CO Oxidation at the Interface of Au Nanoclusters and the Stepped-CeO2(111) Surface by the Mars-van Krevelen Mechanism
CO Oxidation at the Interface of Au Nanoclusters and the Stepped-CeO2(111) Surface by the Mars-van Krevelen Mechanism
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DOI：
10.1021/jz301778b
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发表时间：
2013-01-03
影响因子：
5.7
通讯作者：
Henkelman, Graeme
中科院分区：
文献类型：
--
作者：
Kim, Hyun You;Henkelman, Graeme
台阶ceo2（111）表面支撑的Au-12纳米团簇氧化CO的DFT+U计算表明，台阶边缘的晶格氧通过Mars-van Krevelen （M-vK）机制氧化了结合在Au NCs上的CO。我们发现CO2的解吸决定了CO的氧化速率，空位形成能是CO氧化反应性的描述符。我们的研究结果表明，M-vK机制对工业催化剂中纳米或介观结构CeO2负载的Au颗粒上的CO氧化活性有显著贡献。
DFT+U calculations of CO oxidation by Au-12 nanoclusters supported on a stepped-CeO2(111) surface show that lattice oxygen at the step edge oxidizes CO bound to Au NCs by the Mars-van Krevelen (M-vK) mechanism. We found that CO2 desorption determines the rate of CO oxidation, and the vacancy formation energy is a reactivity descriptor for CO oxidation. Our results suggest that the M-vK mechanism contributes significantly to CO oxidation activity at Au particles supported on the nano-or meso-structured CeO2 found in industrial catalysts.