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Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis

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    Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis
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    • Pengtao Xu*
      Pengtao Xu
      Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14850, United States
      *Email: [email protected]
      More by Pengtao Xu
      Orcidhttps://orcid.org/0000-0002-4470-446X
    • Ruiyu Wang
      Ruiyu Wang
      Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States
      Center for Complex Materials from First-Principles (CCM), Temple University, Philadelphia, Pennsylvania 19122, United States
      More by Ruiyu Wang
      Orcidhttps://orcid.org/0000-0003-1608-140X
    • Haojian Zhang
      Haojian Zhang
      Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14850, United States
      More by Haojian Zhang
    • Vincenzo Carnevale
      Vincenzo Carnevale
      Institute for Computational Molecular Science, Temple University, Philadelphia, Pennsylvania 19122, United States
      Department of Biology, Temple University, Philadelphia, Pennsylvania 19122, United States
      More by Vincenzo Carnevale
      Orcidhttps://orcid.org/0000-0002-1918-8280
    • Eric Borguet
      Eric Borguet
      Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States
      Center for Complex Materials from First-Principles (CCM), Temple University, Philadelphia, Pennsylvania 19122, United States
      More by Eric Borguet
      Orcidhttps://orcid.org/0000-0003-0593-952X
    • Jin Suntivich*
      Jin Suntivich
      Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14850, United States
      Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, New York 14850, United States
      *Email: [email protected]
      More by Jin Suntivich
      Orcidhttps://orcid.org/0000-0002-3427-4363
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 4, 2426–2434
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c09128
    Published January 16, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    The molecular details of an electrocatalytic interface play an essential role in the production of sustainable fuels and value-added chemicals. Many electrochemical reactions exhibit strong cation-dependent activities, but how cations affect reaction kinetics is still elusive. We report the effect of cations (K+, Li+, and Ba2+) on the interfacial water structure using second-harmonic generation (SHG) and classical molecular dynamics (MD) simulation. The second- (χH2O(2)) and third-order (χH2O(3)) optical susceptibilities of water on Pt are smaller in the presence of Ba2+ compared to those of K+, suggesting that cations can affect the interfacial water orientation. MD simulation reproduces experimental SHG observations and further shows that the competition between cation hydration and interfacial water alignment governs the net water orientation. The impact of cations on interfacial water supports a cation hydration-mediated mechanism for hydrogen electrocatalysis; i.e., the reaction occurs via water dissociation followed by cation-assisted hydroxide/water exchange on Pt. Our study highlights the role of interfacial water in electrocatalysis and how innocent additives (such as cations) can affect the local electrochemical environment.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c09128.

    • Experimental details including electrode preparation, electrochemical, and SHG measurements. Simulation details. Discussion on the SHG response at Pt–water interfaces. Simulated water and ion distribution near the Pt electrode (PDF)

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    Cited By

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    This article is cited by 14 publications.

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 4, 2426–2434
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c09128
    Published January 16, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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