Genetic algorithm aided density functional theory simulations unravel the kinetic nature of Au(100) in catalytic CO oxidation

• Published in: Chinese chemical letters Vol. 30; no. 6; pp. 1346 - 1350
• Main Authors: Fang, Yi, Gong, Xueqing
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.06.2019; Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry&Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China
• Subjects: Density functional theory; Genetic algorithm; Gold catalysts; Potential energy surface; Surface reconstruction; Potential energy surface; Surface reconstruction; Density functional theory; Genetic algorithm; Gold catalysts
• ISSN: 1001-8417; 1878-5964
• DOI: 10.1016/j.cclet.2018.12.025

The interactions of oxygen atoms and Au(100) can affect the surface morphology by inducing the hexagonal type reconstruction to the surface layer and forming a lifted O-Au-O species. [Display omitted] Heterogeneous catalysis is of tremendous importance to modern industries. Exposed atoms of heterogeneous catalysts are heavily involved in surface processes such as the adsorption, activation, diffusion and reaction of substrate molecules. Surfaces of metal or metal oxide based catalysts are usually taken as hard templates that only undergo limited relaxation during catalytic reactions, especially in theoretical simulations. In this work, by using genetic algorithm (GA) aided density functional theory (DFT) calculations, we studied the surface processes involved in CO oxidation on the Au(100) surface. The use of GA greatly improves the capacity of DFT calculations in locating the potential energy surface (PES) of the surface reactions, and surprisingly, it has been found that the Au(100) surface can undergo drastic reconstruction under the influence of O adsorption and the adapted partially oxidized Au surface exhibits unique activities for subsequent adsorptions and reactions. This work depicts the kinetic nature of the Au(100) surface in its catalyzed reactions and also significantly expands our understanding of how surface atoms act in heterogeneous catalysis.