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The key descriptor that dominates the kinetics of the alkaline hydrogen evolution reaction (HER) has not yet been unequivocally identified. Herein, we focus on the adsorbed hydroxyl (OHad ) transfer process (OHad + e- ⇄ OH- ) and reveal its crucial role in promoting the overall kinetics of alkaline HER based on Ni/Co-modified MoSe2 model catalysts (Ni-MoSe2 and Co-MoSe2 ) that feature almost identical water dissociation and hydrogen adsorption energies, but evidently different activity trends in alkaline (Ni-MoSe2 ≫ Co-MoSe2 ) and acidic (Co-MoSe2 ≥ Ni-MoSe2 ) media. Experimental and theoretical calculation results demonstrate that tailoring MoSe2 with Ni not only optimizes the hydroxyl adsorption, but also promotes the desorption of OH- and the electron-involved conversion of OHad to OH- , all of which synergistically accelerate the kinetics of OHad + e- ⇄ OH- and thereby the overall kinetics of the alkaline HER.
Mao et al. (Wed,) studied this question.