Formation of brominated disinfection byproducts from natural organic matter isolates and model compounds in a sulfate radical-based oxidation process.

Formation of brominated disinfection byproducts from natural organic matter isolates and model compounds in a sulfate radical-based oxidation process.
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DOI:
10.1021/es503255j
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发表时间:
2014-12
影响因子:
11.4
通讯作者:
Yuru Wang;Julien Le Roux;Tao Zhang;J. Croué
Yuru Wang;Julien Le Roux;Tao Zhang;J. Croué
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Yuru Wang;Julien Le Roux;Tao Zhang;J. Croué

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基于硫酸根的高级氧化工艺(SR-AOP)在水/废水污染物去除中的应用越来越受到关注。然而,对其副作用的了解有限。研究了水中溴离子和有机物对总有机溴(TOBr)和溴化消毒副产物(Br-DBPs)产生的副作用。过一硫酸根的非均相催化活化生成硫酸根自由基。分离的天然有机物(NOM)组分以及低分子量(LMW)化合物被用作模型有机物。SR-AOP产生了大量的TOBr,其中溴仿(TBM)和二溴乙酸(DBAA)被确定为主要的Br-DBPs。一般来说,SR-AOP有利于DBAA的形成,这与用HOBr/OBr(-)溴化(更多的TBM产生)是完全不同的。SR-AOP实验结果表明,溴掺入分布在疏水性和亲水性NOM馏分。模型前体的研究表明,低分子量酸是反应性的TBM前体(柠檬酸>琥珀酸>丁二酸>马来酸)。柠檬酸、天冬氨酸和天冬酰胺可形成较高的DBAA;天冬氨酸和天冬酰胺分别是二溴乙腈和二溴乙酰胺的主要前体。
A sulfate radical-based advanced oxidation process (SR-AOP) has received increasing application interest for the removal of water/wastewater contaminants. However, limited knowledge is available on its side effects. This study investigated the side effects in terms of the production of total organic bromine (TOBr) and brominated disinfection byproducts (Br-DBPs) in the presence of bromide ion and organic matter in water. Sulfate radical was generated by heterogeneous catalytic activation of peroxymonosulfate. Isolated natural organic matter (NOM) fractions as well as low molecular weight (LMW) compounds were used as model organic matter. Considerable amounts of TOBr were produced by SR-AOP, where bromoform (TBM) and dibromoacetic acid (DBAA) were identified as dominant Br-DBPs. In general, SR-AOP favored the formation of DBAA, which is quite distinct from bromination with HOBr/OBr(-) (more TBM production). SR-AOP experimental results indicate that bromine incorporation is distributed among both hydrophobic and hydrophilic NOM fractions. Studies on model precursors reveal that LMW acids are reactive TBM precursors (citric acid > succinic acid > pyruvic acid > maleic acid). High DBAA formation from citric acid, aspartic acid, and asparagine was observed; meanwhile aspartic acid and asparagine were the major precursors of dibromoacetonitrile and dibromoacetamide, respectively.