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Accelerated Fe2+ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex

  • Mingyue Liu
    Mingyue Liu
    School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    More by Mingyue Liu
  • Zhiyuan Feng
    Zhiyuan Feng
    School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    More by Zhiyuan Feng
  • Xinmiao Luan
    Xinmiao Luan
    State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    More by Xinmiao Luan
  • Wenhai Chu
    Wenhai Chu
    State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    More by Wenhai Chu
  • Hongying Zhao*
    Hongying Zhao
    School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    *Email: [email protected]. Tel.: +86-(0)21-65988570-8436. Fax: +86-(0)21-65982287
  • , and 
  • Guohua Zhao
    Guohua Zhao
    School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. China
    More by Guohua Zhao
Cite this: Environ. Sci. Technol. 2021, 55, 9, 6042–6051
Publication Date (Web):February 22, 2021
https://doi.org/10.1021/acs.est.0c08018
Copyright © 2021 American Chemical Society
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Abstract

The regeneration rate of Fe2+ from Fe3+ dictates the performance of the electro-Fenton (EF) process, represented by the amount of produced hydroxyl radicals (·OH). Current strategies for the acceleration of Fe2+ regeneration normally require additional chemical reagents, to vary the redox potential of Fe2+/Fe3+. Here, we report an attempt at using the intrinsic property of the electrode to our advantage, i.e., nitrogen-doped carbon aerogel (NDCA), as a reducing agent for the regeneration of Fe2+ without using foreign reagents. Moreover, the pyrrolic N in NDCA provides unpaired electrons through the carbon framework to reduce Fe3+, while the graphitic and pyridinic N coordinate with Fe3+ to form a C–O–Fe–N2 bond, facilitating electron transfer from both the external circuit and pyrrolic N to Fe3+. Our Fe2+/NDCA-EF system exhibits a 5.8 ± 0.3 times higher performance, in terms of the amount of generated ·OH, than a traditional Fenton system using the same Fe2+ concentration. In the subsequent reaction, the Fe2+/NDCA-EF system demonstrates 100.0% removal of dimethyl phthalate, 3-chlorophenol, bisphenol A, and sulfamethoxazole with a low specific energy consumption of 0.17–0.36 kW·h·g–1. Furthermore, 90.1 ± 0.6% removal of dissolved organic carbon and 83.3 ± 0.9% removal of NH3-N are achieved in the treatment of domestic sewage. The purpose of this work is to present a novel strategy for the regeneration of Fe2+ in the EF process and also to elucidate the role of different N species of the carbonaceous electrode in contributing to the redox cycle of Fe2+/Fe3+.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c08018.

  • Experimental details of chemicals, characterization methods, electrochemical procedures, concentration of H2O2, distribution of Fe species, and analytical procedure; the atom ratio of Fe(II) and Fe(III) of the NDCA cathode; the atom ratio of pyrrolic-N, graphitic-N, pyridinic-N, and pyrrolic-N+-O in NDCA, NDCA-C1, and NDCA-C2; physical and chemical properties of NDCA, NDCA-C1, and NDCA-C2; intermediate products in the DMP degradation process determined by GC–MS; toxicity of intermediate products in the DMP degradation process; SEM, TEM, and EDX mapping image of NDCA; DMP removal efficiency in the electrosorption process; H2O2 yield of the NDCA cathode; concentration of total dissolved iron; N 1s XPS spectra of NDCA-C1 and NDCA-CA; Fe2+ regeneration efficiency with different speciations of N atoms; EPR spectra of DMPO-·OH at different times in the Fe2+/NDCA-EF system from 5 to 240 min; the speciation of Fe(II) species; and the degradation pathway of DMP by ·OH (PDF)

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Cited By


This article is cited by 7 publications.

  1. Jinxing Zhang, Zhaoyu Zhou, Zhiyuan Feng, Hongying Zhao, Guohua Zhao. Fast Generation of Hydroxyl Radicals by Rerouting the Electron Transfer Pathway via Constructed Chemical Channels during the Photo-Electro-Reduction of Oxygen. Environmental Science & Technology 2021, Article ASAP.
  2. Jihong Xu, Peisheng Zhou, Penghui Shi, Yulin Min, Qunjie Xu. Insights into the multiple mechanisms of chlorophenols oxidation via activating peroxymonosulfate by 3D N-doped porous carbon. Journal of Environmental Chemical Engineering 2021, 9 (6) , 106545. https://doi.org/10.1016/j.jece.2021.106545
  3. Pei Su, Xuedong Du, Yang Zheng, Wenyang Fu, Qizhan Zhang, Minghua Zhou. Interface-confined multi-layered reaction centers between Ce-MOFs and [email protected] for heterogeneous electro-Fenton at wide pH 3–9: Mediation of Ce3+/Ce4+ and oxygen vacancy. Chemical Engineering Journal 2021, 47 , 133597. https://doi.org/10.1016/j.cej.2021.133597
  4. Xiaomei Liu, Yang Li, Xiaobin Fan, Fengbao Zhang, Guoliang Zhang, Wenchao Peng. Photo-accelerated Co 3+ /Co 2+ transformation on cobalt and phosphorus co-doped g-C 3 N 4 for Fenton-like reaction. Journal of Materials Chemistry A 2021, 9 (39) , 22399-22409. https://doi.org/10.1039/D1TA06026K
  5. Yunhao Tian, Nan Jia, Liang Zhou, Juying Lei, Lingzhi Wang, Jinlong Zhang, Yongdi Liu. Photo-Fenton-like degradation of antibiotics by inverse opal WO3 co-catalytic Fe2+/PMS, Fe2+/H2O2 and Fe2+/PDS processes: A comparative study. Chemosphere 2021, 271 , 132627. https://doi.org/10.1016/j.chemosphere.2021.132627
  6. Xiang Li, Yan Jia, Jiajia Zhang, Yang Qin, Yijia Wu, Minghua Zhou, Jianhui Sun. Efficient removal of tetracycline by H2O2 activated with iron-doped biochar: Performance, mechanism, and degradation pathways. Chinese Chemical Letters 2021, 32 https://doi.org/10.1016/j.cclet.2021.08.054
  7. Zining Wang, Mingyue Liu, Fan Xiao, Georgeta Postole, Hongying Zhao, Guohua Zhao. Recent advances and trends of heterogeneous electro-Fenton process for wastewater treatment-review. Chinese Chemical Letters 2021, 31 https://doi.org/10.1016/j.cclet.2021.07.044