@article{Gao2026, 
author = {Yuanfeng Gao and Junyu Wang and Yusheng Yang and Liang Wu and Aimin Yu and Dong-sheng Li and Cunman Zhang and Chenghua Sun and Hong Lv},
title = {Superior activity hydrogen evolution enabled by interfacial water orientation and concerted proton–electron transfer},
year = {2026},
journal = {Nano Research},
volume = {19},
number = {9},
pages = {94908648},
keywords = {hydrogen bond network, concerted proton-electron transfer (CPET), interfacial water structure, interfacial solvation effect, high current density},
url = {https://www.sciopen.com/article/10.26599/NR.2026.94908648},
doi = {10.26599/NR.2026.94908648},
abstract = {Proton transfer (PT) at the catalyst-electrolyte interface is a fundamental step in the hydrogen evolution reaction (HER), yet its interfacial dynamics is poorly understood. Here, we report 15% Co/O-FeP supported on multiwalled carbon nanotubes (MWCNTs) as a highly efficient HER catalyst, delivering an overpotential of only 58 mV at 10 mA·cm−2 and sustaining 500 mA·cm−2 for over 111 h without noticeable degradation. Outstanding HER performance and high-current stability make industrial-level hydrogen evolution feasible. Using in-situ Raman spectroscopy and ab initio molecular dynamics (AIMD) simulations, we reveal that the orientation of interfacial water molecules, particularly interfacial H+ solvation effect induced by H-down configurations, governs HER kinetics by accelerating proton migration and enabling a concerted proton-electron transfer (CPET). Mechanically, PT proceeds through a two-step pathway: (i) Protons migrate from bulk solution to the electrical double layer (EDL) to form H3O+ and (ii) H3O+ undergoes rapid proton exchange with catalyst active sites. H-down water configurations within the inner Helmholtz plane (IHP) stabilizes de-solvation shells and couples efficiently with interfacial electrons, lowering kinetic barriers. These findings establish a direct correlation between interfacial water structure, hydrogen-bond network, and CPET efficiency, providing fundamental insights for the rational design of advanced electrocatalytic interfaces.}
}