氮掺杂多孔碳包覆铁纳米粒子催化剂用于高效碱性介质中氧还原反应  

Fe Nanoparticles Encapsulated in N-doped Porous Carbon for Efficient Oxygen Reduction in Alkaline Media

作　　者：李春艳 张蕊 巴笑杰 姜晓乐 阳耀月 Chun-Yan Li;Rui Zhang;Xiao-Jie Ba;Xiao-Le Jiang;Yao-Yue Yang(Key Laboratory of General Chemistry of the National Ethnic Affairs Commission,School of Chemistry and Environment,Southwest Minzu University,Chengdu,Sichuan,610041,China)

机构地区：[1]化学基础国家民委重点实验室,西南民族大学化学与环境学院,四川成都610041

出　　处：《电化学》2023年第5期12-23,共12页Journal of Electrochemistry

基　　金：supported by the National Natural Science Foundation of China(Grants 22002121,22172121);the National Undergraduate Training Program for Innovation and Entrepreneurship(Grant S202210656087).

摘　　要：合理设计和合成非贵金属催化剂对提高氧还原反应的催化活性和稳定性具有重要意义,但仍然存在重大挑战。本工作采用功能化金属有机框架材料为前驱体,合成了氮掺杂多孔碳包覆Fe纳米粒子催化剂(Fe@N-C)。Fe纳米颗粒的嵌入提高了催化剂的石墨化程度和石墨化氮的比例,同时促进了中孔的形成。Fe@N-C-30催化剂在碱性溶液中表现出良好的氧还原反应活性(E_(0)=0.97V vs.RHE,E1/2=0.89V vs.RHE)。此外,与商用Pt/C相比,Fe@N-C-30催化剂具有更好的耐甲醇性和循环稳定性。其优异的电催化活性归因于高的电化学表面积、相对高比例的石墨化氮、独特的孔结构以及包覆的Fe颗粒与碳层之间的协同效应。本工作为利用金属有机框架材料制备高效非贵金属ORR催化剂提供了一种有前景的方法。Rational design and synthesis of non-precious-metal catalyst plays an important role in improving the activity and stability for oxygen reduction reaction(ORR)but remains a major challenge.In this work,we used a facile approach to synthesize iron nanoparticles encapsulated in nitrogen-doped porous carbon materials(Fe@N-C)from functionalized metal-organic frameworks(MOFs,MET-6).Embedding Fe nanoparticles into the carbon skeleton increases the graphitization degree and the proportion of graphitic N as well as promotes the formation of mesopores in the catalyst.The Fe@N-C-30 catalyst showed the excellent ORR activity in alkaline solutions(E^(0)=0.97 V vs.RHE,E1/2=0.89 V vs.RHE).Moreover,the Fe@N-C-30 catalyst exhibited better methanol resistance and long-term stability when compared to commercial Pt/C.The superior ORR performance could be attributed to the combination of high electrochemical surface area,relative high portion of graphitic-N,unique porous structures and the synergistic effect between the encapsulated Fe particles and the N-doped carbon layer.This work provides a promising method to construct efficient non-precious-metal ORR catalyst through MOFs.

关 键 词：金属有机框架 多孔结构 铁纳米粒子 氧还原反应 

分 类 号：TQ426[化学工程] TM911.4[电气工程—电力电子与电力传动]