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基于活性炭电极体系的消毒副产物的还原脱卤。

Reductive dehalogenation of disinfection byproducts by an activated carbon-based electrode system.

机构信息

Department of Civil and Environmental Engineering, Stanford University, Jerry Yang and Akiko Yamazaki Energy and Environment Building, 473 Via Ortega, Stanford, CA 94305, United States; National Science Foundation Engineering Research Center for Re-Inventing the Nation's Urban Water Infrastructure (ReNUWIt), United States.

Department of Civil and Environmental Engineering, Stanford University, Jerry Yang and Akiko Yamazaki Energy and Environment Building, 473 Via Ortega, Stanford, CA 94305, United States; Adrian Wilcox High School, Santa Clara, CA 95015, United States.

出版信息

Water Res. 2016 Jul 1;98:354-62. doi: 10.1016/j.watres.2016.04.019. Epub 2016 Apr 13.

Abstract

Low molecular weight, uncharged, halogenated disinfection byproducts (DBPs) are poorly removed by the reverse osmosis and advanced oxidation process treatment units often applied for further treatment of municipal wastewater for potable reuse. Granular activated carbon (GAC) treatment effectively sorbed 22 halogenated DBPs. Conversion of the GAC to a cathode within an electrolysis cell resulted in significant degradation of the 22 halogenated DBPs by reductive electrolysis at -1 V vs. Standard Hydrogen Electrode (SHE). The lowest removal efficiency over 6 h electrolysis was for trichloromethane (chloroform; 47%) but removal efficiencies were >90% for 13 of the 22 DBPs. In all cases, DBP degradation was higher than in electrolysis-free controls, and degradation was verified by the production of halides as reduction products. Activated carbons and charcoal were more effective than graphite for electrolysis, with graphite featuring poor sorption for the DBPs. A subset of halogenated DBPs (e.g., haloacetonitriles, chloropicrin) were degraded upon sorption to the GAC, even without electrolysis. Using chloropicrin as a model, experiments indicated that this loss was attributable to the partial reduction of sorbed chloropicrin from reducing equivalents in the GAC. Reducing equivalents depleted by these reactions could be restored when the GAC was treated by reductive electrolysis. GAC treatment of an advanced treatment train effluent for potable reuse effectively reduced the concentrations of chloroform, bromodichloromethane and dichloroacetonitrile measured in the column influent to below the method detection limits. Treatment of the GAC by reductive electrolysis at -1 V vs. SHE over 12 h resulted in significant degradation of the chloroform (63%), bromodichloromethane (96%) and dichloroacetonitrile (99%) accumulated on the GAC. The results suggest that DBPs in advanced treatment train effluents could be captured and degraded continuously by reductive electrolysis using a GAC-based cathode.

摘要

低分子量、不带电荷、卤素化的消毒副产物(DBPs)通过反渗透和高级氧化处理单元的处理去除效果较差,而这些处理单元通常用于进一步处理城市污水以实现饮用水再利用。颗粒活性炭(GAC)处理有效地吸附了 22 种卤代 DBPs。在电解槽内将 GAC 转化为阴极,通过对 -1 V(相对于标准氢电极 (SHE))的还原性电解,导致 22 种卤代 DBPs 发生显著降解。在 6 小时电解过程中,三氯甲烷(氯仿;47%)的去除效率最低,但 22 种 DBPs 中有 13 种的去除效率>90%。在所有情况下,DBP 的降解均高于无电解对照,并且通过还原产物卤化物的生成来验证降解。与石墨相比,活性炭和木炭更适合用于电解,而石墨对 DBPs 的吸附效果较差。一部分卤代 DBPs(例如,卤乙腈、氯仿)在被 GAC 吸附时会发生降解,即使没有电解。以氯仿为例的实验表明,这种损失归因于 GAC 中还原当量对吸附氯仿的部分还原。当 GAC 进行还原性电解处理时,这些反应消耗的还原当量可以得到恢复。用于饮用水再利用的高级处理工艺流出物的 GAC 处理有效地将柱入口处测量的氯仿、二溴二氯甲烷和二氯乙腈的浓度降低到方法检测限以下。用 -1 V(相对于 SHE)对 GAC 进行还原性电解 12 小时,导致 GAC 上积累的氯仿(63%)、二溴二氯甲烷(96%)和二氯乙腈(99%)发生显著降解。结果表明,通过使用基于 GAC 的阴极进行还原性电解,可以连续捕获和降解高级处理工艺流出物中的 DBPs。

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