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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Coupling Surface Coverage and Electrostatic Effects on the Interfacial Adlayer-Water Structure of Hydrogenated Single-Crystal Platinum Electrodes
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Coupling Surface Coverage and Electrostatic Effects on the Interfacial Adlayer-Water Structure of Hydrogenated Single-Crystal Platinum Electrodes

机译：耦合表面覆盖和静电单晶铂电极界面侧面水结构的静电效应

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摘要

Atomically flat, single-crystal solid-liquid interfaces attract considerable interest through their electrochemical relevance and well-defined structure facilitating controlled atomistic characterization. Yet, crucial details especially regarding the nanoscale adlayer-water dynamics remain uncertain. Here, the influence of adsorbate coverage on the interfacial structure and solvent relaxation on hydrogenated Pt(111) is examined by extensive density functional molecular dynamics simulations. Pronounced water dynamics is observed with increasing hydrogen coverage, for which an interpretation based on displacement of specifically co-adsorbed water and strong screening of the electrostatic interaction across the interface is proposed. However, the magnitude of the solvent fluctuations is argued to be partly overestimated by the employed RPBE-D3 exchange-correlation functional, which impedes water chemisorption and charge transfer to sparsely hydrogenated platinum. This manifests as overestimated equilibrium electrode potentials compared to experimental adsorption isotherms, which are conversely well reproduced by static calculations invoking the computational hydrogen electrode formalism. By coupling the interfacial structure with electrostatic properties, our work underscores the profound importance of functional choice as well as the persisting value and comparable precision of carefully employed static approximations in electrochemical simulations.
机译：由原子平，单晶的固液界面通过其电化学相关性和促进受控原子表征的明确结构来吸引相当大的兴趣。然而，特别是关于纳米透视adlayer-水动态的重要细节仍然不确定。这里，通过广泛的密度官能分子动力学模拟检查吸附覆盖对氢化Pt（111）上的界面结构和溶剂弛豫的影响。提出了一种随着氢覆盖率的增加观察到明显的水动力学，其中提出了基于专门共吸收水的位移和对整个界面上的静电相互作用的强筛分的解释。然而，溶剂波动的幅度被认为是由所用的RPBE-D3交换 - 相关官能偏估的部分高估，其将水化学吸附和电荷转移阻碍稀疏氢化铂。与实验吸附等温线相比，这种情况表现为高估的平衡电极电位，这反映了通过调用计算氢电极形式主义的静态计算再现。通过将界面结构与静电性能耦合，我们的工作强调了功能选择的深刻重要性以及仔细使用电化学模拟中的静态近似的持续价值和相当的精度。

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