State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, SINOPEC Shanghai Research Institute of Petrochemical Technology, Shanghai, 201208, China.
School of Materials Science and Engineering, Shanghai University of Engineering Science, Shanghai, 201620, China.
J Mol Model. 2023 Jan 17;29(2):41. doi: 10.1007/s00894-023-05447-1.
Single-atom catalysts (SACs) in heterogeneous catalysts have attracted increasing attention and the adsorption and nucleation of single atom on the surface are closely related to the performance of the catalyst. The present work employed density functional theory calculations to examine the adsorption of single Au atom and nucleation on γ-AlO surfaces at the atomic level. The effect of surface hydroxyls group on the adsorption and nucleation of single Au atom on γ-AlO surfaces is explored. It was found that the spillover reactions of surface hydroxyls H atoms with the deposited Au are not available on the hydroxylated surface. The interaction of Au to the clean surface is the stronger than to the hydroxylated surface. The even-odd alternations of Au and weak binding of single Au atoms to γ-AlO leads to large even-numbered Au cluster on the surface. Density of states and electron density difference analysis show that the electronic structure of Au/γ-AlO is quite different from the reported Cu and Pd on AlO.
单原子催化剂（SACs）在多相催化剂中引起了越来越多的关注，单原子在表面上的吸附和成核与催化剂的性能密切相关。本工作采用密度泛函理论计算，从原子水平上研究了单原子 Au 在γ-AlO 表面上的吸附和成核。考察了表面羟基对单原子 Au 在γ-AlO 表面上吸附和成核的影响。结果表明，在羟基化表面上，表面 H 原子的溢流反应与沉积 Au 不可用。Au 与清洁表面的相互作用强于与羟基化表面的相互作用。Au 的奇偶交替和单 Au 原子与γ-AlO 的弱结合导致表面上较大的偶数 Au 团簇。态密度和电子密度差分析表明，Au/γ-AlO 的电子结构与报道的 AlO 上的 Cu 和 Pd 明显不同。
