Lacking strategies to simultaneously address the intrinsic activity, site density, electrical transport, and stability problems of chalcogels is restricting their application in catalytic hydrogen production. Herein, we resolve these challenges concurrently through chemically activating the molybdenum disulfide (MoS2) surface basal plane by doping with a low content of atomic palladium using a spontaneous interfacial redox technique. Palladium substitution occurs at the molybdenum site, simultaneously introducing sulfur vacancy and converting the 2H into the stabilized 1T structure. Theoretical calculations demonstrate the sulfur atoms next to the palladium sites exhibit low hydrogen adsorption energy at –0.02 eV. The final MoS2 doped with only 1wt% of palladium demonstrates exchange current density of 805 μA cm−2 and 78 mV overpotential at 10 mA cm−2, accompanied by a good stability. The combined advantages of our surface activating technique open the possibility of manipulating the catalytic performance of MoS2 to rival platinum.

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