燃料电池中石墨烯基非金属催化剂及其氧还原催化机理研究

项目名称： 燃料电池中石墨烯基非金属催化剂及其氧还原催化机理研究

项目编号： No.21303054

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： 王潇

作者单位： 华东理工大学

项目金额： 25万元

中文摘要： 氧气在燃料电池中的还原反应是一个动力学慢反应，这导致了燃料电池的效率大大降低。开发可替代铂基催化剂的非金属燃料电池催化剂对燃料电池的广泛应用及发展具有重要的意义。本项目以设计高活性非金属石墨烯基催化剂为目标，利用密度泛函理论对多种非金属元素掺杂修饰的石墨烯非金属催化剂的形成与稳定性以及掺杂元素对石墨烯结构电子性质和化学吸附性质的影响进行系统深入的研究，并通过寻找酸性及碱性条件下石墨烯基非金属催化剂氧还原过程的最优反应路径，提出不同非金属元素掺杂下石墨烯结构的催化活性点及催化机理，建立"结构-催化活性"相互关系，并开发设计酸性条件下具有高活性高稳定性的二元及多元掺杂非金属石墨烯材料作为氧还原催化剂。通过本项目，将为高活性非金属催化剂的制备研究提供新的途径和思路，丰富和完善碳基非金属催化剂的研究。

中文关键词： 非金属掺杂；石墨烯；氧还原；自由能；

英文摘要： Since the reaction rate at the cathode is much lower than that at the anode, the oxygen reduction reaction (ORR) at the cathode plays a key role in controlling the performance of a fuel cell. Platinum has conventionally been employed as the cathode catalyst due to its high activity for the ORR. However, the large-scale application of fuel cells has been hampered by the high cost and inadequacy, poor stability and deactivation in the presence of CO (a by-product from the use of methanol) of this metal. Thus, developing inexpensive electrocatalysts with high catalytic activity will accelerate the process of fuel cell commercialization. The aim of this project is to design metal-free catalyst with stability and high catalytic efficiency, especially in acid solution. In this project, not only the catalytic pathways of ORR on nitrogen doped grapheme but also on other non-metal elements doped ones are investigated using density functional theory. Combined with the study of the change of their electronic structures, we will propose their catalytic mechanism and establish the correlation between ORR activities and material microstructure. Based on these results, some new graphene based metal-free catalysts will be designed by co-doping or multi-doping to further improve their catalytic efficiency. This study will provid

英文关键词： Non-metal doping；Graphene；Oxygen reduction；Free energy；