Collaborative effect between single-atom Re and S vacancy on modulating localized electronic structure of MoS_(2) catalysts for alkaline hydrogen evolution  

作　　者：Yajing Zhang Xingkun Wang Xiangju Song Heqing Jiang 

机构地区：[1]Key Laboratory of Functional Membrane Material and Membrane Technology, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, China [2]Shandong Energy Institute, Qingdao, 266101, China [3]Qingdao New Energy Shandong Laboratory, Qingdao, 266101, China [4]University of Chinese Academy of Sciences, Beijing, 100049, China

出　　处：《Nano Research》2024年第11期9507-9517,共11页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(No.22209193);Natural Science Foundation of Shandong Province(Nos.ZR2020ZD10 and ZR2021QB111);the Taishan Scholars Program of Shandong Province(No.tstq20221151);the Innovation Funds of Shandong Energy Institute(No.SEI I202140).

摘　　要：Optimizing the catalytic activity and stability of molybdenum disulfide (MoS_(2)) towards alkaline hydrogen evolution reaction (HER) is significant for sustaining green hydrogen. A moderate localized electronic structure of active sites plays a crucial role in determining the activity and stability of the catalysts, yet how to construct such localized electronic structure still remains indeterminacy. Enlightened by theoretical prediction, herein, the introduction of both single-atom Re and the adjacent S vacancy in MoS_(2) (denoted as Re-MoS_(2)-Vs) exhibits collaborative effect on regulating the localized electronic structure of active sites (viz. Re-(S, Vs)-Mo). Such regulated electronic structure helps to decrease the energy barrier of the water dissociation and optimize hydrogen adsorption energy for enhancing alkaline HER performance. Most importantly, Mo-S bonds in the above local Re-(S, Vs)-Mo configurations are also strengthened for preventing the leaching of Mo and S atoms and then ensuring the long-time stability. Consequently, the deliberately designed Re-MoS_(2)-Vs with a Re coordination number of ~ 5.0 is experimentally verified to exhibit a comparable electrocatalytic performance and robust operational stability over 120 h. This strategy provides a promising guidance for modulating the electronic structure of MoS_(2) based catalysts via double-tuning atomic-scale local configuration for HER applications.

关 键 词：molybdenum disulfide localized electronic structure atomic Re doping S vacancy alkaline hydrogen evolution 

分 类 号：O64[理学—物理化学]