Improved atomistic first-principles description of structures and processes at electrochemical electrode/electrolyte interfaces

改进了电化学电极/电解质界面结构和过程的原子第一原理描述

• 批准号: 428022078
• 负责人: Professor Dr. Axel Groß
• 金额: --
• 依托单位: Institut für Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2019
• 资助国家: 德国
• 起止时间: 2018-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/428022078?language=en
• 关键词: Improved; atomistic; first; principles; description

Structures and processes at electrochemical electrode/electrolyte interfaces are not only interesting from a fundamental scientific point of view, they are also technologically relevant in the context of electrochemical energy conversion and storage. Still, the atomisticfirst-principles modelling of these structures and processes is hampered by two factors: first, the presence of liquid electrolytes requires numerically demanding statistical averages; and second, the simulation of electrochemical processes requires to control the electrode potential along a simulation, but current implementations of electronic structure codes typically keep the charge constant, not the electrode potential. In this project, we want to address both issues. We want to run extensive ab initio molecular dynamics simulations including explicit solvent molecules which shall also serve as a benchmark to validate or improve implicit solvent models. And we want to extent a counter-charge scheme we previously implemented and use it as a basis for a constant potential scheme.

电化学电极/电解质界面的结构和过程不仅从基础科学的角度来看是有趣的，它们在电化学能量转换和存储的背景下也是技术相关的。尽管如此，这些结构和过程的原子第一性原理建模受到两个因素的阻碍：第一，液体电解质的存在需要数值上苛刻的统计平均值;第二，电化学过程的模拟需要控制电极电位沿着模拟，但当前电子结构代码的实现通常保持电荷恒定，而不是电极电位。在这个项目中，我们希望解决这两个问题。我们希望运行广泛的从头算分子动力学模拟，包括明确的溶剂分子，这也将作为一个基准，以验证或改进隐式溶剂模型。我们想扩展我们以前实施的反电荷方案，并将其用作恒定电位方案的基础。