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

IF 16.8 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Nano Energy Pub Date : 2025-04-06 DOI:10.1016/j.nanoen.2025.110975

Jian Guo, Rui Ding, Yi Li, Yiqing Lu, Ziyang Yan, Zhiqiang Chen, Yuming He, Qingcheng Yang, Xinchang Guo, Yibo Zhang, Jiajie Luo

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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 (η₁₀ = 12 mV), 0.5 _M H₂SO₄ (η₁₀ = 42 mV), and 1 _M phosphate buffer solution (η₁₀ = 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.

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来源期刊

Nano Energy CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

30.30

自引率

7.40%

发文量

1207

审稿时长

23 days

期刊介绍： Nano Energy is a multidisciplinary, rapid-publication forum of original peer-reviewed contributions on the science and engineering of nanomaterials and nanodevices used in all forms of energy harvesting, conversion, storage, utilization and policy. Through its mixture of articles, reviews, communications, research news, and information on key developments, Nano Energy provides a comprehensive coverage of this exciting and dynamic field which joins nanoscience and nanotechnology with energy science. The journal is relevant to all those who are interested in nanomaterials solutions to the energy problem. Nano Energy publishes original experimental and theoretical research on all aspects of energy-related research which utilizes nanomaterials and nanotechnology. Manuscripts of four types are considered: review articles which inform readers of the latest research and advances in energy science; rapid communications which feature exciting research breakthroughs in the field; full-length articles which report comprehensive research developments; and news and opinions which comment on topical issues or express views on the developments in related fields.