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Origin of Hydrogen Incorporated into Ethylene during Electrochemical CO2 Reduction in Membrane Electrode Assembly

  • Woong Choi
    Woong Choi
    Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
    More by Woong Choi
  • Seongho Park
    Seongho Park
    School of Chemical and Biological Engineering, Seoul National University, Gwanak-ro 1, Gwanak-gu, Seoul 08826, South Korea
    More by Seongho Park
  • Wonsang Jung
    Wonsang Jung
    Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
    Division of Energy and Environmental Technology, KIST School, Korea University of Science and Technology (UST), Seoul 02792, Republic of Korea
    More by Wonsang Jung
  • Da Hye Won
    Da Hye Won
    Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
    Division of Energy and Environmental Technology, KIST School, Korea University of Science and Technology (UST), Seoul 02792, Republic of Korea
    More by Da Hye Won
  • Jonggeol Na*
    Jonggeol Na
    Department of Chemical Engineering and Materials Science, Graduate Program in System Health Science and Engineering, Ewha Womans University, Seoul 03760, Republic of Korea
    *Email: [email protected]
    More by Jonggeol Na
  • , and 
  • Yun Jeong Hwang*
    Yun Jeong Hwang
    Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea
    Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
    *Email: [email protected]
Cite this: ACS Energy Lett. 2022, 7, 3, 939–945
Publication Date (Web):February 10, 2022
https://doi.org/10.1021/acsenergylett.1c02658
Copyright © 2022 American Chemical Society

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    Abstract

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    A catholyte-free membrane electrode assembly (MEA) has been proposed for practical application in the electrochemical CO2 reduction reaction (eCO2RR), and water management becomes critical in its catalyst–membrane interface. We investigate roles of the water supply within the MEA for ethylene production by utilizing deuterium-labeled water. The protons of ethylene originated mainly from the anolyte not the humidified water through the cathode, indicating that dominant water flux from the anolyte acts as a major proton supplier for the eCO2RR. Meanwhile, humidification of CO2 is still important in the Faradaic efficiency and current density because it affects the water activity at the catalyst junction, supported by multiphysics simulations. At low cell potentials, the eCO2RR dominates and is kinetically controlled, and the mass transport of CO2 and water limits its performance as the potential increases. This understanding of the water kinetics and transportation provides valuable insights into the design of active MEAs.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.1c02658.

    • Experimental methods for electrode fabrication, characterization, measurement, and computational calculation, including details for electrode preparation, electrochemical CO2RR performance test, D-labeled CO2RR measurement, and multiphysics simulations (PDF)

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