ABSTRACT
The combination of hetero-elemental doping and vacancy engineering will be developed as one of the most efficient strategies to design excellent electrocatalysts for hydrogen evolution reaction (HER). Herein, a novel strategy for N-doping coupled with Co-vacancies is demonstrated to precisely activate inert S atoms adjacent to Co-vacancies and significantly improve charge transfer for CoS toward accelerating HER. In this strategy, N-doping favors the presence of Co-vacancies, due to greatly decreasing their formation energy. The as-developed strategy realizes the upshift of S 3p orbitals followed by more overlapping between S 3py and H 1s orbitals, which results in the favorable hydrogen atom adsorption free energy change (ΔGH ) to activate inert S atoms as newborn catalytical sites. Besides, this strategy synergistically decreases the bandgap of CoS, thereby achieving satisfactory electrical conductivity and low charge-transfer resistance for the as-obtained electrocatalysts. With an excellent HER activity of -89.0 mV at 10.0 mA cm-2 in alkaline environments, this work provides a new approach to unlocking inert sites and significantly improving charge transfer toward cobalt-based materials for highly efficient HER.
ABSTRACT
Herein, we have demonstrated synergistic zinc doping and defect engineering toward MoS2 nanosheet arrays assembled on carbon cloth (CC) by a one-pot hydrothermal approach for the first time, which are employed directly as a cathode for the hydrogen evolution reaction (HER). In our strategy, simultaneously doping sufficient Zn atoms and introducing a defect-rich structure into a MoS2 nanosheet can synergistically increase active sites. Additionally, the assembly of such nanosheets on CC can achieve lower charge-transfer resistance for the highly efficient HER.
