H and CO Co-Induced Roughening of Cu Surface in CO2 Electroreduction Conditions

化学 亚稳态 化学物理 分子动力学 动力学蒙特卡罗方法 蒙特卡罗方法 计算化学 统计 数学 有机化学
作者
Zisheng Zhang,Winston Gee,Philippe Sautet,Anastassia N. Alexandrova
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (23): 16119-16127 被引量:13
标识
DOI:10.1021/jacs.4c03515
摘要

The dynamic restructuring of Cu has been observed under electrochemical conditions, and it has been hypothesized to underlie the unique reactivity of Cu toward CO2 electroreduction. Roughening is one of the key surface phenomena for Cu activation, whereby numerous atomic vacancies and adatoms form. However, the atomic structure of such surface motifs in the presence of relevant adsorbates has remained elusive. Here, we explore the chemical space of Cu surface restructuring under coverage of CO and H in realistic electroreduction conditions, by combining grand canonical DFT and global optimization techniques, from which we construct a potential-dependent grand canonical ensemble representation. The regime of intermediate and mixed CO and H coverage─where structures exhibit some elevated surface Cu─is thermodynamically unfavorable yet kinetically inevitable. Therefore, we develop a quasi-kinetic Monte Carlo simulation to track the system's evolution during a simulated cathodic scan. We reveal the evolution path of the system across coverage space and identify the accessible metastable structures formed along the way. Chemical bonding analysis is performed on the metastable structures with elevated Cu*CO species to understand their formation mechanism. By molecular dynamics simulations and free energy calculations, the surface chemistry of the Cu*CO species is explored, and we identify plausible mechanisms via which the Cu*CO species may diffuse or dimerize. This work provides rich atomistic insights into the phenomenon of surface roughening and the structure of involved species. It also features generalizable methods to explore the chemical space of restructuring surfaces with mixed adsorbates and their nonequilibrium evolution.
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