纳米团簇Au19Pd和Au19Pt催化解离N2O

doi:10.3866/PKU.WHXB201501191

摘要/Abstract

摘要：

采用密度泛函理论研究Au-Pd和Au-Pt 纳米团簇催化解离N₂O. 首先根据计算得到Au₁₉Pd和Au₁₉Pt 团簇的最优构型(杂原子均位于团簇的表面). 以Au₁₉Pd催化解离N₂O为例研究催化解离的反应机理. 对此主要考虑两个反应机理, 分别是Eley-Rideal (ER)和Langmuir-Hinshelwood (LH). 第一个机理中N₂O解离的能垒是1.118 eV, 并且放热0.371 eV. N₂分子脱附后, 表面剩余的氧原子沿着ER路径消除需要克服的能垒是1.920eV, 这比反应沿着LH路径的能垒高0.251 eV. 此外根据LH机理, 氧原子在表面的吸附能是-3.203 eV, 而氧原子在表面转移所需的能垒是0.113 eV, 这表明氧原子十分容易在团簇表面转移, 从而促进氧气分子的生成. 因此, LH为最优反应路径. 为了比较Au₁₉Pd和Au₁₉Pt 对N₂O解离的活性, 根据最优的反应路径来研究Au₁₉Pt 催化解离N₂O, 得到作为铂族元素的铂和钯对N₂O的解离有催化活性, 尤其是钯. 同时, 将团簇与文献中的Au-Pd合金相比较, 得到这两种团簇对N₂O 解离有较高的活性, 尤其是Au₁₉Pd团簇. 再者, O₂的脱附不再是影响反应的主要原因, 这可以进一步提高团簇解离N₂O的活性.

关键词: 纳米团簇, 催化活性, N₂O解离, 反应机理

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

MSC2000:

O641

俞炜铃, 左会文, 陆春海, 李奕, 章永凡, 陈文凯. 纳米团簇Au₁₉Pd和Au₁₉Pt催化解离N₂O[J]. 物理化学学报, 2015, 31(3): 425-434.

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.

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纳米团簇Au₁₉Pd和Au₁₉Pt催化解离N₂O

Nitrous Oxide Decomposition Catalyzed by Au₁₉Pd and Au₁₉Pt Clusters

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