Surface reconstruction of Se-doped NiS_(2) enables high-efficiency oxygen evolution reaction

查看全文 作　　者：Mengxin [1]Chen;Yuanyuan [1]Zhang;Ran [2]Wang;Bin [1]Zhang;Bo [2]Song;Yanchao [3]Guan;Siwei [4]Li;Ping [1]Xu 机构地区：[1]MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage,School of Chemistry and Chemical Engineering,Harbin Institute of Technology,Harbin 150001,Heilongjiang,China;[2]National Key Laboratory of Science and Technology on Advanced Composites in Special Environments,Harbin Institute of Technology,Harbin 150001,Heilongjiang,China;[3]Key Laboratory of Micro-systems and Micro-structures Manufacturing,Ministry of Education,Harbin Institute of Technology,Harbin 150001,Heilongjiang,China;[4]Institute of Industrial Catalysis,School of Chemical Engineering and Technology,Xi’an Jiaotong University,Xi’an 710049,Shaanxi,China 出　　处：《Journal of Energy Chemistry》索引2023年第9期,共8页 基　　金：supported by the financial support from the National Natural Science Foundation of China (21871065, 22071038, 22209129);the Heilongjiang Touyan Team (HITTY20190033);the Interdisciplinary Research Foundation of HIT (IR2021205)。 摘　　要：Surface reconstruction of electrocatalysts has been widely witnessed during the electrochemical processes.Here,NiS_(2),NiSe_(2), and Se doped NiS_(2)(Se-NiS_(2)) are fabricated for oxygen evolution reaction(OER) through a mild sulfuration and/or selenylation process of Ni(OH)_(2) supported on carbon cloth(CC).Through careful in-situ Raman spectroscopy and ex-situ X-ray photoelectron spectroscopy,surface reconstruction of NiS_(2),NiSe_(2),and Se-NiS_(2) during the OER process has been revealed.A potentialdependent study shows that Se-NiS_(2) undergoes surface evolution at lower potentials and requires the lowest potential for conversion to NiOOH as a highly OER-active species,accompanied by the leaching of SO_(4)^(2-) and SeO_(4)^(2-) that can again be adsorbed on the catalyst surface to enhance the catalytic activity.Density functional theory(DFT) calculations confirm that Se-NiS_(2) is more susceptible to surface oxidation through the OER process.Therefore,Se-NiS_(2) exhibits outstanding OER activity and stability in alkaline conditions,requiring an overpotential of 343 mV at a current density of 50 mA cm^(-2).A novel insight is provided by our work in understanding the surface reconstruction and electrocatalytic mechanism of Ni-based chalcogenides. 关 键 词：Oxygen evolution reaction Se-NiS_(2) In-situ Raman spectroscopy Anion leaching Surface reconstruction