水源中的消毒副产物及其前体物——来源、影响因素和环境启示

肖融 ,  邓扬 ,  徐祖信 ,  楚文海

工程（英文） ›› 2024, Vol. 36 ›› Issue (5) : 40 -55.

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工程（英文） ›› 2024, Vol. 36 ›› Issue (5) : 40 -55. DOI: 10.1016/j.eng.2023.08.017
研究论文

水源中的消毒副产物及其前体物——来源、影响因素和环境启示

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Disinfection Byproducts and Their Precursors in Drinking Water Sources: Origins, Influencing Factors, and Environmental Insights

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摘要

对水源中的污染物进行溯源并明晰天然和人为因素的影响有利于维护生态安全和公共健康。然而目前的分析方法通常费力、耗时或在技术上存在瓶颈。消毒副产物（disinfection byproducts, DBPs）是一类在水消毒过程中由化学消毒剂与DBPs前体物反应生成的次生污染物。考虑到DBPs前体物的来源十分广泛，包括天然源、生活源、工业源和农业源等，且特定消毒条件下不同来源前体物生成的DBPs存在特异性，本研究提出DBPs及其前体物可以用作评估水源受污染程度以及判断污染来源的替代指示物。本文首先介绍了水源中DBPs及其前体物的来源以及不同来源前体物在消毒时生成DBPs的特性，随后综述了多种天然和人为因素对DBPs及其前体物的影响情况。在实际操作中，水源水中初始存在的以及后续消毒生成的DBPs的浓度和种类可以一定程度反映水源受污染情况。此外，将DBPs及其前体物与其他水质参数（如溶解性有机碳、溶解性有机氮、荧光光谱和分子量分布情况）以及特定新污染物（如一些药物及个人护理品）联合考虑可以更全面地了解水污染情况，从而更好地管理水资源并确保人类健康。

Abstract

Tracing the contamination origins in water sources and identifying the impacts of natural and human processes are essential for ecological safety and public health. However, current analysis approaches are not ideal, as they tend to be laborious, time-consuming, or technically difficult. Disinfection byproducts (DBPs) are a family of well-known secondary pollutants formed by the reactions of chemical disinfectants with DBP precursors during water disinfection treatment. Since DBP precursors have various origins (e.g., natural, domestic, industrial, and agricultural sources), and since the formation of DBPs from different precursors in the presence of specific disinfectants is distinctive, we argue that DBPs and DBP precursors can serve as alternative indicators to assess the contamination in water sources and identify pollution origins. After providing a retrospective of the origins of DBPs and DBP precursors, as well as the specific formation patterns of DBPs from different precursors, this article presents an overview of the impacts of various natural and anthropogenic factors on DBPs and DBP precursors in drinking water sources. In practice, the DBPs (i.e., their concentration and speciation) originally present in source water and the DBP precursors determined using DBP formation potential tests—in which water samples are dosed with a stoichiometric excess of specific disinfectants in order to maximize DBP formation under certain reaction conditions—can be considered as alternative metrics. When jointly used with other water quality parameters (e.g., dissolved organic carbon, dissolved organic nitrogen, fluorescence, and molecular weight distribution) and specific contaminants of emerging concern (e.g., certain pharmaceuticals and personal care products), DBPs and DBP precursors in drinking water sources can provide a more comprehensive picture of water pollution for better managing water resources and ensuring human health.

关键词

消毒副产物 / 消毒副产物前体物 / 水源水 / 污染指示物 / 天然因素 / 人为因素

Key words

Disinfection byproducts / Disinfection byproduct precursors / Drinking water sources / Contamination indicator / Natural factors / Human factors

引用本文

引用格式 ▾
肖融,邓扬,徐祖信,楚文海. 水源中的消毒副产物及其前体物——来源、影响因素和环境启示[J]. 工程（英文）, 2024, 36(5): 40-55 DOI:10.1016/j.eng.2023.08.017

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1 引言

天然和人工水系统的水污染事件在世界各地多有发生，其中饮用水源受到污染会威胁到生态安全和公共卫生。联合国儿童基金会（United Nations Children’s Fund, UNICEF）和世界卫生组织（World Health Organization, WHO）的报告指出：“尽管全球90%的人口可以获得基本的饮用水源，但水污染普遍存在，至少有20亿人使用的饮用水源存在粪便污染。”[1]为保护水环境以及保障饮用水安全，我们需要识别水源中污染物的潜在来源并评估由此引发的污染风险[2‒3]。按照来源对原水中的有害化学成分进行分类可以将其分为天然存在的化学物质、工业源化学物质、生活源化学物质以及农业活动产生的化学物质[2]。而自然过程（如气候变化和洪水、干旱、山火等自然灾害）和人类活动（如城市化、采矿、生活/农业/工业污废水排放和天然气开采）均会影响水源水甚至饮用水的水质和水量[4‒6]。

目前，用于水污染溯源的方法主要包括污染物排放的清单分析、水文建模、稳定同位素示踪和多变量统计[7]。此外，一些特定的污染物已被用作不同污染源的指示物。例如扑米酮和卡马西平的检出表明水源可能受到污水排放污染[8]，咖啡因的检出可能与粪便和未经处理的废水污染有关，当咖啡因与卡马西平的比值较高时表明地表水中存在大部分未经处理或未经充分处理的污水[9‒10]。三氯蔗糖是一种在水环境中频繁检出的人造甜味剂，其在未受到污水影响的天然水体中不会存在，但在受污水影响的天然水体中被持续检出[11]。因此，有研究者提出可将三氯蔗糖用作污水污染的指示物[11‒12]。

消毒副产物（disinfection byproducts, DBPs）是一类在消毒过程中产生的次生污染物，其是由化学消毒剂与天然有机物（natural organic matter, NOM）、人为污染物和卤化物等前体物反应生成[13‒14]。自20世纪70年代DBPs首次在氯消毒饮用水中被检出以来，DBPs因其具有的潜在健康风险受到了广泛关注[15]。DBPs前体物的来源包括陆地系统、天然水系统、大气系统、污水处理厂（wastewater treatment plants, WWTPs）、工业排放、生活排放、水产养殖和农业活动等[16‒18]。一般来说，水污染与城市、工业或农业的人类活动直接相关，另已有研究发现自然现象会导致地表水质量下降[4,19‒22]。因此，越来越多学者开始关注自然过程和人类活动对饮用水源中DBPs和DBP前体物的影响。例如，台风现象会极大地改变天然水体中溶解性有机物（dissolved organic matter, DOM）的组成成分和浓度水平，其中也包括饮用水源，进而可能影响后续饮用水厂消毒时产生DBPs的浓度和种类[23]。天然气开采时产生的含溴、含碘废水如果未得到适当处置或是出现泄漏时会导致天然水体中卤素离子含量升高，进而促进后续DBPs的生成，尤其是高毒性的溴代和碘代DBPs [24]。此外，由于消毒工艺通常是污水处理的最后一道屏障，污水处理厂出厂水以及处理后农业和工业污废水的排放可能会将已生成的DBPs引入至天然水体[25‒26]。

由于水源是一个极其复杂的基质，对其中所有组分进行定性识别和定量分析的可行性极低，而DBPs和DBPs前体物[通过DBPs生成潜能（formation potential, FP）实验测试得到]可能提供一种新思路。一方面已有大量研究关注不同污染来源的DBPs前体物以及对应的DBPs生成特性，另一方面未受到消毒污水影响的天然水体中理论上应该不会检出DBPs。鉴于此，本研究提出DBPs及其前体物可以用作评估饮用水源受污染状况的替代指标，用于识别污染源以及评估由自然过程或人类活动引起的水源水质变化。

为此，本研究组织如下：首先，综述了饮用水源中DBPs及其前体物的多类来源以及不同来源前体物生成DBPs的特性；其次，总结了自然因素和人为因素对水源水中DBPs前体物以及已有DBPs的影响；再次，讨论了利用DBPs及其前体物作为饮用水源污染指示物的可行性；最后，提出了相关启示和未来研究需求。

2 DBPs、DBPS前体物以及它们的来源

自20世纪70年代中期三卤甲烷（trihalomethanes, THMs）被识别以来，一系列DBPs在消毒后水体中被检测发现（图1 [13,16,18,27‒53]），包括饮用水、再生水、消毒后医院废水、淡化海水、油气开采处理后污水、工农业污废水等[25,37,54‒58]。一般来说，常见的有机DBPs包括含碳DBPs（carbonaceous DBPs, C-DBPs）和含氮DBPs（nitrogenous DBPs, N-DBPs），其中C-DBPs有卤乙醛（haloacetaldehydes, HALs）及标准内的THMs和卤乙酸（haloacetic acids, HAAs）等，而N-DBPs有亚硝胺（nitrosamines. NAs）、卤乙腈（haloacetonitriles, HANs）、卤乙酰胺（haloacetamides, HAMs）和卤代硝基甲烷（halonitromethanes, HNMs）[37]。包括THMs、HAAs、HALs、HANs、HAMs和HNMs在内的这些DBPs具有相似的CX3R结构（其中X代表H原子、Cl原子、Br原子或I原子，R代表官能团），因此被归类为CX3R型DBPs（附录A中图S1）[18,59]。就DBPs前体物而言，如图1所示，由于人类活动对饮用水源的影响日益受到关注，有关水源中DBPs前体物的研究对象逐渐从天然有机物向人为污染物发展。

2.1 水环境中已存在的DBPs及其来源

DBPs被发现具有潜在的健康风险[13]，考虑到人们会直接暴露于饮用水DBPs，有关DBPs的研究大多关注饮用水DBPs。此外，为了防止污水向受纳水体（如地表水、地下水、海水等）排放时引入入侵水生生物和病原微生物，污水排放前通常需要进行消毒处理，进而也会导致DBPs的生成[58,60‒61]。消毒后污水的排放会导致其中含有的DBPs进入水环境，由于DBPs也具有生态风险[62‒64]，这一现象也受到了广泛关注。有趣的是，Grote等[65]根据处理水的体积和相应类型污废水中的DBP浓度评估了各种工业活动对海洋环境中DBPs的影响情况，结果表明冷却水是DBPs的主要人为来源，其次是海水淡化盐水和压载水。表1 [60,65‒68]汇总了消毒后污废水中的DBPs检出情况，其中有部分污废水可能是水源DBPs的主要来源。

2.2 水源中的DBPS前体物及其来源

图2展示了天然水源中DBPs前体物的不同来源，以及无机和有机DBPs前体物与不同消毒剂反应生成DBPs的大致途径。总体看来，多种来源（天然源、生活源、工业源、农业源等）的卤素离子（溴、碘离子）、各种NOM和污水排放有机物（effluent organic matter, EfOM）以及部分人为污染物均可以充当DBPs前体物。常用的消毒方式包括有自由氯、氯胺、二氧化氯、臭氧、紫外消毒以及组合消毒，已有研究对比了不同消毒剂生成DBPs的情况[69‒70]。一般来说，各类消毒剂有其对应生成的DBPs，而不同消毒剂也会生成一些相同的DBPs [13]。游离氯主要生成THMs和HAAs，而氯胺消毒会导致碘代DBPs和NAs的生成。除了亚氯酸盐和氯酸盐外，二氧化氯消毒几乎不会生成其余卤代DBPs。臭氧消毒时通常关注溴酸盐和甲醛的生成。已有很多文章系统综述了有关水源中代表性DBPs前体物的来源、特性和对应DBPs生成情况[16,71‒75]，本文简要概述如下。

2.2.1 溴、碘离子

淡水中溴离子的浓度通常在每升几微克到几毫克级别[74]，据报道，水源中的碘离子浓度在0.5~200 μg·L-1范围内[76]。自然过程（如海水入侵和地质矿物溶解）和人类活动（如海水淡化、采矿、处理后污废水排放以及天然气开采）均会导致水环境中溴、碘离子浓度水平升高[73,77‒78]。就卤素离子对DBPs生成的影响而言，溴离子的存在一方面会促进卤代DBPs整体浓度升高，另一方面溴代DBPs会占主导地位（表2）[12,17,56,71‒72,76,79‒82]，这是因为活性溴物质（HOBr/OBr‒）相较于氯同类物更容易发生取代反应[72,79]。除了卤代DBPs外，溴离子对不同水基质（如模型化合物配水、地表水和污水）中二甲基亚硝胺（N-nitrosodimethylamine, NDMA）的生成展示出不同的影响效果[83]。同样，含碘水的消毒处理或化学氧化会导致碘代DBPs的生成，而生成特性会取决于取决于水体类型和消毒剂种类[73]。天然水体在不同氧化剂处理时碘代DBPs的生成大致遵循：氯胺 > 自由氯 > 臭氧[84]。

2.2.2 NOM

饮用水源中的NOM主要包括外源性NOM和内源性NOM，其中外源性NOM主要由陆生植物降解产生，具有较高的芳香性；而内源性NOM主要是由浮游植物、大型植物和细菌在天然水体中原位生成，芳香性较低但有机氮含量较高[72,75,85]。

如图1所示，在1980—1990年期间，有关水源中DBPs前体物的研究主要集中在陆源NOM（如腐殖酸和富里酸）和微生物源NOM（如氨基酸和蛋白质）。随后，由于人口增长和城市化进程加快，人们对于水的需求急剧增加并开始寻求替代水源，受到城镇污水排放和藻类暴发影响的水体也被纳入考虑[81]。因此，越来越多研究关注EfOM和藻源有机物（algal organic matter, AOM）这两类溶解性有机氮（dissolved organic nitrogen, DON）含量较高的生物源NOM的DBPs生成情况[71,82]。

腐殖质类物质是THMs和HAAs的主要前体物，其在HNMs的生成中也很重要[72]。此外，氨基酸是N-DBPs的关键前体物，包括HANs、HAMs和HNMs [80‒81]，同时，氨基酸在氯化时也会生成醛类物质，其在后续会进一步转化为水合氯醛（chloral hydrate, CH）[44]。AOM是在藻类富营养化过程中渗出或由细胞裂解产生的，其氮含量很高而芳香性极低，因此具有很高的N-DBPs生成潜能[49]。不论是胞外AOM抑或是胞内AOM生成HAAs的产率均高于THMs，而三氯硝基甲烷（trichloronitromethane, TCNM）和二氯乙腈（dichloroacetonitrile, DCAN）是AOM生成的两类最常见N-DBPs [71]。值得说明的是，在氯胺消毒时，AOM是NAs和碘代DBPs的重要前体物[86‒87]。

2.2.3 人为污染物

多种人为污染物，包括药物和个人护理品（pharmaceuticals and personal care products, PPCPs）、工业化学品及其副产物、灭菌剂和杀虫剂等，可通过污水排放或农业径流等方式进入饮用水源，随后在后续消毒工艺中转化为DBPs [12,17,53]。例如，服用药物人群的排泄过程以及随意的药物处置（如直接将药物扔入厕所）会导致市政污水中的药物浓度升高，而其在污水处理厂中去除效果不佳，随即会被就近排入天然水体中。在再生水无计划间接补充饮用水方式（de facto water reuse）中，排放污水中剩余的药物会进入下游饮用水厂的原水[88]。此外，当畜禽粪便中的兽药或饲料添加剂处置不善时，这些物质可通过农业径流进入到水源水中[88]。

大多有关人为污染物生成DBPs的研究集中在NAs和碘代DBPs上，这两类DBPs具有高致癌性或高毒性[12,76]。NAs及其前体物在未受到污水排放影响的天然水体中浓度极低，但排放污水是NAs及其氯胺反应性和臭氧反应性前体物的一个重要来源[86]。有研究表明，除草剂敌草隆[48]、药物雷尼替丁[52]和药物美沙酮[89]会在氯胺消毒时生成NAs；杀菌剂甲苯基氟尼的分解产物二甲基磺酰胺[90]和在混入工业废水的市政污水中检出的1,1,5,5-四甲基甲酰肼[91]被证明在臭氧消毒时会生成NAs。碘代造影剂是一种在医疗机构广泛使用的化学药物，难以被污水处理厂完全去除，相较于氯胺消毒其更易与氯消毒反应生成碘代DBPs，这一生成特性与常见的碘离子和有机物体系明显不同[51,76]。

3 影响水源中DBPs及其前体物的因素

水源水质，尤其是NOM特性，很大程度上会受到自然现象以及人类活动的影响。图3展示了一系列影响水源中DBPs及其前体物的因素。值得关注的是，气候变化对水源水质有长期的影响，相关参数包括基本的物化指标（如温度、pH、浊度和溶解氧）、DOM、营养物质、金属离子、微污染物和生物污染物（如致病菌和蓝藻）等[4,6]。除了全球年平均地表温度不断升高之外，气候变化也与一些天气和气候相关自然灾害（如干旱、洪水、台风和山火）和极端事件（如海水入侵和藻类暴发）发生的频率和强度增加密切相关，这些现象也会影响水源水的水质和水量[92‒95]。然而，需要说明的是，气候变化并不是导致上述自然灾害或极端事件发生的唯一原因。

人类活动对水源的污染主要包括点源污染和面源污染两种，其中污废水排放（如生活污水、工业废水、农业污水和天然气开采废水等）属于点源污染，而大气沉降和农业/城市径流属于面源污染[96‒97]。一般来说，相较于点源污染，面源污染贡献的污染物更多。

3.1 自然因素

3.1.1 干旱

干旱对饮用水水源有多方面影响。第一，干旱季节下蒸发效应增加，水源水量的减少会导致NOM、卤素离子和人为污染物浓度升高，进而促进后续饮用水消毒过程中DBPs的生成[12,92]。第二，当在再生水无计划间接补充饮用水情景下发生干旱时，受纳水体中再生水占比相应增加，其中卤素离子和EfOM [包含溶解性微生物产物（soluble microbial products, SMPs）和人为污染物]对DBPs生成的贡献增加[58,98]。第三，干旱期间水源中营养物质含量的升高可能引发藻类暴发，进而改变有机物的组成并增加AOM这类DBPs前体物的含量水平[93,99]。由此可知，在富营养化湖泊以及经过低降雨或间歇性降雨的水源中，DBPs前体物的主要是内源性NOM [85]。

3.1.2 暴雨和洪水

极端暴雨和洪水可通过城市排水（如合流制管道溢流）、地下水流、地表径流和底部沉积物冲击等过程增加水源水中的沉积物、有机物、浊度和致病微生物含量[100‒102]。值得说明的是，即使是在水位恢复基本水平后，短期极端洪水事件引发的不利影响也可能持续数周。

暴雨和洪水对DOM和DBPs前体物的影响取决于水体特性和降雨模式等[103‒104]。具体来说，降雨过程会导致具有较高DBPs生成潜能的陆源性DOM进入水环境，而越大的雨量会对应更高的DBPs前体物含量[105]。此外，降雨也会改变水源中有机物的反应活性，其中THMs的生成潜能会升高，但HAAs的生成潜能未出现明显变化[106]。与降雨前相比，降雨期间和降雨后溴代THMs和溴代HAAs的占比呈降低趋势[106]。此外，雨水排放也会贡献NA前体物，总NAs的生成潜能可以达到近100 ng∙L-1 [80]。需要说明的是，台风这类短期极端事件主要发生在沿海区域，通常伴随着大范围的降雨和洪水，已有研究表明台风会向水源引入DBPs前体物并显著影响水源水质[23,107]。

3.1.3 海水入侵

海水入侵的发生与气候变化、地下水过度开采、土地利用变化或海平面波动导致的局部海平面上升和（或）沿海地下水位长期下降有关[94]。除了总溶解固体和氯离子水平升高外，海水入侵还会导致溴、碘离子浓度上升，当河口地表水或沿海地下水作为水源水时后续DBPs的生成浓度和种类分布（如THMs、HAAs和溴酸盐）也会随之改变，这一现象在旱季时尤为明显[108‒110]。

珠江是我国第二大河流，由于海水入侵，珠江的溴离子浓度在旱季时期可达到1975.64 μg∙L-1 [110]。此外，有研究报道美国Sacramento-San Joaquin三角洲水源水由于受到旧金山湾盐水入侵出现了明显的溴离子水平升高现象（可达0.8 mg∙L-1），进而促进了后续氯化消毒时总THMs和溴代DBPs的生成，以及臭氧消毒时溴酸盐的生成[111]。需要注意的是，盐水入侵的细微变化也会显著影响后续消毒时总THMs的生成浓度以及THMs中的溴取代情况[108‒109]。据报道，美国华盛顿特区沿海岛屿的地下水供水系统中卤代有机物DBPs的超标频率日益增高，尤其是溴代THMs和HAAs。这可能是与海水入侵引起的溴离子水平升高有关，另外地下水中DOM的组成和含量与地表水存在差异[112]。

3.1.4 山火

近年来，由于气候变化、燃料负荷积累、大面积干旱或森林中人类活动的增加，全球发生山火的次数、规模和严重程度逐渐增加[95]。火灾后的暴雨会增加地表径流并侵蚀烧毁的灰烬和土壤，进而对森林流域构成了巨大威胁。此外，山火后水环境中营养物质的升高通常伴随着藻类暴发的出现，这一方面会增加悬浮沉积物和金属离子的浓度，另一方面也会改变水源中DOM的含量和组成[5,95]。山火可以在短期内摧毁森林生态系统，而对水源水质的影响可以持续几年甚至几十年[113‒114]。

由山火高温以及后续降雨引起的水源水中DOM含量和组成变化也可能影响饮用水消毒时DBPs的生成浓度和种类分布。有研究者采集了山火后降雨水样发现其中DOM在消毒时具有较高的HANs和TCNM生成潜能，然而其生成THMs和HAAs的反应活性与对照水样区别不大[115]。山火过程同样也会产生更多的NDMA前体物[114]。相较于腐殖酸甚至是藻源和微生物源有机物，受到山火影响的陆源有机物生成N-DBPs的活性更高[115‒117]。需要说明的是，山火过后的水环境中HANs前体物含量的升高通常与藻类暴发有关，这是因为山火及后续过程会向水域引入氮元素[113]。此外，也有研究报道山火的发生会导致水源中溴离子浓度升高，进而促进溴代THMs和HAAs的生成[114,116]。

3.1.5 藻类暴发

富营养化和气候变化会促进有害藻华的繁殖和蔓延，从而影响水源水质、水处理效能和饮用水安全[93]。已有大量研究关注藻源NOM的特性以及其生成DBPs的浓度水平和种类分布[71,85]。AOM和藻毒素均可以在消毒过程中充当DBPs前体物[118‒119]。如前文所述，相较于外源性NOM，AOM具有更低的C-DBPs产率[FP，每毫克溶解有机碳（dissolved organic carbon, DOC）对应C-DBPs的微克数，通过对DBPs生成潜能进行DOC浓度归一化获得，用于评估DOM在形成DBPs中的反应性]，而受到藻类影响的水体通常具有更高的N-DBPs生成潜能[120‒121]。有趣的是，尽管在藻类生长阶段水体的DOC水平出现了变化，但C-DBPs的产率并未与随之变化[121‒122]。一项实际研究证实，水源中出现藻类暴发会导致DBPs前体物的水平升高[123]。另外藻类暴发的出现也可能与山火现象有关，这是因为水中营养物质（如无机氮和磷）输入增加[124]。此外，有研究发现山火后的藻类暴发会通过生物化学作用导致陆源DOM的氯反应性和DBP生成潜能升高[125]。

3.1.6 光照

由于气候变化或臭氧消耗导致的太阳紫外辐射增加可以通过温度变化和光解作用改变淡水系统中有机物的特性。这一现象会受到水源中有机物的来源、组成和形态的影响[126‒127]。尽管天然水体中的DOC浓度未在辐照后出现显著变化，但太阳辐照会导致腐殖质类DOC的芳香性降低和亲水性增强[128]。辐照后天然水体中有机物的HAAs产率随之降低，而THMs和HAAs中的溴取代程度呈升高趋势[128]。此外，当在太阳光照射后，新鲜落叶浸出液的HANs产率和CH产率出现了显著的增加[129]。与NOM不同，EfOM中的SMPs更容易被太阳光光解，这一过程产生的活性中间产物具有更高的THMs、CH和TCNM生成潜能[130]。已有学者研究了太阳光照对污水出水中HANs和TCNM前体物的影响效果[131‒132]。此外，太阳照射可以促进颗粒态有机物中DOM的释放。土壤在受到光照后释放的DOM主要是一些具有较高THMs生成潜能的腐殖质类物质，而落叶在光照后释放的DOM主要是具有较高HAAs生成潜能的蛋白质类物质[133‒134]。此外，太阳光光解会抑制美沙酮在氯胺化时NDMA的生成[135]。

3.2 人为因素

3.2.1 大气沉降

大气污染物排放通常可以分为人为排放（如工业烟囱、城市垃圾焚烧、农业活动和汽车尾气）、自然排放（如火山喷发、森林火灾风吹气体及颗粒物、风吹灰尘、土壤颗粒和海浪等）和二次排放[136]。大气中的含碳颗粒物主要来源于生物质和化石燃料的人为燃烧过程[137]。因此，大气沉降通常被归类为人为因素。

大气沉降对地表水质有显著影响[136,138]，其中干沉降（即颗粒和气体沉降）和湿沉降（即下雨、降雪等）均会导致地表水中DBPs前体物含量增加[18,139‒140]。Hou等[18]发现大气颗粒物来源的DOM在雨水氯化消毒时会生成一些CX3R型DBPs，如三氯乙酸（trichloroacetic acid, TCAA）、DCAN、TCNM和二氯乙酰胺等。此外，He等[139]的研究表明干沉降过程会向地表水中引入DOM和DBPs前体物，主要与三氯甲烷（trichloromethane, TCM）、二氯乙酸和三氯乙酸的生成相关。然而，有关大气颗粒物衍生DBPs前体物的文献信息仍然有限，需要进一步研究。

3.2.2 生活污水排放

市政污水通常包括灰水（即淋浴、厨房水槽、浴室洗脸盆和洗衣房的排水）和黑水（即含有粪便和尿液的冲厕水），其被认为是NAs及其前体物的重要来源[57,86,141]。考虑到生活污水通常会通过排水系统收集，随后在污水处理厂进行处理再排放至附近的天然水体[142]，而在再生水无计划间接补充饮用水场景下EfOM会影响下游饮用水厂原水水质，本节主要关注污水厂出水对受纳水体中DBPs及其前体物的影响。

消毒通常是水处理的最后一道工艺，DBPs即是在这一过程中生成。因此，污水厂出水中同时包含有DBPs前体物以及在污水消毒时生成的DBPs [14,143]。一项针对美国污水厂的研究发现，氯化消毒后的污水厂出水中THMs、HAAs、HANs、二氯代HALs和三氯代HALs浓度水平的中位数分别为57.0、70.0、16.0、7.2和16.0 μg∙L-1 [66]。而就地表水而言，Heng等[26]调研了我国北京一条受到再生水补给的城市河流中挥发性卤代DBPs的浓度分布情况。研究结果表明，所有采集的河流水样中均检出了TCM和CH，对应的最高浓度分别达到485.1和30.8 μg∙L-1。

污水源DBPs前体物同样受到了很多关注[50,144]。一般来说，EfOM是由NOM、SMPs以及痕量有毒化学物质（如人为微污染物）组成的复杂介质[82]，其相较于NOM具有更高的DON含量、更低的DOC∶DON值以及更高的N-DBPs生成潜能[145]。值得关注的是，有研究提出一些饮用水源中一些特定的PPCPs和NDMA生成潜能水平可能用作评估排放污水对天然水体影响的指示指标[8]。

3.2.3 农业废水和农业径流

用于作物栽培（如化肥、除草剂和杀虫剂）、畜牧养殖（如兽药、饲料和添加剂）和水产养殖（如肥料、饲料和添加剂）的化学品以及牲畜和水产排泄物中的成分可能存在于农业废水或农业径流中，并进入至饮用水源中[2,25,146]。已有研究测试了除草剂（如敌草隆和溴化嘧啶）和兽用抗生素（如米诺环素）等特定种类前体物的DBPs产率[48,147‒148]，此外，也有研究者关注农业废水或径流中不同DBPs及其前体物的浓度水平，该结果一方面取决于农业活动中使用的饲料、杀虫剂和药剂等，另一方面也与农业废水的处理工艺有关，其中常用工艺通常包括生物处理、化学氧化和消毒。

Eckard等[149]报道，农业灌溉径流的THMs生成潜能高于天然林区和灌丛/草原流域的径流。然而，相较于生活污水和工业废水，农作物栽培径流中NAs及其前体物的浓度水平明显更低[25,86]。具体来说，畜牧养殖径流是NDMA、N-亚硝基吡咯烷（N-nitrosopyrrolidine, NPYR）以及对应前体物质（氯胺消毒和臭氧消毒）的一类来源[86]。事实上，养猪废水中NDMA、N-亚硝基二乙胺（N-nitrosodiethylamine, NDEA）、NPYR、N-亚硝基吗啉（N-nitrosomorpholine, NMOR）和N-亚硝基二丁胺（N-nitrosodibutylamine, NDBA）的浓度可以达到几百甚至上千ng·L-1的水平[25]。值得注意的是，畜牧废水对NAs及其前体物的贡献情况很大程度上取决于处理过程。例如当畜牧废水经过了完全的厌氧消化时，几乎所有的NAs前体物都会被转化为NAs，而在不完全厌氧消化的情况下，处理后水中仍会存在剩余的NAs前体物[150]。

除了农业活动外，水产养殖产生的废水也存在DBPs及其前体物。有研究发现养虾场出水中的DOC和溴离子含量相对较高，THMs生成潜能达到810~3100 μg∙L-1 [146]。Chen等[25]在水产养殖池中检测到NDMA、NDEA和NDBA的存在，其中NDBA占主导地位。渔塘水的NAs浓度和NAs生成潜能相较其他废水（如污水处理厂出水、工业废水和畜牧废水）更低，然而除了鱼塘水以外，几乎没有在废水中检出N-亚硝基甲基乙胺（N-nitrosomethylethylamine, NMEA）[150]。

3.2.4 工业废水排放

工业废水的组成极其复杂。DBPs及其前体物可能存在于各类处理后工业废水中，其含量和组成在很大程度上取决于工业生产的类型。以下一些例子可以说明工业废水排放对水源中DBPs及其前体物的影响。首先，页岩钻井作业的处理废水、燃煤发电工厂的排放废水、油气井的盐水以及一些特定工业设施的排水中溴离子浓度较高，这些污废水的排放会导致天然水体中溴离子含量增高[151‒152]。以下两小节（3.2.5节和3.2.6节）将进一步详细介绍影响水源水中溴离子含量的人为活动及其对DBPs生成的影响。

其次，已有研究报道包括纺织印染废水、电镀废水、金属加工废水、食品加工废水、制浆废水、精细化工废水、机械工业废水、化妆品和个人护理产品制造废水以及制药废水等在内的工业废水中检测出了NAs及其前体物。值得说明的是，金属加工、电子设备和纺织印染废水中含有较高浓度的NDMA [25,57,150]。纺织印染废水的NDMA生成潜能很高，而电镀工业废水中NDEA浓度以及NDEA生成潜能极高[150]。

再次，除了上述含有溴离子以及NAs及其前体物的工业废水外，还有一些工业废水也会成为DBPs和前体物的来源[65,153]。有趣的是，采用碘和碘消毒剂（如碘伏）的奶制品加工厂污废水排放可能向受纳水体贡献碘代DBPs [154]。在奶制品加工厂及后续污水处理厂中碘、含碘化合物以及消毒剂（如自由氯）的使用会致使碘代DBPs的生成，尤其是碘代THMs。此外，钢铁工业中炼铁和加工产生的炼焦废水具有相对较高的DBPs前体物[155]。

3.2.5 燃煤电厂

采用湿法烟气脱硫的燃煤电厂通常会通过向燃煤单元投加含溴盐（如溴化钙）以提高除汞效能[152]。一般来说，投加的溴离子很难被去除，其最终会被排放至受纳水体，导致水源水以及后续饮用水厂原水中溴离子水平升高[156‒157]。尽管地表水中的溴离子并不会对生态系统构成威胁，但当水源水中溴离子浓度增加时消毒过程中总体DBPs以及溴代DBPs的生成水平均会显著增加[158‒159]。有研究报道一座燃煤电厂由于使用湿法烟气脱硫设备导致下游四个水厂原水中溴离子浓度以及出厂水中溴代DBPs浓度升高[152]。

3.2.6 天然气开采

如今，全球越来越多国家开始利用水力压裂法进行天然气开采，该方法扩大了从地质矿床中提取天然气的范围。在这一过程中，部分注入的水最终会以回流水或者产水（与天然气一起开采得到）的形式返回地表，这两类水中通常含有高浓度的总溶解固体、盐类、有毒金属和准金属等[160‒161]。水力压裂产生的污废水可能在原位重新回用于天然气开采，被注入至地下，或是在处理后排放至地表水[151]。然而，钻井地附近发生的污废水地表泄漏和溢出、未经处理污废水的直接处置以及未完全处理无废水的排放均会对地表水水质产生不利影响。

水力压裂产生污废水对下游饮用水厂中DBPs生成的影响主要与饮用水源中溴离子水平的升高有关[151,162]。例如，研究发现水力压裂产生污废水在处理后排放导致美国一条河流中溴离子浓度的急剧增加，数值达到80~1220 μg∙L-1 [152]。Parker等[24]发现，水力压裂产生污废水对DBPs生成浓度和种类分布的影响很大程度上取决于稀释比例和消毒剂的类型。具体看来，当稀释比例低至0.01%~0.1%时，水力压裂产生污废水会促进氯化过程中THMs和HANs的形成，氯胺化过程中NDMA和碘代THMs的产生，以及臭氧化过程中溴酸盐的生成[24]。此外，当水体受到页岩气开采污废水影响时，后续氯化消毒时THMs、二卤代HAAs、三卤代HAAs和二卤代HANs中溴取代程度会随之增加[163]。

有研究发现，经处理的油气废水中高浓度的氨会促进氯消毒时N-DBPs的生成[164]。此外，金属离子（如镁、钙和钡）和硫酸盐也会通过催化作用影响DBPs的生成[165]。值得注意的是，除了DBPs前体物（如溴离子和酚类）外，经处理的油气废水中总THMs和一氯二溴硝基甲烷浓度可以达到μg·L-1级别，其也可能是溴代DBPs的来源之一[56]。

4 讨论

在本节中，我们将讨论利用DBPs和DBPs前体物作为饮用水源中污染指示物的可行性（图4）。一般来说，饮用水源中的DBPs前体物可以通过DBPs生成潜能试验测定，该试验是通过加入过量消毒剂（如氯、氯胺），在一定条件下反应一段时间以最大限度地形成DBPs [166‒167]。图4中已形成的DBPs主要是来源于消毒后的污废水（如污水处理厂出水、农业废水和工业废水），其在排放至附近的天然水体后会导致饮用水源中存在DBPs。

饮用水源中的DBPs前体物（利用生成潜能试验测定）以及本身存在的DBPs可能可以用于对饮用水源中DOM进行溯源，以及评估天然因素和人为活动对水源水质的影响，此外，将其与其他水质参数[如DOC、DON、254 nm处紫外吸光度（UV254）和荧光光谱]和特定的污染指示物（如扑米酮、卡马西平、咖啡因和三氯蔗糖）结合考虑可以提供更多有意义的信息。下面将进行详细讨论。

4.1 DBPs及其前体物的浓度和种类

由于DBPs是水消毒过程中产生的特有次生污染物，当饮用水源中存在较高浓度的DBPs时，水源可能受到了处理后污水排放的影响[14]。有研究报道在受到污水厂出水影响的水源水中频繁检出了一系列高浓度的DBPs（如THMs、HAAs和HALs）[26,66,168]。此外，碘代DBPs的检出可能是因为饮用水源受到含有高浓度碘代DBPs污废水的影响，例如奶制品加工过程产生的废水等[154]。值得注意的是，水源水中高浓度的NAs可能是与污水厂出水或处理后农业/工业废水排放相关，在农业/工业废水的处理过程中会生成一些特定的NAs类DBPs [25,150]。更具体地说，金属加工和电子设施生产、纺织品印花和染色产生的废水中通常含有高浓度的NDMA，而NMEA仅在鱼塘废水中检出[25,150]。

而就DBPs前体物而言，污水厂出水中的EfOM和由藻类大量繁殖产生的AOM是饮用水源中DON的重要来源，在消毒时对于N-DBPs（如HANs、HAMs、HNMs和NAs）的生成有重要贡献（图4）[71, 145]。值得注意的是，除了水体富营养化和气候变化之外，干旱和山火也会引发藻类的大量繁殖。DBPs生成潜能试验中出现的DBPs整体生成量和溴掺入程度升高现象可能是与饮用水源中溴离子浓度的增加有关。同样，水源水中碘离子浓度的升高会促进碘代DBPs的生成，该现象在氯胺消毒时尤为明显。如上所述，水源水中溴离子和碘离子含量的升高可能是由于海水入侵、水产养殖废水排放、燃煤电厂废水排放或天然气开采废水排放等引起的。多类污废水（如农业废水、工业废水和生活污水）中的微污染物，包括PPCPs、工业化学品、灭菌剂和杀虫剂等可以在消毒时充当NAs的前体物[17]。此外，使用游离氯进行DBPs生成潜能实验时，碘代DBPs生成量的升高可能是因为水源水受到了含有高浓度碘代造影剂废水排放的影响[51,169]。HANs生成潜能与THMs生成潜能的比值已被用于评估山火对于水源水的影响程度[115]，这意味着不同种DBPs生成潜能的比值可以用于指示水源污染。

4.2 结合考虑DBPs及其前体物与其它常规水质参数或特定污染指示物

多种分析方法已被用于解析水源中的有机物并评估水厂工艺的处理效能，包括测定综合性参数（如DOC、DON）、光谱方法（如紫外和可见光吸收光谱、荧光）、色谱方法（如高效尺寸排阻色谱）和质谱方法（如液相色谱-质谱法和气相色谱法-质谱法）[170‒171]。本节主要讨论将DBPs及其前体物与其它常规水质参数或特定污染指示物结合的相关研究，以确定饮用水源中的污染来源以及评估由于自然或人为因素引起的水源水质变化。

通过DOC浓度使DBP FP归一化而获得的特定DBP FP（μg DBP/mg DOC）通常被认为可以用于评估有机物与消毒剂的反应性，因此也可为DBPs前体物的来源提供信息[20‒21]。例如，山火后降雨水样在消毒时生成HAN和TCNM的反应性增加，而山火对DOM反应生成THM和HAA活性的影响不显著[5,116]。然而，未来需要进一步建立有关特定DBP FP数值与DOM来源的量化关系，以进一步对水源中的DOM进行溯源。具有高DON含量和低DOC∶DON值的污水在排放后会导致受污水影响的水体中N-DBPs生成潜能升高[145]。近期，利用尺寸排阻色谱和荧光光谱，本研究团队从流域尺度系统研究了DOM特性的空间变化，并测定了水源水在氯化后36种DBPs的生成情况[172]。基于DOM解析和DBPs生成结果，Fang等[172]报道了长江沿线DOM和DBPs生成特性呈现明显变化。此外，有学者提出饮用水DBPs的监测结果可以用于深入了解流域内水文生物地球化学动力学，基于这一观点，Leonard等[173]结合历史饮用水数据（包括DBPs的种类和浓度）、流域采样和针对性光谱表征方法识别一条亚高山源头溪流中DOM的输出点位。

除了上述的常规参数外，特定的污染指示物也可与DBPs及其前体物结合考虑，以提供有关饮用水源污染的更多信息。扑米酮、卡马西平和NDMA FP已被证明是污废水排放的潜在指示指标[8]。基于这一发现，Aydin等[19]通过分析咖啡因、THM FP和NDMA FP水平以对土耳其某水域的污染物进行溯源。在该研究中，咖啡因和THM FP的检出被认为与市政污水的排放有关，而NDMA FP主要与生活污水、工业废水和（或）农业径流有关。通过结合考虑这些指示物，Aydin等[19]确定了该水域的特定污染源。

5 总结和环境启示

饮用水源中的DBPs前体物来源广泛，包括天然源、生活源、工业源和农业源等。这些前体物通常被分为无机卤素离子、NOM和人为污染物。其中溴、碘离子的存在会整体促进DBPs的生成，尤其是溴代DBPs和碘代DBPs。就NOM而言，外源性NOM通常呈现出高芳香含量，其是C-DBPs的主要前体物；而具有低芳香性和高有机氮含量的内源性NOM对N-DBPs的生成贡献较大。有关人为污染物消毒生成DBPs的研究主要关注NAs和碘代DBPs，其中氯胺和臭氧是NAs生成的关键消毒剂，另有研究表明污水厂出水是NAs前体物的主要来源。值得说明的是，碘代DBPs主要是由碘离子、NOM和氯胺反应生成，然而在氯化消毒时碘代造影剂的存在会显著促进碘代DBPs的生成。

表3总结了不同自然过程和人为活动对饮用水源中DOM的影响情况。显然，不同过程引起的水源水质变化大不相同，但也存在一些相似之处。例如，干旱通常会导致水源水中卤素离子、NOM和人为污染物的浓度升高；而在发生暴雨和洪水事件时，雨水径流可能向水源水输送陆源DOM，污水中的污染物也会通过城市点源污染进入天然水体。相比之下，溴离子浓度的升高既可能与自然过程有关，也可能由人为活动引起。

不同来源的DBPs前体物（如天然源、生活源、工业源和农业源）具有不同的DBPs生成特性。此外，由于DBPs是水消毒过程产生的次生污染物，当天然水体未受到污废水排放影响时理论上应该不会检出DBPs，由此推测当饮用水源中存在较高浓度的DBPs时，可能是因为水源受到了处理后污水排放（如污水处理厂出水、农业废水和工业废水）的影响。鉴于此，本研究提出水源水中的DBPs及其前体物可以用作评估水源受污染程度以及判断污染来源的替代指示物。此处从三个方面强调了相关环境启示和未来研究需求。

（1）水源水中的DBPs及其前体物的浓度和种类可以提供有关饮用水源污染程度的信息并用于污染物溯源。当与其他常见水质指标（如DOC、DON、UV254、荧光和分子量分布）或特定污染物（如扑米酮、卡马西平、咖啡因和三氯蔗糖）结合考虑时，DBPs及其前体物可以用于评估自然过程和人为活动对饮用水源水质的影响并进一步提供更多信息。

（2）对饮用水源进行高效的风险管控需要识别有害物质及污染来源，关注对水源水质和水量构成潜在威胁的风险事件。本研究提出DBPs及其前体物可以用作污染指示物，以提高政策制定者、利益相关者和研究人员对饮用水源中主要污染物来源的理解程度。基于此，相关人员可以相应地调整管理策略以尽可能低减少污染影响。

（3）未来研究亟需提供更多定量信息，并创建有关使用DBPs及其前体物作为污染指示物的数据集。举例来说，建立不同DOM来源以及特定DBP FP或DBP FP比值（如HAN FP∶THM FP）之间的定量关系可能可以用于对饮用水源中的DOM进行溯源。此外，在未来研究中也需要关注如何更好地将DBPs及其前体物与传统水质参数结合使用这一问题。

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