异原子过渡金属和磷共掺杂碳的制备及其对氧气还原催化机理的研究

项目名称： 异原子过渡金属和磷共掺杂碳的制备及其对氧气还原催化机理的研究

项目编号： No.51272167

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 一般工业技术

项目作者： 杨瑞枝

作者单位： 苏州大学

项目金额： 80万元

中文摘要： 寻求低成本和高催化活性的非贵金属催化剂，是解决质子交换膜燃料电池(PEMFC)由Pt基贵金属催化剂带来的成本高问题的重要途径。本项目提出制备异原子过渡金属和磷共掺杂碳作为阴极氧气还原的催化剂。通过过渡金属和磷共掺杂调控碳的电子结构以及对氧气还原的催化活性，针对异原子掺杂碳催化剂的催化活性位以及对氧气还原机理存在的争议，研究具有给电子性异原子掺杂对催化活性位的形成以及对氧气还原机理的影响。以含磷的离子液体、含碳有机物和过渡金属盐为前驱体，采用模板法制备材料。以原位X-射线衍射（XRD）和原位X-射线吸收谱（XAS）研究催化剂的催化活性位；利用原位拉曼光谱分析氧气还原的中间产物，结合氧气电极过程动力学研究，阐明具有给电子性异原子掺杂碳对氧气还原的催化机理，为设计、制备高催化活性的异原子掺杂碳非贵金属催化剂提供理论和实验基础。

中文关键词： 碳；掺杂；催化剂；氧气还原反应；催化机理

英文摘要： The development of low cost and highly active non-noble metal catalysts will lead to a significant cost reduction brought by Pt in the Proton Exchange Membrane Fuel Cells(PEMFCs).Heteroatoms of transition metal and phosphorus co-doped carbon catalysts for the oxygen reduction reaction at the cathode of the PEMFC are proposed in this project. The co-doping of transition metal and phosphorus in carbon will be used to modify the electronic structure of the carbon and the catalytic activiy of the carbon for the oxygen reduction reaction.The effect of doping with the electron-donor heteroatoms on the active sites of the catalysts and the oxygen reduction reaction mechanism will be studied.The debates on the active sites of electron-donor heteroatom-doped carbon and the oxygen reduction mechanism will be addressed. The transition metal and phosphorus co-doped carbon catalysts will be prepared by a template method with phosphorus-containing ionic liquids,carbon-containing organic compounds and transition metal salts as precursors.The nature of the active sites will be studied by in-situ X-ray Diffraction and in-situ X-ray Absorption Spectroscopy. The intermediates produced in the oxygen reduction reaction will be studied by in-situ Raman. Electrode kinetics of the oxgyen reduction reaction on the prepared catalysts wil

英文关键词： Carbon；Doped；Catalyst；Oxygen Reduction Reaction；Catalytic Mechanism