文献类型：期刊文献

英文题名：P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution

作者：Meng, Chao[1,2] Gao, Yuanfeng[3] Zhou, Yue[3] Sun, Kang[4] Wang, Yanmin[3] Han, Ye[5] Zhao, Qianqian[2] Chen, Xuemin[6] Hu, Han[1] Wu, Mingbo[1]

第一作者：Meng, Chao

通信作者：Hu, H[1];Zhou, Y[2];Han, Y[3]

机构：[1]China Univ Petr East China, Inst New Energy, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China;[2]Shandong Univ Sci & Technol, Coll Elect Engn & Automat, Qingdao 266590, Peoples R China;[3]Shandong Univ Sci & Technol, Coll Energy Storage Technol, Qingdao 266590, Peoples R China;[4]Chinese Acad Forestry, Inst Chem Ind Forest Prod, Nanjing 210042, Peoples R China;[5]Shandong Univ Sci & Technol, Sch Mat Sci & Engn, Qingdao 266590, Peoples R China;[6]Hebei Univ Sci & Technol, Coll Sci, Shijiazhuang 050018, Peoples R China

年份：0

外文期刊名：NANO RESEARCH

收录：;EI(收录号：20225013253780);Scopus(收录号：2-s2.0-85143767660);WOS:【SCI-EXPANDED(收录号:WOS:001023725400024)】；

基金：AcknowledgementsThis work was supported by the National Natural Science Foundation of China (Nos. 51901115 and 51802075), the Shandong Provincial Natural Science Foundation, China (Nos. ZR2019PEM001, ZR2019BB009, and ZR2020ZD08), and the Young Talents Program in University of Hebei Province, China (No. BJ2019002).

语种：英文

外文关键词：molybdenum disulfide; p-orbital electron structure; basal S sites; hydrogen evolution; synergistic mechanism

摘要：The edge S sites of thermodynamically stable 2H MoS2 are active for hydrogen evolution reaction (HER) but the active sites are scarce. Despite the dominance of the basal S sites, they are generally inert to HER because of the low p-band center. Herein, we reported a synergistic combination of phase engineering and NH4+ intercalation to promote the HER performance of MoS2. The rational combination of 1T and 2H phases raises the p-band center of the basal S sites while the intercalated NH4+ ions further optimize and stabilize the electronic band of these sites. The S sites with regulated band structures afford moderate hydrogen adsorption, thus contributing to excellent HER performance over a wide pH range. In an acid medium, this catalyst exhibits a low overpotential of 169 mV at 10 mA.cm(-2) and Tafel slope of 39 mV.dec(-1) with robust stability, superior to most of recently reported MoS2-based non-noble catalysts. The combined use of in/ex-situ characterizations ravels that the appearance of more unpaired electrons at the Mo 4d-orbital reduces the d-band center which upshifts the p-band center of the adjacent S for essentially improved HER performance. This work provides guidelines for the future development of layered transition-metal-dichalcogenide catalysts.