聚苯乙烯模板制备中空Co-N共掺杂碳基复合材料及氧还原性能  

Preparation of Hollow Co-N Co-Doped Carbon Matrix Composites With Polystyrene Templating Agentand Oxygen Reduction Properties

作　　者：贺新福[1,2] 韩鹏飞 蔡江涛 吴红菊[1] 唐勇 常廖博[1] 高凡 李可可 张展瑞 张亚婷[1,2] 周安宁 He Xinfu;Han Pengfei;Cai jiangtao;Wu Hongju;Tang Yong;Chang Liaobo;Gao Fan;Li Keke;Zhang Zhanrui;Zhang Yating;Zhou Anning(School of Chemistry and Chemical Engineering,Xi’an University of Science and Technology,Xi'an 710054,China;Key Laboratory of Coal Resources Exploration and Comprehensive Utilization,Ministry of Natural Resource,Xi'an 710021,China)

机构地区：[1]西安科技大学化学与化工学院,西安710054 [2]自然资源部煤炭资源勘查与综合利用重点实验室,西安710021

出　　处：《工程塑料应用》2022年第6期36-43,共8页Engineering Plastics Application

基　　金：国家自然科学基金项目(U1703251,U1810113);陕西省重点研发计划项目(2022GY-168)。

摘　　要：采用一种简单有效的模板辅助方法制备了具有分级多孔和中空结构的Co,N共掺杂碳基复合材料(CoNHC)。通过在聚苯乙烯(PS)微球表面原位生长沸石咪唑盐骨架(ZIF-67),以及热解去除PS模板同时碳化ZIF-67,构建了该催化剂独特的结构。所得催化剂在碱性电解质溶液中显示出优异的氧还原反应(ORR)活性,其中Co-NHC-5的起始电位、半波电位和极限扩散电流密度分别是0.94V,0.82V和5.45mA/cm^(2),优于商业Pt/C催化剂;其ORR过程转移电子数为3.89,接近四电子转移过程;其优异的ORR性能归因于其具有大的比表面积、多孔结构、高含量的吡啶氮和石墨氮活性位点。该催化剂还显示出比Pt/C更好的甲醇耐受性和稳定性,可用作燃料电池的ORR电催化剂。Co,N co-doped carbon-based composites(Co-NHC)with graded porous and hollow structures were prepared by using a simple and effective template-assisted method.The unique structure of the catalyst was constructed by in situ growth of zeolite imidazolium salt skeletons(ZIF-67)on the surface of polystyrene(PS)microspheres,and by pyrolytic removal of the PS template and carbonization of ZIF-67.The resulting catalysts show excellent oxygen reduction reaction(ORR)activity in alkaline electrolyte solutions,of which the onset potential,half-wave potential and limiting current density of Co-NHC-5 are 0.94 V,0.82 V and 5.45 mA/cm~2,respectively,which are higher than those of commercial Pt/C catalyst.The number of transferred electrons of CoNHC-5 obtained from the K-L curve is 3.89,indicating that its ORR process is dominant by four-electron process.The excellent ORR performance is attributed to its large specific surface area,porous structure,high content of pyridine and graphite nitrogen active sites.The Co-NHC-5 also shows better methanol tolerance and stability than commercial Pt/C catalyst.

关 键 词：聚苯乙烯微球模板 氧还原反应 电催化剂 金属有机框架 

分 类 号：TQ152[化学工程—电化学工业]