{"title":"超临界二氧化碳在Ru/MoSe2中引入了2H到1T的相变,增强了析氢性能","authors":"Haowen Lei, Pengfei Yan, Heng Lu, Tianpei Ge, Weiqian Kong, Xiaoli Zheng, Mengdi An, Qun Xu","doi":"10.1021/acssuschemeng.5c02269","DOIUrl":null,"url":null,"abstract":"The development of highly efficient hydrogen evolution reaction (HER) catalysts for water splitting is one of the most promising strategies to achieve peak CO<sub>2</sub> emission and carbon neutrality targets. In this study, we demonstrate a supercritical carbon dioxide (SC CO<sub>2</sub>)-assisted phase transition strategy to engineer metastable 1T phase Ru/MoSe<sub>2</sub> from its 2H phase counterpart. Experimental and theoretical results reveal that the incorporation of Ru significantly lowered the kinetic energy barrier of the 2H → 1T phase transition, while the introduction of SC CO<sub>2</sub> provides additional support for the long-term stability of the 1T phase, thus facilitating the phase transition of MoSe<sub>2</sub>. The synergistic combination of Ru’s exceptional water dissociation capability and the superior intrinsic conductivity and catalytic efficiency of 1T-MoSe<sub>2</sub> creates an optimized electronic structure that significantly enhances HER kinetics. Specifically, the optimized SC Ru/MoSe<sub>2</sub> exhibits remarkable catalytic performance, achieving an ultralow overpotential of 52 mV at 10 mA cm<sup>–2</sup> with a Tafel slope of 32 mV dec<sup>–1</sup> in 1 M KOH, overperforming commercial Pt/C benchmarks.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"43 1","pages":""},"PeriodicalIF":7.3000,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Supercritical Carbon Dioxide Introduced a 2H to 1T Phase Transition in Ru/MoSe2 with Enhanced Hydrogen Evolution Performance\",\"authors\":\"Haowen Lei, Pengfei Yan, Heng Lu, Tianpei Ge, Weiqian Kong, Xiaoli Zheng, Mengdi An, Qun Xu\",\"doi\":\"10.1021/acssuschemeng.5c02269\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The development of highly efficient hydrogen evolution reaction (HER) catalysts for water splitting is one of the most promising strategies to achieve peak CO<sub>2</sub> emission and carbon neutrality targets. In this study, we demonstrate a supercritical carbon dioxide (SC CO<sub>2</sub>)-assisted phase transition strategy to engineer metastable 1T phase Ru/MoSe<sub>2</sub> from its 2H phase counterpart. Experimental and theoretical results reveal that the incorporation of Ru significantly lowered the kinetic energy barrier of the 2H → 1T phase transition, while the introduction of SC CO<sub>2</sub> provides additional support for the long-term stability of the 1T phase, thus facilitating the phase transition of MoSe<sub>2</sub>. The synergistic combination of Ru’s exceptional water dissociation capability and the superior intrinsic conductivity and catalytic efficiency of 1T-MoSe<sub>2</sub> creates an optimized electronic structure that significantly enhances HER kinetics. Specifically, the optimized SC Ru/MoSe<sub>2</sub> exhibits remarkable catalytic performance, achieving an ultralow overpotential of 52 mV at 10 mA cm<sup>–2</sup> with a Tafel slope of 32 mV dec<sup>–1</sup> in 1 M KOH, overperforming commercial Pt/C benchmarks.\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"43 1\",\"pages\":\"\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2025-06-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acssuschemeng.5c02269\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acssuschemeng.5c02269","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
开发高效析氢反应(HER)水裂解催化剂是实现二氧化碳峰值排放和碳中和目标的最有前途的策略之一。在这项研究中,我们展示了一种超临界二氧化碳(SC CO2)辅助相变策略,从2H相的对应物中设计出亚稳的1T相Ru/MoSe2。实验和理论结果表明,Ru的加入显著降低了2H→1T相变的动能势垒,而SC CO2的引入为1T相的长期稳定性提供了额外的支持,从而促进了MoSe2的相变。钌优异的水解离能力与1T-MoSe2优异的固有电导率和催化效率的协同结合,创造了优化的电子结构,显著提高了HER动力学。具体而言,优化后的SC Ru/MoSe2表现出卓越的催化性能,在10 mA cm-2下实现了52 mV的超低过电位,在1 M KOH下的Tafel斜率为32 mV / dec1,优于商业Pt/C基准。
Supercritical Carbon Dioxide Introduced a 2H to 1T Phase Transition in Ru/MoSe2 with Enhanced Hydrogen Evolution Performance
The development of highly efficient hydrogen evolution reaction (HER) catalysts for water splitting is one of the most promising strategies to achieve peak CO2 emission and carbon neutrality targets. In this study, we demonstrate a supercritical carbon dioxide (SC CO2)-assisted phase transition strategy to engineer metastable 1T phase Ru/MoSe2 from its 2H phase counterpart. Experimental and theoretical results reveal that the incorporation of Ru significantly lowered the kinetic energy barrier of the 2H → 1T phase transition, while the introduction of SC CO2 provides additional support for the long-term stability of the 1T phase, thus facilitating the phase transition of MoSe2. The synergistic combination of Ru’s exceptional water dissociation capability and the superior intrinsic conductivity and catalytic efficiency of 1T-MoSe2 creates an optimized electronic structure that significantly enhances HER kinetics. Specifically, the optimized SC Ru/MoSe2 exhibits remarkable catalytic performance, achieving an ultralow overpotential of 52 mV at 10 mA cm–2 with a Tafel slope of 32 mV dec–1 in 1 M KOH, overperforming commercial Pt/C benchmarks.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.