纳米团簇Au19Pd和Au19Pt催化解离N2O

doi:10.3866/PKU.WHXB201501191

Abstract

Abstract:

The catalytic decomposition of N₂O using Au₁₉Pd and Au₁₉Pt clusters as catalysts with optimized geometries was studied using density functional theory (DFT). The optimized geometries of the Au₁₉Pd and Au₁₉Pt clusters were obtained as a function of structural and thermodynamic analyses, in which the heteroatoms are on the surfaces of the clusters. We selected the Au₁₉Pd cluster as a model cluster to investigate the reaction mechanism of N₂O decomposition. There are two reaction pathways to be considered: Eley-Rideal (ER) and Langmuir-Hinshelwood (LH). We found that the first N₂O decomposition needs to surmount an energy barrier of 1.118 eV, and is exothermic by 0.371 eV. The elimination of the residual oxygen atom on the surface has an energy barrier of 1.920 eV along the ER pathway after N₂ desorption, which is higher than that along the LH channel (1.669 eV). The adsorption energy of the oxygen atom on the surface is -3.203 eV, and the oxygen atom diffusion on the surface needs to surmount an energy barrier of 0.113 eV along the LH pathway. This indicates that the oxygen atom is prone to transfer on the cluster to promote the generation of the O₂ molecule, and therefore the LH is the optimized reaction pathway. We investigated the catalytic activity of Au₁₉Pt for N₂O decomposition along the LH pathway in comparison with the Au₁₉Pd cluster. Both platinum and palladium have catalytic activities for N₂O decomposition, especially the palladium in this study. Comparison between this work and the theoretical study on periodic systems shows that these two clusters can be used as better catalysts for N₂O decomposition, especially the Au₁₉Pd cluster. Furthermore, the O₂ desorption is no longer the main barrier to the reaction, which further enhances the catalytic activities of these two clusters for N₂O decomposition.

Key words: Nanocluster, Catalytic activity, N₂O decomposition, Reaction mechanism

YU Wei-Ling, ZUO Hui-Wen, LU Chun-Hai, LI Yi, ZHANG Yong-Fan, CHEN Wen-Kai. Nitrous Oxide Decomposition Catalyzed by Au₁₉Pd and Au₁₉Pt Clusters[J]. Acta Phys. -Chim. Sin. 2015, 31(3), 425-434. doi: 10.3866/PKU.WHXB201501191

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Nitrous Oxide Decomposition Catalyzed by Au₁₉Pd and Au₁₉Pt Clusters

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Nitrous Oxide Decomposition Catalyzed by Au₁₉Pd and Au₁₉Pt Clusters