First-principles-based kinetic Monte Carlo simulations of CO oxidation on catalytic Au(110) and Ag(110) surfaces

文献情報

出版日 2021-06-01

DOI 10.1039/D1CP00729G

インパクトファクター 3.676

著者

Jose L. C. Fajín, Ana S. Moura, M. Natália D. S. Cordeiro

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要旨

At the core of the development of more efficient and reliable fuel cells (FCs), there are several essential chemical reactions, namely carbon monoxide (CO) oxidation. This reaction is a keystone in the cleaning of hydrogen fuel used in fuel cells due to strong poisoning by this species of the platinum catalyst used in these devices. The present work aims to provide insight regarding the activation of CO oxidation by gold or silver microfacets possessing low coordinated atoms. To achieve this, density functional theory (DFT) quantum calculations, which determined two competing reaction pathways for CO oxidation, i.e., by molecularly adsorbed oxygen, and by dissociated oxygen, are combined with first-principles kinetic Monte Carlo (1p-kMC) simulations, which employed the resulting DFT parameters in order to address the effect of temperature and partial pressures and the interplay of the elementary reaction events. The use of 1p-kMC is a step further from available works regarding the CO oxidation on gold- and silver-based catalysts for cleansing of hydrogen that is used as a fuel in FCs. Indeed, this research contributes to the conclusion that CO oxidation should preferentially occur on silver microfacets, while the obtained turnover frequencies (TOFs) reinforced such a conclusion.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.