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<p>The electric double layer (EDL) governs electrocatalysis, energy conversion, and storage, yet its atomic structure, capacitance, and reactivity remain elusive. Here we introduce a machine learning interatomic potential framework that incorporates long-range electrostatics, enabling nanosecond simulations of metal-electrolyte interfaces under applied electric bias with near-quantum-mechanical accuracy. At the benchmark Pt(111)-water and Pt(111)-aqueous KF electrolyte interfaces, we simulate the molecular structure of the EDL, reveal proton-transfer mechanisms underlying anodic water dissociation and the diffusion of ionic water species, and compute differential capacitance. We find that the nominally inert K<sup>+</sup> and F<sup>−</sup> ions, while leaving interfacial water structure largely unchanged, screen bulk fields, slow proton transfer, and generate a prominent capacitance peak near the potential of zero charge. Our simulations quantify how ion-specific interactions, which are ignored in mean-field models, modulate capacitance and reactivity, providing a molecular basis for interpreting experiments and designing electrolytes.</p>

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Ion-modulated structure, proton transfer, and capacitance in the Pt-water electric double layer

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月14日

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  • Xiaoyu Wang,
  • Junmin Chen,
  • Zezhu Zeng,
  • Frederick Stein,
  • Junho Lim,
  • Bingqing Cheng

摘要

The electric double layer (EDL) governs electrocatalysis, energy conversion, and storage, yet its atomic structure, capacitance, and reactivity remain elusive. Here we introduce a machine learning interatomic potential framework that incorporates long-range electrostatics, enabling nanosecond simulations of metal-electrolyte interfaces under applied electric bias with near-quantum-mechanical accuracy. At the benchmark Pt(111)-water and Pt(111)-aqueous KF electrolyte interfaces, we simulate the molecular structure of the EDL, reveal proton-transfer mechanisms underlying anodic water dissociation and the diffusion of ionic water species, and compute differential capacitance. We find that the nominally inert K+ and F− ions, while leaving interfacial water structure largely unchanged, screen bulk fields, slow proton transfer, and generate a prominent capacitance peak near the potential of zero charge. Our simulations quantify how ion-specific interactions, which are ignored in mean-field models, modulate capacitance and reactivity, providing a molecular basis for interpreting experiments and designing electrolytes.