Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential
Abstract Effective hydrogen evolution reaction (HER) under high current density and enhanced hydrogen oxidation reaction (HOR) over a wide potential range remain challenges for Ru‐based electrocatalysts because its strong affinity to the adsorbed hydroxyl (OHad) inhibits the supply of the adsorbed h...
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2024-12-01
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Online Access: | https://doi.org/10.1002/advs.202410881 |
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author | Luyun Chen Chunlei Li Mengling Liu Ziruo Dai Haibin Wang Xuan Zhou Qiuping Zhao Yuanyuan Cong |
author_facet | Luyun Chen Chunlei Li Mengling Liu Ziruo Dai Haibin Wang Xuan Zhou Qiuping Zhao Yuanyuan Cong |
author_sort | Luyun Chen |
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description | Abstract Effective hydrogen evolution reaction (HER) under high current density and enhanced hydrogen oxidation reaction (HOR) over a wide potential range remain challenges for Ru‐based electrocatalysts because its strong affinity to the adsorbed hydroxyl (OHad) inhibits the supply of the adsorbed hydrogen (Had). Herein, the coexisting Ru─O─Ti and Ru─Ti bonds are constructed by taking TiO2 crystal confined flat‐Ru clusters (F‐Ru@TiO2) to cope with above‐mentioned obstacles. The different electronegativity (χTi = 1.54 < χRu = 2.20< χO = 3.44) can endow Ti in Ru─O─Ti bonds with more positive charge and stabilize Ru of Ru–Ti bonds with the low‐valence. The strength of Ru─OHad is then weakened by the oxophilicity of positively charged Ti in Ru─O─Ti bonds and the stronger Ti─OHad bond could release active Ru, especially for low‐valence Ru in Ru─Ti bonds, to serve as exclusive Had sites. As expected, F─TiRu@TiO2 shows a low HER overpotential of 74 mV at 1000 mA cm−2 and an ultrahigh mass activity (j0,m) of 3155 A gRu−1 for HOR. More importantly, F─Ru@TiO2 can tolerate the HER current density of 1000 mA cm−2 for 100 h and the high anodic potential for HOR up to 0.5 V versus RHE. |
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language | English |
publishDate | 2024-12-01 |
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spelling | doaj-art-b43358d4cb4c46ab8b3b3f837d1aa8182024-12-27T13:00:47ZengWileyAdvanced Science2198-38442024-12-011148n/an/a10.1002/advs.202410881Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High PotentialLuyun Chen0Chunlei Li1Mengling Liu2Ziruo Dai3Haibin Wang4Xuan Zhou5Qiuping Zhao6Yuanyuan Cong7School of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaSchool of Petrochemical Technology Lanzhou University of Technology Lanzhou Gansu 730050 ChinaAbstract Effective hydrogen evolution reaction (HER) under high current density and enhanced hydrogen oxidation reaction (HOR) over a wide potential range remain challenges for Ru‐based electrocatalysts because its strong affinity to the adsorbed hydroxyl (OHad) inhibits the supply of the adsorbed hydrogen (Had). Herein, the coexisting Ru─O─Ti and Ru─Ti bonds are constructed by taking TiO2 crystal confined flat‐Ru clusters (F‐Ru@TiO2) to cope with above‐mentioned obstacles. The different electronegativity (χTi = 1.54 < χRu = 2.20< χO = 3.44) can endow Ti in Ru─O─Ti bonds with more positive charge and stabilize Ru of Ru–Ti bonds with the low‐valence. The strength of Ru─OHad is then weakened by the oxophilicity of positively charged Ti in Ru─O─Ti bonds and the stronger Ti─OHad bond could release active Ru, especially for low‐valence Ru in Ru─Ti bonds, to serve as exclusive Had sites. As expected, F─TiRu@TiO2 shows a low HER overpotential of 74 mV at 1000 mA cm−2 and an ultrahigh mass activity (j0,m) of 3155 A gRu−1 for HOR. More importantly, F─Ru@TiO2 can tolerate the HER current density of 1000 mA cm−2 for 100 h and the high anodic potential for HOR up to 0.5 V versus RHE.https://doi.org/10.1002/advs.202410881hydrogen energy conversioninterfacial Ru–O–Ti bondinterfacial Ru–Ti bondlattice confined Rusynergistic effect |
spellingShingle | Luyun Chen Chunlei Li Mengling Liu Ziruo Dai Haibin Wang Xuan Zhou Qiuping Zhao Yuanyuan Cong Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential Advanced Science hydrogen energy conversion interfacial Ru–O–Ti bond interfacial Ru–Ti bond lattice confined Ru synergistic effect |
title | Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential |
title_full | Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential |
title_fullStr | Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential |
title_full_unstemmed | Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential |
title_short | Confining Flat Ru Islands into TiO2 Lattice with the Coexisting Ru–O–Ti and Ru–Ti Bonds for Ultra‐Stable Hydrogen Evolution at Amperometric Current Density and Hydrogen Oxidation at High Potential |
title_sort | confining flat ru islands into tio2 lattice with the coexisting ru o ti and ru ti bonds for ultra stable hydrogen evolution at amperometric current density and hydrogen oxidation at high potential |
topic | hydrogen energy conversion interfacial Ru–O–Ti bond interfacial Ru–Ti bond lattice confined Ru synergistic effect |
url | https://doi.org/10.1002/advs.202410881 |
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