Liu Chao, Liu Hang, Hu Chengzhi, Chow Alex T, Karanfil Tanju
Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
Department of Environmental Engineering and Earth Sciences, Clemson University, Anderson, South Carolina 29625, United States.
ACS ES T Water. 2024 Nov 25;4(12):5890-5901. doi: 10.1021/acsestwater.4c00855. eCollection 2024 Dec 13.
Seasonal algal blooms in surface waters can adversely impact drinking water quality. Oxidative treatment has been demonstrated as an effective measure for the removal of algal cells. However, this, in turn, leads to the release of algal organic matter (AOM). Effects of oxidative treatment using chlorine, bromine, chloramine, ozone, and permanganate on the molecular alterations of the AOM were studied using Fourier transform ion cyclotron resonance mass spectrometry. Increased chemodiversity, decreased aromaticity, and elevated average oxidation state of carbon () were observed after oxidation. Of the oxidants, ozone caused the most pronounced changes. There was a positive correlation between the increases in and reduction potentials of oxidants (i.e., ozone > chlorine ≈ bromine > permanganate > chloramine). Oxygen transfer and oxidative dehydrogenation were major pathways (42.3-52.8%) for AOM oxidation, while other pathways (e.g., deamination, dealkylation, decarboxylation, and halogen substitution/addition) existed. Moreover, the halogen substitution/addition pathway only accounted for 1.3-10.3%, even for chlorine or bromine treatment. Oxidative treatment could decrease the reactivity of AOM in postchlorination, thereby decreasing the trichloromethane formation. However, the formation of oxygen-rich disinfection byproducts (DBPs, e.g., trichloronitromethane) could be favored, especially for ozonation. This study provides molecular-level insights into the effects of oxidative treatment on AOM and derived DBP formation in water treatment.
地表水中的季节性藻华会对饮用水质量产生不利影响。氧化处理已被证明是去除藻类细胞的有效措施。然而,这反过来又会导致藻类有机物(AOM)的释放。使用傅里叶变换离子回旋共振质谱法研究了氯、溴、氯胺、臭氧和高锰酸盐氧化处理对AOM分子变化的影响。氧化后观察到化学多样性增加、芳香性降低以及碳的平均氧化态升高。在这些氧化剂中,臭氧引起的变化最为显著。氧化剂的增加与还原电位之间存在正相关(即臭氧>氯≈溴>高锰酸盐>氯胺)。氧转移和氧化脱氢是AOM氧化的主要途径(42.3 - 52.8%),同时还存在其他途径(如脱氨、脱烷基、脱羧和卤素取代/加成)。此外,即使是氯或溴处理,卤素取代/加成途径也仅占1.3 - 10.3%。氧化处理可以降低AOM在后续氯化过程中的反应性,从而减少三氯甲烷的形成。然而,富含氧的消毒副产物(DBPs,如三氯硝基甲烷)的形成可能会增加,尤其是对于臭氧化处理。本研究提供了氧化处理对水处理中AOM和衍生DBP形成影响的分子水平见解。