燃料电池热裂解铁催化剂活性中心结构测定的化学方法与模型

项目名称： 燃料电池热裂解铁催化剂活性中心结构测定的化学方法与模型

项目编号： No.21303206

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 李文木

作者单位： 中国科学院福建物质结构研究所

项目金额： 25万元

中文摘要： 在燃料电池催化相关的研究开发中,第一性原理的理论模型是一个不可或缺的工具。本项目将建立分子模型，在原子与分子水平上研究铁催化剂催化氧还原反应的机理与机制，测定高温热裂解铁催化剂的活性中心的化学结构，进而探索影响铁催化剂活性与稳定性的相关因素，为新一代铁催化剂的设计与开发提供理论指导。具体内容包括：i)通过将具有不同化学性能的取代基引入到铁酞菁分子,制备一系列新型的铁酞箐分子；ii）通过系统表征铁酞菁在酸性介质中氧还原反应催化性能、分子扰动实验与其它的电化学性质，研究铁催化剂催化氧还原反应的机理、活性与稳定性的决定因素；iii）建立分子扰动的化学模型，测定高温热裂解铁催化剂活性中心的化学结构，研究热裂解工艺与催化剂性能的关系；iv）优化铁催化剂的制备工艺，设计新型铁催化剂，验证理论的正确性。

中文关键词： 燃料电池；铁基催化剂；活性中心；模型；氧还原反应

英文摘要： In rational development of fuel cell catalysis, first principles theoretical modelling is an indispensable tool. In this proposal, first principles modeling will be employed to study non-noble oxygen reduction reaction (ORR) iron catalysts. The main objective is to gain fundamental understanding of ORR mechanism, the fators which govern the activity and stability of iron catalysts, and the chemical structur of active sites of pyrolyzed iron catalysts. The ultimate goal is to develop criteria that could guide the design and down-selection of ORR iron catalyst material.This proposal includes:i)Design and ynthesis of novel iron phthalocyanines with well designed substitutes; ii)In order to gain fundamental understanding of ORR mechanism and factors which controls the activity and stability of iron catalysts, comprehensive evaluation of the ORR performance with and without strong ligand interruption of iron phthalocyanines model compounds would be carried out in acid solution;iii) The theoretical study will explore the active site structures of pyrolyzed iron catalysts, investigate the interaction between catalysts and various reactant. New chemical models on how the ligands faciliate the ORR will be proposed; iv) New catalyst material development.High performance pyrolyzed iron catalysts will be explored based on w

英文关键词： Fuel cells；Fe-based catalysts；active sites；model；oxygen reduction reaction