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首页> 外文期刊>Physical review >Potential of zero charge and surface charging relation of metal-solution interphases from a constant-potential jellium-Poisson-Boltzmann model
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Potential of zero charge and surface charging relation of metal-solution interphases from a constant-potential jellium-Poisson-Boltzmann model

机译：恒势Jell-Poisson-Boltzmann模型的金属-溶液相的零电荷电位和表面电荷关系

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摘要

The potential of zero charge (pzc), a fundamental concept in interfacial electrochemistry, is revisited using a jellium-Poisson-Boltzmann model. Under constant-potential description of the metal-solution interphase, this model is able to calculate the surface charging relation (surface free charge density as a function of the electrode potential) and then to determine the pzc therefrom. The potential corresponding to the minimum of differential double-layer capacitance curve is shown to be lower than the pzc determined from surface charging relation, which is caused by free metal electrons entering the solution phase. The model further reveals that the pzc decreases when the vacuum gap between the solution phase and the metal surface, d, becomes narrower. This is consistent with the common observation that the pzc of metal-solution interphase is lower than that calculated from the work function of metal-vacuum interphase (the latter corresponds to d = ∞). Multifaceted roles played by the solvent, including electrostatic screening, polaron effect, and orthogonalizational repulsion, are analyzed. Also discussed are the effects of specific adsorption of ions and potential-dependent d on the surface charging relation.
机译：使用jellium-Poisson-Boltzmann模型重新研究了界面电化学的基本概念零电荷（pzc）的潜力。在金属溶液中间相的恒电位描述下，该模型能够计算表面电荷关系（表面自由电荷密度与电极电位的函数），然后从中确定pzc。对应于最小化双层电容曲线的最小值的电势显示为低于根据表面电荷关系确定的pzc，这是由自由金属电子进入溶液相而引起的。该模型进一步揭示，当固溶相和金属表面之间的真空间隙d变窄时，pzc减小。这与通常的观察结果一致，即金属-溶液界面的pzc低于根据金属-真空界面的功函数计算的pzc（后者对应于d =∞）。分析了溶剂发挥的多方面作用，包括静电筛选，极化子效应和正交排斥。还讨论了离子的特异性吸附和电势依赖性d对表面电荷关系的影响。

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  • 来源
    《Physical review》 |2020年第12期|125422.1-125422.9|共9页
  • 作者

    Jun Huang; Peng Li; Shengli Chen;

  • 作者单位

    Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical Engineering Central South University Changsha 410083 China;

    Hubei Key Laboratory of Electrochemical Power Sources Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education) Department of Chemistry Wuhan University Wuhan 430072 China;

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