Hard Lewis acid induced chloride repulsion for durable neutral seawater electrolysis

IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Suyang Feng , Gai Li , Qingyi Wei , Tianjiao Wang , Yingjie Hua , Jing Li , Wenyu Wang , Peng Ling , Daoxiong Wu , Yuliang Yuan , Xinlong Tian , Zhenye Kang
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Abstract

The development of efficient and stable catalysts for the neutral seawater oxygen evolution reaction (OER) is essential for sustainable hydrogen production; however, the competitive chlorine evolution reaction (CER) poses a critical challenge. Herein, nanosheet-like RuO₂@Nb₂O₅ catalysts are constructed and applied to repel Cl⁻ in seawater based on the Lewis acid-base theory. Experiments combined with density functional calculations reveal that Nb₂O₅ as a hard Lewis acid is able to promote the decomposition of H₂O molecules, and the in-situ generated OH⁻ layer significantly reduces Cl⁻ interaction. Notably, Nb₂O₅ also modulates the electronic structure of RuO₂, weakening Cl⁻ adsorption and shifting the OER pathway from the lattice oxygen mechanism to the more stable adsorbate evolution mechanism. After electrolysis for the same duration, the concentration of ClO⁻ in the electrolyte of RuO₂@Nb₂O₅ is approximately one magnitude lower than that of commercial RuO₂. The obtained RuO₂@Nb₂O₅ shows impressive OER activity in neutral seawater (pH ≈ 7.8) and displays considerable durability for up to 100 h.

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来源期刊
Nano Energy
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.
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