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Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO2-to-Ethylene Electrosynthesis at High Current over One Month

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2024, 146, 39, 27060-27069
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    Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO2-to-Ethylene Electrosynthesis at High Current over One Month
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    • Mingwei Fang
      Mingwei Fang
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
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    • Xiang Miao
      Xiang Miao
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
      More by Xiang Miao
    • Zihao Huang
      Zihao Huang
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
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    • Meiling Wang
      Meiling Wang
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
      More by Meiling Wang
    • Xiaochen Feng
      Xiaochen Feng
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
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    • Zewen Wang
      Zewen Wang
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
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    • Ying Zhu*
      Ying Zhu
      Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
      Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing 100191, China
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-5611-4291
    • Liming Dai*
      Liming Dai
      Australian Carbon Materials Centre (A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW 2052, Australia
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-7536-160X
    • Lei Jiang
      Lei Jiang
      CAS Key Laboratory of Bio-Inspired Materials and Interface Science, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
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      Orcidhttps://orcid.org/0000-0003-4579-728X
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 39, 27060–27069
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c09168
    Published September 19, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Electrosynthesis of multicarbon products, such as C2H4, from CO2 reduction on copper (Cu) catalysts holds promise for achieving carbon neutrality. However, maintaining a steady high current-level C2H4 electrosynthesis still encounters challenges, arising from unstable alkalinity and carbonate precipitation caused by undesired ion migration at the cathode under a repulsive electric field. To address these issues, we propose a universal “charge release” concept by incorporating tiny amounts of an oppositely charged anionic ionomer (e.g., perfluorinated sulfonic acid, PFSA) into a cationic covalent organic framework on the Cu surface (cCOF/PFSA). This strategy effectively releases the hidden positive charge within the cCOF, enhancing surface immobilization of cations to impede both outward migration of generated OH– and inward migration of cations, inhibiting carbonate precipitation and creating a strong alkaline microenvironment. Meanwhile, the ionomer’s hydrophobic chains create a hydrophobic environment within the cCOF, facilitating efficient gas transport. In situ characterizations and theoretical calculations demonstrate that the cCOF/PFSA catalyst establishes a hydrophobic strong alkaline microenvironment, optimizing the adsorption strength and configuration of *CO intermediates to promote the C2H4 formation. The optimized catalyst achieves a 70.5% Faradaic efficiency for C2H4 with a partial current density over 470 mA cm–2. Notably, it delivers a high single-pass carbon efficiency of 96.5% for CO2RR and sustains an exceptional stability over 760 h. When implemented in a large-area MEA electrolyzer and a 5-cell MEA stack, the system achieves an industrial current of 15 A and continuous C2H4 production exceeding 19 mL min–1, marking a significant step toward industrial feasibility in CO2RR-to-C2H4 conversion.

    Copyright © 2024 American Chemical Society

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 39, 27060–27069
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c09168
    Published September 19, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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