PdAu纳米团簇上一氧化碳反应的第一性原理研究
First-principles studies of CO oxidation on PdAu nanocluster
利用第一性原理方法， 本文研究了金团簇上Pd原子催化一氧化碳氧化的反应活性。计算发现：对CO+O2--CO2+Of反应，Pd monomer，dimer和trimer具有高的反应活性，其反应机制为association mechanism。反应过程中，只需要克服小的能垒（0.19-0.32eV）就能形成一个中间产物OOCO。反应CO+O2 -- CO2+O 留下的氧原子，在PdAu团簇通过Langmuir-Hinshelwood 机制或者 Eley-Rideal 机制氧化CO分子。 计算结果说明Au团簇上Pd原子能明显改善其催化性能。
This paper investigated the catalytic activity of Pd atoms incorporated into Au(111) facet through first-principles calculations, and found that the Pd monomer, dimer, and trimer are highly reactive for the reaction of CO+O2--CO2+O via association mechanism, in which an intermediate state (OOCO) is formed.Significantly, a low energy barrier(0.19-0.32 eV) was found for the formation of OOCO.The atomic oxygen left by CO+O2 -- CO2+O2 reaction can be removed by another CO on Pd-decorated Au cluster via Langmuir-Hinshelwood or Eley-Rideal mechanism. the studies indicate Pd ensembles incorporated into Au(111) facet markedly improve the catalytic activity of gold nanocluster.
袁定旺、刘自然
化学物理学
计算物理金团簇一氧化碳氧化第一性原理计算
computational physics and chemistrygold clusterCO oxidationfirst-principles calculation
袁定旺,刘自然.PdAu纳米团簇上一氧化碳反应的第一性原理研究[EB/OL].(2012-03-28)[2025-08-17].http://www.paper.edu.cn/releasepaper/content/201203-738.点此复制
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