富氢条件下CO选择性氧化机理的原位动态红外光谱研究

项目名称： 富氢条件下CO选择性氧化机理的原位动态红外光谱研究

项目编号： No.21203167

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 物理化学

项目作者： 胡庚申

作者单位： 浙江师范大学

项目金额： 26万元

中文摘要： 富氢条件下CO选择性氧化对提高质子交换膜燃料电池的活性和稳定性具有重要的意义。项目针对CO选择性氧化反应机理研究存在的问题，采用原位动态衰减全反射红外光谱结合准原位XPS和理论计算研究H2和CO在模型催化剂表面的吸附和氧化；研究金属不同晶面和表面缺陷位对CO氧化反应的贡献；探索表面吸附H与CO的相互作用和表面H对催化剂CO选择性氧化性能的影响；考察载体和水汽对CO选择性氧化性能的影响。通过综合分析实验和理论计算结果，提出表面吸附H与金属之间的相互作用机制，阐明金属不同晶面和表面缺陷位对CO氧化反应的贡献，揭示富氢条件下载体和水汽影响金属催化剂CO氧化性能的作用机制，为设计和开发新型高效的CO选择性氧化催化剂提供理论基础和科学依据。

中文关键词： 原位红外光谱；氢吸附；气固界面；CO选择性氧化；机理研究

英文摘要： Preferential oxidation of CO in hydrogen-rich gas has vital significance to improve the activity and stability of Proton Exchange Membrane Fuel Cell (PEMFC). Aiming at the problems in mechanistic study of CO selective oxidation in hydrogen-rich gas, this project will employ in-situ real-time Attenuated Total Reflection Infrared (ATR-IR) in conjunction with quasi-in situ XPS and theoretical calculations to investigate the adsorption and oxidation of H2 and CO on model catalysts; explore the contributions of different crystal surfaces and surface defects of metals to CO oxidation; examine the interaction between surface-adsorbed H and CO and the influence on CO oxidation performance of surface H; investigate the effects of supports and moisture on CO oxidation. Based on the experimental and theoretical results, the mechanism of interaction between surface-adsorbed H and metals will be proposed; the contributions from different crystal surfaces and surface defects of metals for CO oxidation will be clarified; the roles of supports and moisture for CO oxidation in hydrogen-rich gas will be revealed. The study will provide theoretical and scientific basis for designing and developing highly-active catalysts for CO selective oxidation.

英文关键词： in-situ IR；hydrogen adsorption；gas-soild interface；preferential CO oxidation；mechanism study