催化作用
甲醇
分子动力学
化学
吸附
格式化
液态金属
从头算
化学物理
金属
解吸
计算化学
有机化学
作者
Charlie Ruffman,Krista G. Steenbergen,Anna L. Garden,Nicola Gaston
出处
期刊:Chemical Science
[The Royal Society of Chemistry]
日期:2024-01-01
卷期号:15 (1): 185-194
摘要
Liquid metals have recently emerged as promising catalysts that can outcompete their solid counterparts for many reactions. Although theoretical modelling is extensively used to improve solid-state catalysts, there is currently no way to capture the interactions of adsorbates with a dynamic liquid metal. We propose a new approach based on ab initio molecular dynamics sampling of an adsorbate on a liquid catalyst. Using this approach, we describe time-resolved structures for formate adsorbed on liquid Ga-In, and for all intermediates in the methanol oxidation pathway on Ga-Pt. This yields a range of accessible adsorption energies that take into account the at-temperature motion of the liquid metal. We find that a previously proposed pathway for methanol oxidation on Ga-Pt results in unstable intermediates on a dynamic liquid surface, and propose that H desorption must occur during the path. The results showcase a more accurate way to treat liquid metal catalysts in this emerging field.
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