Nonprecious transition metal phosphides (TMPs) have emerged as robust electrocalysts for the hydrogen evolution reaction (HER). However, the TMPs suffer from low activity for water dissociation, which greatly limits the efficiency for alkaline HER. Here, a facile yet robust strategy is reported to boost the HER of metal phosphides by coating defective TiO 2 overlayers. The oxygen vacancies (O v ) on defective TiO 2 overlayers are found to possess high activity for adsorption and dissociation of water, thereby significantly promoting the initial Volmer step of HER to generate the reactive hydrogen atoms. Moreover, the porous (Co, Ni) 2 P (i.e., Co 2 P and Ni 2 P) nanosheets provide enough active sites for adsorption and recombination of reactive hydrogen atoms to produce hydrogen gas. The catalytic synergy of (Co, Ni) 2 P and O v coupled with the hierarchically porous structure renders the porous (Co, Ni) 2 P@0.1TiO 2 nanosheet arrays excellent electrocatalysts for HER, showing a small overpotential (92 mV) to yield a current density of 10 mA cm −2 , a small Tafel slope (49 mV dec −1 ), and an outstanding stability. This work demonstrates a surface decoration route for enhancing the activity of nonprecious metal‐based electrocatalysts for HER.
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Liu et al. (2018) studied this question.