Edge-enriched N, S co-doped hierarchical porous carbon for oxygen reduction reaction

查看全文 作　　者：Fangfang [1,2]Chang;Panpan [1]Su;Utsab [1]Guharoy;Runping [1]Ye;Yanfu [1]Ma;Huajun [3]Zheng;Yi [3]Jia;Jian [1,4]Liu 机构地区：[1]State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;[2]University of Chinese Academy of Sciences,Beijing 100049,China;[3]Department of Applied Chemistry and Zhejiang Carbon Neutral Innovation Institute,Zhejiang University of Technology,Hangzhou 310032,China;[4]DICP-Surrey Joint Centre for Future Materials,Department of Chemical and Process Engineering,University of Surrey,Guildford,Surrey GU27XH,United Kingdom 出　　处：《Chinese Chemical Letters》索引2023年第34卷第2期,共6页 基　　金：supported financially by the National Natural Science Foundation of China (No. 21905271);Liaoning Natural Science Foundation (No. 20180510029);the Dalian National Laboratory for Clean Energy (DNL), DNL Cooperation Fund, Chinese Academy of Sciences (No. DNL180402)。 摘　　要：The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts. 关 键 词：Porosity engineering N S co-doped carbon materials Hierarchical porous carbon Edge-enriched carbon Oxygen reduction reaction DFT calculation