碱性介质中CO对甲醇在PtAu(111)和Pt(111)表面氧化生成甲酸的影响的第一性原理研究(英文)  

First-Principles Study of Effect of CO to Oxidize Methanol to Formic Acid in Alkaline Media on Pt Au(111) and Pt(111) Surfaces

作　　者：刘建红[1] 吕存琴[1,2] 晋春[1] 王贵昌[3] 

机构地区：[1]山西大同大学化学与环境工程学院,山西大同037009 [2]先进能源材料化学教育部重点实验室(南开大学),天津300071 [3]南开大学化学学院,天津市金属与分子基材料化学重点实验室(南开大学),天津300071

出　　处：《物理化学学报》2016年第4期950-960,共11页Acta Physico-Chimica Sinica

基　　金：supported by the National Natural Science Foundation of China(21503122,21346002);Natural Science Foundation of Shanxi for Youths,China(2014021016-2);Scientific and Technological Programs in Shanxi Province,China(2015031017);Foundation of Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),China~~

摘　　要：采用密度泛函理论计算研究了碱性介质中甲醇在清洁的Pt Au(111)和Pt(111)表面、及有CO存在的Pt Au(111)和Pt(111)表面的氧化。计算结果表明,在碱性介质中,预吸附的CO促进了甲醇在Pt Au(111)和Pt(111)表面氧化的每一步反应,这与其在Au(111)表面的作用相似。究其原因,是由于CO的吸附增强了OH的稳定性和碱性,从而增强了OH夺取氢原子的能力。Density functional theory calculations have been performed to investigate methanol oxidation to formic acid on Pt Au（111） and Pt（111） surfaces with and without CO in alkaline media. The calculated results show that the pre-adsorbed CO species promotes almost every step involved in the oxidation of methanol on Pt Au（111） and Pt（111） surfaces, which is similar to that observed on a Au（111） surface. These findings may be attributed to the relatively high stability and strong basicity of the OH species induced by the adsorption of CO,and the enhanced ability to strip the H atoms.

关 键 词：甲醇氧化 M(111)(M=Pt Au Pt) 碱性介质 CO促进作用 密度泛函理论计算 

分 类 号：O623.611[理学—有机化学]