Hydrogen etching induced hierarchical meso/micro-pore structure with increased active density to boost ORR performance of Fe-N-C catalyst

作     者：Liqin Gao Meiling Xiao Zhao Jin Changpeng Liu Junjie Ge Wei Xing Liqin Gao;Meiling Xiao;Zhao Jin;Changpeng Liu;Junjie Ge;Wei Xing

作者机构：State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of ScienceChangchun 130022 Jilin China University of Chinese Academy of SciencesBeijing 100039 China Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChangchun 130022 Jilin China 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2019年第28卷第8期

页      面：17-23,I0002页

核心收录：

学科分类：0820[工学-石油与天然气工程] 0808[工学-电气工程] 07[理学] 0817[工学-化学工程与技术] 0807[工学-动力工程及工程热物理] 0827[工学-核科学与技术] 0703[理学-化学] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China(21633008,21433003,U1601211,21733004) National Science and Technology Major Project(2016YFB0101202) Jilin Province Science and Technology Development Program(20150101066JC,20160622037JC,20170203003SF,20170520150JH) Hundred Talents Program of Chinese Academy of Sciences and the Recruitment Program of Foreign Experts(WQ20122200077) 

主　　题：Hierarchical meso/micro-pore structure Hydrogen etching Single site Fe-N-C catalysts Carbon-nitrogen-coordinated iron(FeN4) Oxygen reduction reaction 

摘      要：Rational regulation on pore structure and active site density plays critical roles in enhancing the performance of Fe-N-C catalysts. As the microporous structure of the carbon substrate is generally regarded as the active site hosts, its hostility to electron/mass transfer could lead to the incomplete fulfillment of the catalytic activity. Besides, the formation of inactive metallic Fe particles during the conventional catalyst synthesis could also decrease the active site density and complicate the identification of real active site. Herein, we developed a facial hydrogen etching methodology to yield single site Fe-N-C catalysts featured with micro/mesoporous hierarchical structure. The hydrogen concentration in pyrolysis process was designated to effectively regulate the pore structure and active site density of the resulted catalysts.The optimized sample achieves excellent ORR catalytic performance with an ultralow H2O2 yield(1%)and superb stability over 10,000 cycles. Our finding provides new thoughts for the rational design of hierarchically porous carbon-based materials and highly promising non-precious metal ORR catalysts.