铜腐蚀产物存在下氯化过程中氧阴离子对氧化剂衰减、溴酸盐和溴代消毒副产物形成的影响。
Effect of oxoanions on oxidant decay, bromate and brominated disinfection by-product formation during chlorination in the presence of copper corrosion products.
机构信息
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China; International Joint Research Center for Sustainable Urban Water System, Tongji University, Shanghai, 200092, China.
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China.
出版信息
Water Res. 2019 Dec 1;166:115087. doi: 10.1016/j.watres.2019.115087. Epub 2019 Sep 13.
The present study investigated the effect of oxoanions on catalytic behaviour of copper corrosion products (CCPs) during chlorination of bromide-containing waters. Three types of oxoanions (carbonate, sulphate, and phosphate) and four types of CCPs (Cu, Cu(OH), CuO, and CuO) were involved in investigation and the effect of oxoanions concentration was also examined. The result indicated that carbonate and sulphate slightly inhibited oxidant decay in the presence of CCPs, but the formation of brominated disinfection by-products (Br-DBPs) remained largely unchanged. In contrast, the presence of phosphate (0.2-1 mM) almost eliminated the catalytic effect of Cu. For CCP solids (i.e. Cu(OH), CuO, and CuO), phosphate preferentially inhibited the formation of bromate rather than Br-DBPs. Despite the catalysis by CCP solids was reduced to some extent, the oxidant decay rate and bromate and Br-DBP formation were still significantly higher than blank groups, even at high phosphate concentration. By testing different addition scheme (simultaneous/sequential addition), it was proposed that phosphate was a strong competitor for hypohalites, rapidly destroying CCPs-hypohalites complexes on some adsorption sites. However, there were some specific sites that can only be adsorbed by hypohalites, leading to the incomplete inhibition of phosphate. Finally, the inhibition effect of phosphate on CCPs catalysis was tested in real water matrix. For Cu, higher reduction of bromate and Br-DBPs was found in raw water rather than filtered water, while converse pattern was true for Cu(OH) and CuO, and this discrepancy can be ascribed to the difference in catalytic mechanism between Cu and CCP solids.
本研究考察了氧阴离子对含溴水中氯化过程中铜腐蚀产物（CCP）催化行为的影响。涉及三种氧阴离子（碳酸盐、硫酸盐和磷酸盐）和四种 CCP（Cu、Cu(OH)、CuO 和 CuO），并考察了氧阴离子浓度的影响。结果表明，在 CCP 存在的情况下，碳酸盐和硫酸盐略微抑制了氧化剂的衰减，但溴代消毒副产物（Br-DBP）的形成基本保持不变。相比之下，磷酸盐（0.2-1 mM）的存在几乎消除了 Cu 的催化作用。对于 CCP 固体（即 Cu(OH)、CuO 和 CuO），磷酸盐优先抑制溴酸盐的形成而不是 Br-DBP。尽管 CCP 固体的催化作用在一定程度上受到抑制，但氧化剂的衰减速率以及溴酸盐和 Br-DBP 的形成仍然明显高于空白组，即使在高磷酸盐浓度下也是如此。通过测试不同的添加方案（同时/顺序添加），提出磷酸盐是次卤酸盐的强竞争者，迅速破坏了一些吸附位点上的 CCP-次卤酸盐复合物。然而，存在一些只能被次卤酸盐吸附的特定位点，导致磷酸盐的抑制不完全。最后，在实际水基质中测试了磷酸盐对 CCP 催化的抑制作用。对于 Cu，在原水中发现溴酸盐和 Br-DBP 的去除率高于过滤水，而对于 Cu(OH)和 CuO 则相反，这种差异可归因于 Cu 和 CCP 固体之间催化机制的差异。
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