{"title":"铁和氧空位共调吸附演化和点阵氧双路机制的水氧化。","authors":"Xiwen Tao, Li Hou, Xinyi Wang, Jing Jin, Huana Li, Faming Gao","doi":"10.1038/s41467-025-63844-x","DOIUrl":null,"url":null,"abstract":"<p><p>Conjointly activating metal and oxygen sites to trigger the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for balancing activity and stability in oxygen evolution reaction catalysts, yet confronting great challenges. Herein, we develop Fe species and oxygen vacancies co-regulated Ni-(oxy)hydroxide from the deep reconstruction of Fe-Ni<sub>2</sub>P/NiMoO<sub>4</sub> pre-catalyst achieving the adsorbate evolution and lattice oxygen dual-path mechanism. Experimental details and theoretical calculation analysis reveal the enhanced adsorbate evolution mechanism kinetics at the Ni sites via the co-regulation of Fe species and oxygen vacancies, while the Fe incorporation activates the O sites with preferable adsorption free energy for lattice oxygen mechanism intermediates. Benefiting from the dual-path mechanism, the activated catalyst affords an ampere-scale current density of 1.0 A cm<sup>-2</sup> at low overpotentials of 274.5 ± 4.2 and 299.1 ± 2.8 mV in alkaline freshwater and seawater, respectively, and maintains seawater electrocatalysis for 500 h in the anion exchange membrane water electrolysis. This work demonstrates a strategy to trigger the coupled mechanism for efficient and stable electrocatalytic water splitting under harsh conditions.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"16 1","pages":"8788"},"PeriodicalIF":15.7000,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Iron and oxygen vacancies co-modulated adsorption evolution and lattice oxygen dual-path mechanism for water oxidation.\",\"authors\":\"Xiwen Tao, Li Hou, Xinyi Wang, Jing Jin, Huana Li, Faming Gao\",\"doi\":\"10.1038/s41467-025-63844-x\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Conjointly activating metal and oxygen sites to trigger the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for balancing activity and stability in oxygen evolution reaction catalysts, yet confronting great challenges. Herein, we develop Fe species and oxygen vacancies co-regulated Ni-(oxy)hydroxide from the deep reconstruction of Fe-Ni<sub>2</sub>P/NiMoO<sub>4</sub> pre-catalyst achieving the adsorbate evolution and lattice oxygen dual-path mechanism. Experimental details and theoretical calculation analysis reveal the enhanced adsorbate evolution mechanism kinetics at the Ni sites via the co-regulation of Fe species and oxygen vacancies, while the Fe incorporation activates the O sites with preferable adsorption free energy for lattice oxygen mechanism intermediates. Benefiting from the dual-path mechanism, the activated catalyst affords an ampere-scale current density of 1.0 A cm<sup>-2</sup> at low overpotentials of 274.5 ± 4.2 and 299.1 ± 2.8 mV in alkaline freshwater and seawater, respectively, and maintains seawater electrocatalysis for 500 h in the anion exchange membrane water electrolysis. This work demonstrates a strategy to trigger the coupled mechanism for efficient and stable electrocatalytic water splitting under harsh conditions.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"16 1\",\"pages\":\"8788\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-10-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-63844-x\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-63844-x","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
联合激活金属和氧位点触发吸附质演化和晶格氧机制耦合路径有望平衡析氧反应催化剂的活性和稳定性,但面临着很大的挑战。本文通过对Fe- ni2p /NiMoO4预催化剂的深度重构,开发了Fe和氧空位共调控的Ni-(氧)氢氧化物,实现了吸附质演化和点阵氧双路机制。实验细节和理论计算分析表明,Fe和氧空位的共同调节增强了Ni位点上吸附物的演化机理动力学,而Fe的加入激活了O位点,对晶格氧机制中间体具有更好的吸附自由能。利用双路机制,活性催化剂在碱性淡水和海水中分别在274.5±4.2和299.1±2.8 mV的低过电位下提供1.0 A cm-2的安培级电流密度,并在阴离子交换膜电解中维持海水电催化500 h。这项工作展示了一种在恶劣条件下触发高效稳定电催化水分解耦合机制的策略。
Iron and oxygen vacancies co-modulated adsorption evolution and lattice oxygen dual-path mechanism for water oxidation.
Conjointly activating metal and oxygen sites to trigger the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for balancing activity and stability in oxygen evolution reaction catalysts, yet confronting great challenges. Herein, we develop Fe species and oxygen vacancies co-regulated Ni-(oxy)hydroxide from the deep reconstruction of Fe-Ni2P/NiMoO4 pre-catalyst achieving the adsorbate evolution and lattice oxygen dual-path mechanism. Experimental details and theoretical calculation analysis reveal the enhanced adsorbate evolution mechanism kinetics at the Ni sites via the co-regulation of Fe species and oxygen vacancies, while the Fe incorporation activates the O sites with preferable adsorption free energy for lattice oxygen mechanism intermediates. Benefiting from the dual-path mechanism, the activated catalyst affords an ampere-scale current density of 1.0 A cm-2 at low overpotentials of 274.5 ± 4.2 and 299.1 ± 2.8 mV in alkaline freshwater and seawater, respectively, and maintains seawater electrocatalysis for 500 h in the anion exchange membrane water electrolysis. This work demonstrates a strategy to trigger the coupled mechanism for efficient and stable electrocatalytic water splitting under harsh conditions.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.