半离子型C-F优化了Rh/F， n共掺杂多孔碳的金属负载相互作用，以实现高效的全ph制氢

IF 17.1 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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引用次数: 0

摘要

在不同的pH条件下，设计高效、稳定、具有强金属-载体相互作用的rh基析氢反应电催化剂具有重要的意义和挑战性。本文采用水凝胶密封-热解-蚀刻策略将超细Rh纳米颗粒（Rh NPs）锚定在n掺杂多孔碳（Rh/NPC）上，进一步引入强电负性F掺杂剂来加强金属-载体相互作用，从而获得高电活性Rh NPs/ F， n共掺杂多孔碳复合材料（Rh/FNPC）。最佳的8Rh/FNPC在1 M KOH （η10 = 12 mV）、0.5 M H2SO4 （η10 = 42 mV）和1 M磷酸盐缓冲溶液（η10 = 64 mV）中具有超低过电位。密度泛函理论（DFT）模拟表明，F掺杂剂可以优化反应中间体的吸附自由能，加快反应在Rh活性位点上的速率决定步骤，从而获得较高的本征活性和优异的Rh/FNPC电活性。本研究为构建各种催化应用的高级催化剂提供了新的视角和途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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

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

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.