文献类型：期刊文献

英文题名：Iodine-Doping-Induced Electronic Structure Tuning of Atomic Cobalt for Enhanced Hydrogen Evolution Electrocatalysis

作者：Liu, Jianbin[1,2];Wang, Dashuai[3,4];Huang, Kang[1,2];Dong, Juncai[5];Liao, Jiangwen[5];Dai, Sheng[6,7];Tang, Xuan[6,7];Yan, Minmin[1,2];Gong, Haisheng[1,2];Liu, Jingjing[1,2];Gong, Zhichao[1,2];Liu, Rui[1,2];Cui, Chunyu[1,2];Ye, Gonglan[1,2];Zou, Xiaolong[3,4];Fei, Huilong[1,2]

机构：[1]Hunan Univ, State Key Lab Chemo Biosensing & Chemometr, Adv Catalyt Engn Res Ctr, Minist Educ, Changsha 410082, Peoples R China;[2]Hunan Univ, Coll Chem & Chem Engn, Changsha 410082, Peoples R China;[3]Tsinghua Univ, Shenzhen Geim Graphene Ctr, Tsinghua Berkeley Shenzhen Inst, Shenzhen 518055, Peoples R China;[4]Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China;[5]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China;[6]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[7]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Inst Fine Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2021

卷号：15

期号：11

起止页码：18125

外文期刊名：ACS NANO

收录：;EI(收录号：20214711191017);WOS:【SCI-EXPANDED(收录号:WOS:000747115200088)】；

基金：H.F. acknowledges financial support from the National Natural Science Foundation of China (Grant No. 51902099), the Hunan high-level talent gathering project (Grant No. 2019RS1021), Fundamental Research Funds for the Central Universities (Grant No. 531119200087), and the Innovative Research Groups of Hunan Province (Grant No. 2020JJ1001). G.Y. acknowledges support from the Hunan Province Natural Science Foundation (Grant No. 2020JJ4204) and Fundamental Research Funds for the Central Universities (Grant No. 531118010707). J. D. acknowledges support from Youth Innovation Promotion Association CAS. We thank the beamlines MCD-A and MCD-B (Soochow Beamline for Energy Materials) at NSRL for access and support that contributed to the results presented here. X.Z. acknowledges support from Guangdong Innovative and Entrepreneurial Research Team Program (Grant No. 2017ZT07C341) and the Bureau of Industry and Information Technology of Shenzhen for the 2017 Graphene Manufacturing Innovation Center Project (Grant No. 201901171523). S.D. acknowledges support from the Fundamental Research Funds for the Central Universities (Grant No. JKVJ1211022), Shanghai Rising-star Program (Grant No. 20QA1402400), and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center. J.L. acknowledges support from the Postgraduate Scientific Research Innovation Project of Hunan Province (Grant No. CX20200440).

语种：英文

外文关键词：electronic structure tuning; iodine doping; single-atom catalysts; metal-nitrogen-carbon materials; hydrogen evolution reaction

摘要：The development of strategies for tuning the electronic structure of the metal sites in single-atom catalysts (SACs) is the key to optimizing their activity. Herein, we report that iodine doping within the carbon matrix of a cobalt-nitrogen-carbon (Co-N-C) catalyst can effectively modulate its electronic structure and catalytic activity toward the hydrogen evolution reaction (HER). The iodine-doped Co-N-C catalyst shows exceptional HER activity in acid with an overpotential of merely 52 mV at 10 mA cm(-2), a small Tafel slope of 56.1 mV dec(-1), making it among the best SACs based on both precious and nonprecious metals. Moreover, this catalyst possesses a high turnover frequency (TOF) value of 1.88 s(-1) (eta = 100 mV), which is about 1 order of magnitude larger than that (0.2 s(-1)) of the iodine-free counterpart. Experimental and theoretical studies demonstrate that the introduction of iodine dopants lowers the chemical oxidation state of the Co sites, resulting in the optimized hydrogen adsorption and facilitated HER kinetics. This work provides an alternative strategy to regulate the electronic structure of SACs for improved performance.