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电化学激活过硫酸盐过程在分槽和不分槽体系中不同阴极上的自由基和非自由基氧化机理。

The radical and non-radical oxidation mechanism of electrochemically activated persulfate process on different cathodes in divided and undivided cell.

机构信息

Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Urban Ecology Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.

Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, Nankai University, Tianjin 300350, China; Tianjin Key Laboratory of Urban Ecology Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.

出版信息

J Hazard Mater. 2021 Aug 15;416:125804. doi: 10.1016/j.jhazmat.2021.125804. Epub 2021 Apr 6.

DOI:10.1016/j.jhazmat.2021.125804
PMID:33865104
Abstract

Electrochemically activated persulfate (PS) employing stainless steel (SS), carbon felt (CF) and carbon black modified CF (CB-CF) as the cathode, in the divided and undivided cell, respectively, for degradation of atrazine (ATZ) was first investigated using novel B, Co-doped TiO nanotubes (B, Co-TNT) anode. In undivided cell, ATZ degradation was followed the order of CF<CB-CF<SS. The main radical for ATZ removal in SS and CF system was OH, while on CB-CF cathode, it was the comprehensive contribution of OH and SO. OH in SS system was more inclined to free OH, while in CF and CB-CF systems it was more likely to be surface OH. In divided anode cell, OH was responsible for ATZ degradation in all three cathodes system. However, in divided cathode cell, OH played a major role for ATZ degradation in SS cathode system. In CF and CB-CF cathode systems, the ATZ degradation was the comprehensive effect of OH and SO with the contribution of OH and SO was 91.7%, 8.3%, and 96.3%, 3.6%, respectively. The quenching studies showed that non-radical oxidation occurred in anode chamber in the presence of PS. Besides, the intermediates in divided and undivided cell were detected by LC-MS, and the possible degradation pathway was proposed.

摘要

电化学激活过硫酸盐(PS)采用不锈钢(SS)、碳纤维毡(CF)和炭黑改性碳纤维毡(CB-CF)分别作为阴极,在分隔和不分隔的电池中,首次使用新型 B、Co 掺杂 TiO 纳米管(B、Co-TNT)阳极研究了莠去津(ATZ)的降解。在不分隔电池中,ATZ 的降解顺序为 CF<CB-CF<SS。在 SS 和 CF 体系中,ATZ 去除的主要自由基是 OH,而在 CB-CF 阴极上,是 OH 和 SO 的综合贡献。SS 体系中的 OH 更倾向于游离 OH,而在 CF 和 CB-CF 体系中更倾向于表面 OH。在分隔阳极电池中,OH 是三种阴极体系中 ATZ 降解的主要原因。然而,在分隔阴极电池中,OH 在 SS 阴极体系中对 ATZ 降解起主要作用。在 CF 和 CB-CF 阴极体系中,ATZ 的降解是 OH 和 SO 的综合作用,OH 和 SO 的贡献分别为 91.7%、8.3%和 96.3%、3.6%。猝灭研究表明,在 PS 的存在下,阳极室中发生了非自由基氧化。此外,通过 LC-MS 检测到了分隔和不分隔电池中的中间产物,并提出了可能的降解途径。

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