Work

Semi-ionic C-F optimizes metal-support interaction of Rh/F, N-codoped porous carbon for efficient all-pH hydrogen production

Year: 2025

Type: article

Abstract: Designing efficient and robust Rh-based electrocatalysts with strong metal-support interaction for hydrogen evolution reaction (HER) across various pH conditions is of great significance and challenge. Herein, a hydrogel sealing-pyrolyzing-etching strategy is engineered to anchor ultrafine Rh nanoparticles (Rh NPs) on N-doped porous carbon (Rh/NPC), further introducing strong electronegativity F-dopants to strengthen the metal-support interaction for obtaining high electroactivity Rh NPs/ F, N-codoped porous carbon composite (Rh/FNPC) toward HER. The optimal 8Rh/FNPC renders ultralow overpotentials in 1 M KOH (η 10 = 12 mV), 0.5 M H 2 SO 4 (η 10 = 42 mV), and 1 M phosphate buffer solution (η 10 = 64 mV). Density functional theory (DFT) simulations unveil that the F dopants can optimize the adsorption free energies of reaction intermediates and accelerate the rate-determining steps on the Rh active site, thereby achieving high intrinsic activity and exceptional electroactivity of Rh/FNPC. This work affords new perspectives and avenues for constructing advanced catalysts in various catalytic applications.

Source: Nano Energy

DOI: 10.1016/j.nanoen.2025.110975