Semi‐Ionic F Modified N‐Doped Porous Carbon Implanted with Ruthenium Nanoclusters toward Highly Efficient pH‐Universal Hydrogen Generation

作者：Jian Guo, Rui Ding, Yi Li, Jinmei Xie, Qi Fang, Miao Yan, Yuzhen Zhang, Ziyang Yan, Zhiqiang Chen, Yuming He, Xiujuan Sun, Enhui Liu · 发表于：Small · 年份：2024 · DOI：10.1002/smll.202403151 · 被引用次数：14 · 研究领域：Electrocatalysts for Energy Conversion、Hydrogen Storage and Materials、Advanced battery technologies research

Abstract Developing high electroactivity ruthenium (Ru)‐based electrocatalysts for pH‐universal hydrogen evolution reaction (HER) is challenging due to the strong bonding strengths of key Ru─H/Ru─OH intermediates and sluggish water dissociation rates on active Ru sites. Herein, a semi‐ionic F‐modified N‐doped porous carbon implanted with ruthenium nanoclusters (Ru/FNPC) is introduced by a hydrogel sealing‐pyrolying‐etching strategy toward highly efficient pH‐universal hydrogen generation. Benefiting from the synergistic effects between Ru nanoclusters (Ru NCs) and hierarchically F, N‐codoped porous carbon support, such synthesized catalyst displays exceptional HER reactivity and durability at all pH levels. The optimal 8Ru/FNPC affords ultralow overpotentials of 17.8, 71.2, and 53.8 mV at the current density of 10 mA cm −2 in alkaline, neutral, and acidic media, respectively. Density functional theory (DFT) calculations elucidate that the F‐doped substrate to support Ru NCs weakens the adsorption energies of H and OH on Ru sites and reduces the energy barriers of elementary steps for HER, thus enhancing the intrinsic activity of Ru sites and accelerating the HER kinetics. This work provides new perspectives for the design of advanced electrocatalysts by porous carbon substrate implanted with ultrafine metal NCs for energy conversion applications.