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在中性初始pH条件下利用铁-乙二胺-N,N'-二琥珀酸络合物对过一硫酸盐进行电化学共催化活化

Utilization of Fe-Ethylenediamine-N,N'-Disuccinic Acid Complex for Electrochemical Co-Catalytic Activation of Peroxymonosulfate under Neutral Initial pH Conditions.

作者信息

Zhang Bolin, Chen Yu, Wang Yongjian, Zhang Igor Ying, Huang Rongfu

机构信息

Sichuan Provincial Key Laboratory of Universities on Environmental Science and Engineering, MOE Key Laboratory of Deep Earth Science and Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China.

Shanghai Key Laboratory of Molecular Catalysis and Innovation Materials, Collaborative Innovation Centre of Chemistry for Energy Materials, MOE Laboratory for Computational Physical Science, Shanghai Key Laboratory of Bioactive Small Molecules, Department of Chemistry, Fudan University, Shanghai 200433, China.

出版信息

Molecules. 2023 Aug 28;28(17):6290. doi: 10.3390/molecules28176290.

Abstract

The ethylenediamine-N,N'-disuccinic acid (EDDS) was utilized to form Fe-EDDS complex to activate peroxymonosulfate (PMS) in the electrochemical (EC) co-catalytic system for effective oxidation of naphthenic acids (NAs) under neutral pH conditions. 1-adamantanecarboxylic acid (ACA) was used as a model compound to represent NAs, which are persistent pollutants that are abundantly present in oil and gas field wastewater. The ACA degradation rate was significantly enhanced in the EC/PMS/Fe(III)-EDDS system (96.6%) compared to that of the EC/PMS/Fe(III) system (65.4%). The addition of EDDS led to the formation of a stable complex of Fe-EDDS under neutral pH conditions, which effectively promoted the redox cycle of Fe(III)-EDDS/Fe(II)-EDDS to activate PMS to generate oxidative species for ACA degradation. The results of quenching and chemical probe experiments, as well as electron paramagnetic resonance (EPR) analysis, identified significant contributions of OH, O, and SO in the removal of ACA. The ACA degradation pathways were revealed based on the results of high resolution mass spectrometry analysis and calculation of the Fukui index. The presence of anions, such as NO, Cl, and HCO, as well as humic acids, induced nonsignificant influence on the ACA degradation, indicating the robustness of the current system for applications in authentic scenarios. Overall results indicated the EC/PMS/Fe(III)-EDDS system is a promising strategy for the practical treatment of NAs in oil and gas field wastewater.

摘要

在电化学(EC)共催化体系中,利用乙二胺 - N,N'-二琥珀酸(EDDS)形成铁 - EDDS络合物来活化过一硫酸盐(PMS),以便在中性pH条件下有效氧化环烷酸(NAs)。1-金刚烷羧酸(ACA)用作代表NAs的模型化合物,NAs是油气田废水中大量存在的持久性污染物。与EC/PMS/Fe(III)体系(65.4%)相比,EC/PMS/Fe(III)-EDDS体系中ACA的降解率显著提高(96.6%)。EDDS的加入导致在中性pH条件下形成稳定的铁 - EDDS络合物,有效促进了Fe(III)-EDDS/Fe(II)-EDDS的氧化还原循环,以活化PMS生成氧化物种用于ACA降解。猝灭和化学探针实验结果以及电子顺磁共振(EPR)分析确定了·OH、·O和SO在ACA去除中的重要贡献。基于高分辨率质谱分析结果和福井指数计算揭示了ACA的降解途径。NO、Cl和HCO等阴离子以及腐殖酸的存在对ACA降解的影响不显著,表明当前体系在实际场景应用中的稳健性。总体结果表明,EC/PMS/Fe(III)-EDDS体系是实际处理油气田废水中NAs的一种有前景的策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4e40/10488724/a933a66b9e0a/molecules-28-06290-g001.jpg

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