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

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

doi:10.3390/molecules28176290

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

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

Authors

Bolin Zhang¹, Yu Chen¹, Yongjian Wang¹, Igor Ying Zhang², Rongfu Huang¹

Affiliations

¹ 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.
² 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.

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, ¹O₂, and SO₄^•- 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 NO₃^-, Cl^-, and HCO₃^-, 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.

Keywords: electrochemical catalysis; ethylenediamine-N,N′-disuccinic acid; naphthenic acids; petroleum wastewater.

Grants and funding

This research was funded by National Natural Science Foundation of China with grant number (21973015, 22125301). This work was also supported by the 14th Recruitment Program of Young Professionals of IYZ, the funding of the Innovative research team of high-level local universities in Shanghai, and a key laboratory program of the Education Commission of Shanghai Municipality (ZDSYS14005). The authors would like to acknowledge the Initialization Fund for Talents of Sichuan University (No. YJ202033) and the Special Funds for Scientific and Technological Collaboration of SCU-Zigong (No. 2022CDZG-3). This work was also supported by the State Key Laboratory of Physical Chemistry of Solid Surfaces (No. 202105) in Xiamen University and the Key Laboratory of Spectrochemical Analysis and Instrumentation (Xiamen University), Ministry of Education-SCAI2006.