Abstract
Regulating the electronic structure of MoS2 by constructing cationic vacancies is an effective method to activate and improve its intrinsic properties. Herein, we synthesize the MoS2-based composite with abundant single atomic Mo cation vacancies through uniformly loading nickel-cobalt-Prussian blue analogues (NiCoPBA) (NiCoPBA-MoS2-VMo) by immersing a single Ni atom-decorated MoS2 (Ni-MoS2) into K3[Co(CN)6] solution. Subsequently, NiCoP-MoS2-VMo with improved conductivity is obtained by phosphating the composite as a high-efficiency hydrogen evolution reaction (HER) catalyst. Experiments and theoretical calculations indicate that the electrons of NiCoP are spontaneously transferred to the substrate MoS2-VMo nanosheets in NiCoP-MoS2-VMo, and the moderately oxidized NiCoP is beneficial to the adsorption of OH*. Meanwhile, the mono-atomic Mo cation vacancies of the catalyst modulate the electronic structure of S, optimizing the adsorption of hydrogen in the reaction process. Therefore, NiCoP-MoS2-VMo has enhanced chemical adsorption for H* (on MoS2-VMo) and OH*(on NiCoP), expediting the water-splitting step and HER catalysis, and benefiting from the regulation of the electronic structure induced by the construction of metallic Mo vacancies in MoS2, the as-prepared catalyst displays an overpotential of only 67 mV at 10 mA cm-2 with long-term stability (no current decay over 20 h). This work affords not only a kind of efficient HER catalysts but also a new valuable route for developing inexpensive and high-performance catalysts with single atomic cation vacancies.
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