important precursors of halonitromethanes. The actual monitoring results showed that snowfall significant increased the haloacetaldehydes and nitrogenous DBP formation levels of surface water. Considering increased DBP formation and DBP-associated toxicity, it was demonstrated that DOM derived from snowfall in atmosphere-polluted areas could deteriorate surface water quality and pose potential risks to drinking water.

The Yangtze River basin covers one-fifth of China's land area and serves as a water source for one-third of China's population. During long-distance water transport from upstream to downstream, various sources of dissolved organic matter (DOM) lead to considerable variation in DOM properties, significantly impacting water treatability and disinfection byproduct (DBP) formation after chlorination. Using size-exclusion chromatography and fluorescence spectroscopy, the spatial variation in DOM characteristics was comprehensively investigated on a basin scale. The formation of 36 DBPs and speciated total organic halogen in chlorinated samples was determined. Overall, the Yangtze River waters featured a high proportion of terrestrially derived humic substances that served as important precursors for trihalomethanes and haloacetic acids, which was responsible for the increase in total DBP formation along the Yangtze River. The downstream waters were characterized by high levels of microbially derived protein-like biopolymers, which significantly contributed to the formation of haloacetaldehydes and haloacetonitriles that dominated DBP-associated mammalian cell cytotoxicity. Moreover, the precursors of haloacetaldehydes and haloacetonitriles in downstream waters were highly hydrophilic, posing a challenge for water treatment. This study presents an extensive basin-scale study, providing insights into DOM variations along the Yangtze River, illustrating the impact of DOM properties on drinking water from a DBP perspective.