材料科学
催化作用
兴奋剂
氢
分解水
化学工程
碱土金属
无机化学
纳米技术
冶金
有机化学
金属
光电子学
光催化
化学
工程类
作者
Jingwen Yin,Tingyu Lu,Jing Li,Jiayi Liu,Yingzi Lin,Dongmei Sun,Lin Xu,Qun Zhao,Huan Pang,Songtao Zhang,Yawen Tang
标识
DOI:10.1002/adfm.202417034
摘要
Abstract The rational design of single atom‐based catalysts and precise elucidation of the synergistic interaction between the metal site and substrate are pivotal to identifying the real active sites and explicating the catalytic mechanisms at the atomic scale, thus contributing to the development of high‐performance catalysts for diverse industrial implementations. Herein, a Ru single‐atom doping strategy is developed to activate the MoC substrate with superior hydrogen evolution reaction (HER) activity in an alkaline medium. The atomically dispersed Ru sites are elaborately doped into MoC nanoparticles loaded on 3D N‐doped carbon nanoflowers (Ru‐SAs@MoC/NCFs hereafter). The experimental results and theoretical calculations manifest that the atomically isolated Ru dopants can effectively trigger the Mo sites with thermodynamically favorable water adsorption/dissociation energies and facilitate the OH − desorption on Ru sites and H adsorption on N sites, thus synergistically expediating the overall alkaline HER kinetics. As such, the well‐designed Ru‐SAs@MoC/NCFs demonstrate extraordinary HER activity with a low overpotential of 16 mV at 10 mA cm −2 in 1.0 m KOH electrolyte, outperforming Pt/C benchmark and a vast of molybdenum/ruthenium‐based HER catalysts reported to date. These findings disclose the alkaline HER mechanistic induced by the atomic doping modulation and suggest a design principle of high‐efficiency electrocatalysts via the atomic‐level manipulation leverage.
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