Electronic Interaction Enables Pt Nanoparticles on N-Doped Porous Carbon Aerogel as Efficient Electrocatalysts for...

Alkaline water electrolysis for hydrogen evolution reaction (HER) with Pt-based electrocatalysts as the cathodes is still sluggish due to the unfavorable activation of water. Herein, the three-dimensional N-doped carbon aerogel (NCA) is adopted as the defect-rich support for uniform loading of ultra-fine Pt nanoparticles to prepare Pt/NCA for alkaline HER. Doping N into carbon aerogel (CA) promotes the strong electronic interaction between Pt nanoparticles and NCA, thus resulting in the electron transfer from Pt to NCA to optimize the free energy for hydrogen adsorption and facilitate the adsorption and dissociation of water. The hierarchical feature of NCA and electronic interaction enables the Pt/NCA to exhibit a smaller overpotential of 14.2 mV for the current density of 10 mA cm^-2 compared to Pt/CA. Additionally, the anion exchange membrane water electrolyzer with Pt/NCA as cathode can achieve an industrial-level current density of 1 A cm^-2 under 1.71 V and maintain stably over 200 h at 60 °C. This work suggests the efficient modulation in the heterogeneous interface between Pt and NCA support to benefit the water activation and thereafter enhance the alkaline HER for practical water electrolysis.