The Superaerophobic N‐Doped Carbon Nanocage with Hydrogen Spillover Effort for Enhanced Hydrogen Evolution

Abstract Under the high current density, the excessive strong adsorption of H* intermediates and H₂ accumulation the catalysts are the major obstacle to the industrial application of hydrogen evolation reaction (HER) catalysts. Herein, through experimental exploration, it is found that the superaerophobic Nitrogen (N)‐doped carbon material can promote the rapid release of H₂ and provide H* desorption site for the hydrogen spillover process, which makes it have great potential as the catalysts support for hydrogen spillover. Based on this discovery, this work develops the hydrogen spillover catalyst with electron‐rich Pt sites loaded on N‐doped carbon nanocage (N‐CNC) with adjustable work function. Through a series of comprehensive electrochemical tests, the existence of hydrogen spillover effort has been proved. Moreover, the in situ tests showed that pyrrolic‐N can activate adjacent carbon sites as the desorption sites for hydrogen spillover. The Pt@N‐1‐CNC with the minimum work function difference (ΔΦ) between Pt NPs and support shows superior hydrogen evolution performance, only needs overpotential of 12.2 mV to reach current density of 10 mA cm⁻², outstanding turnover frequency (TOF) (44.7 s⁻¹@100 mV) and superior durability under the 360 h durability tests at current density of 50 mA cm⁻².