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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Main Authors: Luyun Chen, Chunlei Li, Mengling Liu, Ziruo Dai, Haibin Wang, Xuan Zhou, Qiuping Zhao, Yuanyuan Cong
Format: Article
Language:English
Published: Wiley 2024-12-01
Series:Advanced Science
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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
collection DOAJ
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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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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