富氢条件下CO选择性氧化机理的原位动态红外光谱研究

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.

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。

本项目的主要成果有：（1）设计加工了新型原位红外光谱池，并获得了专利授权；（2）研究了H2在模型催化剂上的吸附、脱附和氧化行为；（3）考察了CO在模型催化剂上的吸附、脱附和氧化行为；考察了载体对CO氧化速率和反应级数的影响；（4）考察了H2和CO在模型催化剂上的竞争吸附行为；（5）设计了新型CO2捕捉剂，对新型捕捉剂的捕捉性能进行了考察，并对捕捉性能和物化性质之间的关系进行了研究；（6）培养了3名硕士生。.