开发廉价、高性能的碳基非贵金属氧还原(ORR)催化剂是很多先进能源系统(如:质子交换膜燃料电池、直接甲醇燃料电池等)商业化应用的关键.采用聚丙烯腈前驱体,以升华硫为硫源,以氧化锌为模板,通过聚合、热处理等过程得到了氮、硫共掺杂的多孔类石墨烯ORR催化剂.该催化剂在碱性介质中表现出优异的ORR性能,其中部电位比商业Pt/C催化剂高出32 mV.除了优异的ORR催化性能,该催化剂还具有优异的稳定性、甲醇耐受性及接近100%的四电子催化过程选择性.通过研究催化剂的理化性质与ORR性能之间的关联,发现,引入硫后,催化剂的组成、结构、形貌都发生了明显的变化,而这些变化是催化剂具有优异ORR性能的重要原因.
Low-cost and high performance electrocatalysts toward oxygen reduction reaction (ORR) is important for novel energy systems,such as proton exchange membrane fuel cells,direct methanol fuel cells,and etc.In this work,a N and S codoped porous grapheme-like catalyst was obtained using polyacrylonitrile and sulfur as precursors through a facile pyrolysis procedure.The catalyst exhibited excellent performance in alkaline medium,with a half-wave potential 32 mV more positive than that of commercial Pt/C catalyst.Beside excellent ORR performance,the catalyst also exhibited outstanding methanol tolerance,stability,as well as high catalytic efficiency.By studying the relationship among catalysts structures,compositions and its catalytic performance,we found that the unique compositions,morphologies and porous structures induced by sulfur addition should be the origin to the catalyst's high ORR performance.