电极-电解质界面电子转移的动力学模型：统计力学与电化学方面
A kinetic model of electron transfer at the electrode-electrolyte interface: Statistical mechanics and electrochemical aspects
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中文总结 AI 辅助
本文提出一种基于电子转移与电荷/质量传输无缝结合的动力学模拟方法，自然导出Tafel、Butler-Volmer方程及熵产生等特征，并开发了考虑波动电场影响的改进，以增强电化学界面建模能力。
中文摘要 AI 辅助
一种新的模拟方法（{\it J. Chem. Phys.} {\bf 163}, 164113），基于电极/电解质界面电子转移与电解质溶液中电荷和质量传输的无缝结合，有望推进对电解池和电池等基本电化学器件的综合建模。该模型还包含对非理想电子导电界面处双电层的结构、热力学和统计性质的完全一致处理。因此，诸如Tafel和Butler-Volmer方程、过电位概念以及（稳态）非平衡特征（如熵产生）等微妙方面，自然地从模型中产生，且只需最少的临时假设和对模拟结果的阐述。我们以一个简单的电化学界面模型为例说明这些方面，并讨论旨在增强该方法对电化学感兴趣系统和现象建模能力的进一步改进。其中一项改进，涉及波动电场对电子转移速率的影响，已被明确开发。
英文摘要
A new simulation approach ({\it J. Chem. Phys.} {\bf 163}, 164113), based on the seamless combination of the electron transfer at the electrode/electrolyte interface with the charge and mass transport in electrolyte solutions, holds the promise to advance the comprehensive modeling of basic electrochemical devices such as electrolytic cells and batteries. The underlying model also includes a fully consistent treatment of structural, thermodynamic and statistical properties of the electrical double-layer at non-ideal electron-conducting interfaces. As a result, subtle aspects such as Tafel and Butler-Volmer equations, the overpotential concept, as well as (stationary) non-equilibrium features such as the entropy production, arise naturally from the model, with a minimum of ad-hoc assumptions and elaborations of the simulation results. We illustrate these aspects for a simple model of electrochemical interface, and discuss further improvements of the method meant to enhance its ability to model systems and phenomena of interest for electrochemistry. One such improvement, concerning the effect of fluctuating electric fields on the electron transfer rate, is explicitly developed.
发表机构
- Johannes Gutenberg-Universität Mainz（约翰内斯·古腾堡美因茨大学）
- Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）
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