Carbon-nitrogen/graphene composite as metal-free electrocatalyst for the oxygen reduction reaction  

作　　者：MA YanWen ZHANG LingRong LIJuanJuan NI HaiTao LI Meng ZHANG JinLei FENG XiaoMiao FAN QuLi HU Zheng HUANG Wei 

机构地区：[1]Jiangsu Key Laboratory for Organic Electronics ＆ Information Displays and Institute of Advanced Materials, Nanjing University of Posts and Telecommunications, Nanjing 210046, China [2]Key Laboratory of Mesoscopic Chemistry of Ministry of Education, Jiangsu Provincial Laboratory for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China

出　　处：《Chinese Science Bulletin》2011年第33期3583-3589,共7页

基　　金：supported by the National Basic Research Program of China (2009CB930600);the National Natural Science Foundation of China (20833002, 20903057, 20905038, 20974046);the Research Fund for the Doctoral Program of Higher Education of China (20093223120002);the Natural Science Foundation of Jiangsu Province (BK2010525);the Foundation of Jiangsu Educational Committee (09KJB150007, 08KJB150011);the Scientific Research Foundation of Nanjing University of Posts and Telecommunications (NY208046)

摘　　要：Sheet-like carbon-nitrogen (CNx)/graphene composites with a high content of nitrogen (x≤0.15) was prepared by the carbonization of polypyrrole (PPy)/reduced-graphene-oxide (rGO) composite at 600-800°C. We used rGO instead of graphene oxide (GO) sheets as a template and a substrate to immobilize PPy since the PPy/GO composite agglomerates easily because of the dehydration of excess oxygen-containing groups on the GO sheets during the drying process. The dried PPy/rGO intermediate and its derived CNx/graphene products retain their high dispersion and loose-powder features. The as-prepared CNx/graphene composites have a total nitrogen content of about 10 at% and their nitrogen state is mainly of pyridinic and graphitic type. CNx/graphene composites exhibit excellent performance for the oxygen reduction reaction (ORR) in terms of electrocatalytic activity, stability and immunity towards methanol crossover and CO poisoning, suggesting their potential as metal-free electrocatalysts for the ORR.Sheet-like carbon-nitrogen （CNx）/graphene composites with a high content of nitrogen （x 〈 0.15） was prepared by the carboniza- tion of polypyrrole （PPy）/reduced-graphene-oxide （rGO） composite at 600-800℃. We used rGO instead of graphene oxide （GO） sheets as a template and a substrate to immobilize PPy since the PPy/GO composite agglomerates easily because of the dehydration of excess oxygen-containing groups on the GO sheets during the drying process. The dried PPy/rGO intermediate and its derived CNJgraphene products retain their high dispersion and loose-powder features. The as-prepared CNJgraphene composites have a total nitrogen content of about 10 at% and their nitrogen state is mainly of pyridinic and graphitic type. CNJgraphene composites exhibit excellent performance for the oxygen reduction reaction （ORR） in terms of electrocatalytic activity, stability and immunity towards methanol crossover and CO poisoning, suggesting their potential as metal-free electrocatalysts for the ORR.

关 键 词：氧还原反应 复合金属 电催化剂 石墨复合材料 一氧化碳中毒 石墨氧化物 总氮含量 干燥过程 

分 类 号：TM911.46[电气工程—电力电子与电力传动]