文献类型：期刊文献

英文题名：Realization of all-in-one hydrogen-evolving photocatalysts via selective atomic substitution

作者：Qiu, Bocheng[1];Huang, Pan[3];Lian, Cheng[3];Ma, Yingxin[1];Xing, Mingyang[2];Liu, Honglai[3];Zhang, Jinlong[2,4]

机构：[1]Nanjing Agr Univ, Dept Chem, Coll Sci, Jiangsu Key Lab Pesticide Sci, Nanjing 210095, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalys, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Feringa Nobel Prize Scientist Joint Res Ctr,Sch C, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai Engn Res Ctr Hierarch Nanomat, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China

年份：2021

卷号：298

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20212910641994);WOS:【SCI-EXPANDED(收录号:WOS:000696912300006)】；

基金：This work was supported by National Natural Science Foundation of China (21972040, 21822603, 21773062, 91834301, 2207808), Shanghai Municipal Science and Technology (2018SHZDZX03, 20DZ2250400), Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Program of Introducing Talents of Discipline to Universities (B16017, B20031), and the Fundamental Research Funds for the Central Universities. Prof. B. C. Qiu gratefully acknowledges the support from Nanjing Agriculture University.

语种：英文

外文关键词：Selective substitution; Charge separation; Hydrogen adsorption and desorption; Photocatalytic hydrogen evolution

摘要：Major challenges of realization of all-in-one hydrogen-evolving photocatalysts are the relatively poor charge separation efficiency and unfavorable hydrogen desorption properties owing to the strong correlation between the catalytic site and adsorbed H. Herein, an example of Ni doped few-layer ZnIn2S4 nanosheets (Ni-ZnIn2S4) is carried out to deeply understand the role of Ni dopant in tailoring the charge separation efficiency and weakening the bond energy between electronegative S sites and adsorbed H (S-H ads). Our theoretical calculations demonstrate that Ni ions preferentially incorporates into tetrahedral Zn sites rather than tetrahedral/octahedral In sites, which endows Ni-ZnIn2S4 with improved electronic conductivity and more delocalized charge carriers involved in hydrogen evolution reaction (HER). More importantly, Ni dopants can be capable of exquisitely altering the electronic structure of S sites, leading to a balanced hydrogen adsorption and desorption ability. Consequently, the as-prepared few-layer Ni-ZnIn2S4 nanosheets enable long-lived photo-excited electrons and enhanced photocatalytic HER performance.