Abstract
Catalytic performance can be greatly enhanced by rational modulation of thesurface state. In this study, reasonable adjustment of the surface states around the Fermi level (EF ) of molybdenum carbide (MoC) (α phase) via a Pt-N dual-doping process to fabricate an electrocatalyst named as Pt-N-MoC is performed to promote hydrogen evolution reaction (HER) performance over the MoC surface. Systematically experimental and theoretical analyses demonstrate that the synergistic tuning of Pt and N can cause the delocalization of surface states, with an increase in the density of surface states near the EF . This is beneficial for accumulating and transferring electrons between the catalyst surface and adsorbent, resulting in a positively linear correlation between the density of surface states near the EF and the HER activity. Moreover, the catalytic performance is further enhanced by artificially fabricating a Pt-N-MoC catalyst that has a unique hierarchical structure composed of MoC nanoparticles (0D), nanosheets (2D), and microrods (3D). As expected, the obtained Pt-N-MoC electrocatalyst exhibits superb HER activity with an extremely low overpotential of 39 mV@10mA cm-2 as well as superb stability (over 24 d) in an alkaline solution. This work highlights a novel strategy to develop efficient electrocatalysts via adjusting their surface states.
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