Peroxymonosulfate-Based Electrochemical Advanced Oxidation: Complication by Oxygen Reduction Reaction.
Peroxymonosulfate-Based Electrochemical Advanced Oxidation: Complication by Oxygen Reduction Reaction.
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DOI：
10.1021/acs.est.3c06156
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发表时间：
2023-11
影响因子：
11.4
通讯作者：
Hyun Jeong Lim;David J. Kim;Kali Rigby;Wensi Chen;Huimin Xu;Xuanhao Wu;Jae-Hong Kim
中科院分区：
文献类型：
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作者：
Hyun Jeong Lim;David J. Kim;Kali Rigby;Wensi Chen;Huimin Xu;Xuanhao Wu;Jae-Hong Kim
基于过硫酸盐（PMS）的电化学高级氧化工艺（EAOPs）近年来受到广泛关注，但PMS活化的确切性质及其对整个工艺性能的影响仍知之甚少。本研究首次证明了氧还原反应在PMS的有效利用和随后的整体污染物修复的增强中所发挥的关键作用。我们观察到的同时生成H2 O2通过氧还原过程中的阴极PMS活化模型氮掺杂的碳纳米管催化剂。H2 O2生成和PMS活化之间的复杂相互作用，以及由于氧还原反应导致的电极附近局部pH值升高，导致SO 4·-/·OH-混合氧化环境，促进污染物降解。这项研究的结果突出了PMS驱动和H2 O2驱动的EAOPs之间的独特依赖性，以及对进一步增强基于PMS的治疗过程的先前未探索的途径的新视角。
Peroxymonosulfate (PMS)-based electrochemical advanced oxidation processes (EAOPs) have received widespread attention in recent years, but the precise nature of PMS activation and its impact on the overall process performance remain poorly understood. This study presents the first demonstration of the critical role played by the oxygen reduction reaction in the effective utilization of PMS and the subsequent enhancement of overall pollutant remediation. We observed the concurrent generation of H2O2 via oxygen reduction during the cathodic PMS activation by a model nitrogen-doped carbon nanotube catalyst. A complex interplay between H2O2 generation and PMS activation, as well as a locally increased pH near the electrode due to the oxygen reduction reaction, resulted in a SO4•-/•OH-mixed oxidation environment that facilitated pollutant degradation. The findings of this study highlight a unique dependency between PMS-driven and H2O2-driven EAOPs and a new perspective on a previously unexplored route for further enhancing PMS-based treatment processes.