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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.
This 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).