{"title":"RuO2催化剂中Mn─O─Ru桥接基序在安培电流密度下促进制氢","authors":"Qiqi Li, Qiulin Xu, Zhenxin Pei, Zhixuan Zhang, Wenli Xu, Jiayao Mao, Qing Shang, Yongqiang Ni, Yifan Chen, Yongting Chen, Xinghui Liu, Xuanke Li, Qin Zhang, Nianjun Yang","doi":"10.1002/aenm.202500815","DOIUrl":null,"url":null,"abstract":"Accurately regulating the reactive sites of catalysts is vital for highly efficient catalytic processes but still faces considerable challenges. In view of this, a local oxidation‐state asymmetric Mn‐O‐Ru bridged moiety is developed by introducing Mn atoms into the RuO<jats:sub>2</jats:sub> host. The synergistic effect of the respective active sites on the Mn‐O‐Ru microstructure ensures its excellent alkaline HER performance. Theoretical calculations profiled that induced by the Mn‐O‐Ru bridged moiety, the water dissociation ability of Ru sites is significantly boosted, while the bridging oxygen exhibits the optimal hydrogen adsorption free energy. As predicted, the Mn‐RuO<jats:sub>2</jats:sub> catalyst achieved the overpotentials as low as 118 and 160 mV at the industrial level current densities of 1 and 2 A cm<jats:sup>‒2</jats:sup> in 1 <jats:sc>m</jats:sc> KOH, respectively, superior to the RuO<jats:sub>2</jats:sub> and commercial Pt/C catalyst. Such a Mn‐RuO<jats:sub>2</jats:sub> electrocatalyst can operate stably with a long lifetime of 300 h at 10 mA cm<jats:sup>‒2</jats:sup> under alkaline conditions. Furthermore, it only requires 1.87 V to reach the current density of 1.0 A cm<jats:sup>‒2</jats:sup> when serving as the cathode in an assembled flow cell. This work provides new insight into catalytic local environment design for obtaining ideal efficient HER electrocatalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"3 1","pages":""},"PeriodicalIF":24.4000,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Bridged Mn─O─Ru Motifs in RuO2 Catalyst Promoting Hydrogen Production at Ampere‐Level Current Density\",\"authors\":\"Qiqi Li, Qiulin Xu, Zhenxin Pei, Zhixuan Zhang, Wenli Xu, Jiayao Mao, Qing Shang, Yongqiang Ni, Yifan Chen, Yongting Chen, Xinghui Liu, Xuanke Li, Qin Zhang, Nianjun Yang\",\"doi\":\"10.1002/aenm.202500815\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Accurately regulating the reactive sites of catalysts is vital for highly efficient catalytic processes but still faces considerable challenges. In view of this, a local oxidation‐state asymmetric Mn‐O‐Ru bridged moiety is developed by introducing Mn atoms into the RuO<jats:sub>2</jats:sub> host. The synergistic effect of the respective active sites on the Mn‐O‐Ru microstructure ensures its excellent alkaline HER performance. Theoretical calculations profiled that induced by the Mn‐O‐Ru bridged moiety, the water dissociation ability of Ru sites is significantly boosted, while the bridging oxygen exhibits the optimal hydrogen adsorption free energy. As predicted, the Mn‐RuO<jats:sub>2</jats:sub> catalyst achieved the overpotentials as low as 118 and 160 mV at the industrial level current densities of 1 and 2 A cm<jats:sup>‒2</jats:sup> in 1 <jats:sc>m</jats:sc> KOH, respectively, superior to the RuO<jats:sub>2</jats:sub> and commercial Pt/C catalyst. Such a Mn‐RuO<jats:sub>2</jats:sub> electrocatalyst can operate stably with a long lifetime of 300 h at 10 mA cm<jats:sup>‒2</jats:sup> under alkaline conditions. Furthermore, it only requires 1.87 V to reach the current density of 1.0 A cm<jats:sup>‒2</jats:sup> when serving as the cathode in an assembled flow cell. This work provides new insight into catalytic local environment design for obtaining ideal efficient HER electrocatalysts.\",\"PeriodicalId\":111,\"journal\":{\"name\":\"Advanced Energy Materials\",\"volume\":\"3 1\",\"pages\":\"\"},\"PeriodicalIF\":24.4000,\"publicationDate\":\"2025-04-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/aenm.202500815\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/aenm.202500815","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
准确调节催化剂的活性位点对高效催化过程至关重要,但仍面临相当大的挑战。考虑到这一点,通过将Mn原子引入到RuO2宿主中,形成了局部氧化态的不对称Mn - O - Ru桥接部分。各活性位点对Mn - O - Ru微观结构的协同作用保证了其优异的碱性HER性能。理论计算表明,在Mn - O - Ru桥接部分的诱导下,Ru位点的水解离能力显著提高,而桥接氧表现出最佳的氢吸附自由能。正如预测的那样,在工业级电流密度为1和2 A cm-2、1 m KOH时,Mn - RuO2催化剂的过电位分别达到了118和160 mV,优于RuO2和商业Pt/C催化剂。这种Mn - RuO2电催化剂在碱性条件下,在10 mA cm-2下稳定运行,寿命长达300小时。此外,在组装液流电池中作为阴极时,只需要1.87 V就可以达到1.0 A cm-2的电流密度。本研究为获得理想高效的HER电催化剂提供了催化局部环境设计的新思路。
Bridged Mn─O─Ru Motifs in RuO2 Catalyst Promoting Hydrogen Production at Ampere‐Level Current Density
Accurately regulating the reactive sites of catalysts is vital for highly efficient catalytic processes but still faces considerable challenges. In view of this, a local oxidation‐state asymmetric Mn‐O‐Ru bridged moiety is developed by introducing Mn atoms into the RuO2 host. The synergistic effect of the respective active sites on the Mn‐O‐Ru microstructure ensures its excellent alkaline HER performance. Theoretical calculations profiled that induced by the Mn‐O‐Ru bridged moiety, the water dissociation ability of Ru sites is significantly boosted, while the bridging oxygen exhibits the optimal hydrogen adsorption free energy. As predicted, the Mn‐RuO2 catalyst achieved the overpotentials as low as 118 and 160 mV at the industrial level current densities of 1 and 2 A cm‒2 in 1 m KOH, respectively, superior to the RuO2 and commercial Pt/C catalyst. Such a Mn‐RuO2 electrocatalyst can operate stably with a long lifetime of 300 h at 10 mA cm‒2 under alkaline conditions. Furthermore, it only requires 1.87 V to reach the current density of 1.0 A cm‒2 when serving as the cathode in an assembled flow cell. This work provides new insight into catalytic local environment design for obtaining ideal efficient HER electrocatalysts.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.