Revealing the role of interfacial water and key intermediates at ruthenium surfaces in the alkaline hydrogen evolution reaction
Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectr...
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| Published in | Nature communications Vol. 14; no. 1; pp. 5289 - 11 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
30.08.2023
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
| ISSN | 2041-1723 2041-1723 |
| DOI | 10.1038/s41467-023-41030-1 |
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| Abstract | Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na
+
ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts.
Here, the authors simultaneously capture dynamic Raman spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates, and the interactions between them, demonstrating the regulation of Ru valence state on interfacial water and intermediates for catalytic activity improvement. |
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| AbstractList | Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na
+
ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts. Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na + ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts. Here, the authors simultaneously capture dynamic Raman spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates, and the interactions between them, demonstrating the regulation of Ru valence state on interfacial water and intermediates for catalytic activity improvement. Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na+ ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts.Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na+ ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts. Abstract Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na+ ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts. Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be settled, which are elucidated by combining in situ Raman spectroscopy and theoretical calculations herein. We simultaneously capture dynamic spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates. Ru surfaces exist in different valence states in the reaction potential range, dissociating interfacial water differently and generating two distinct *H, resulting in different activities. The local cation tuning effect of hydrated Na+ ion water and the large work function of high-valence Ru(n+) surfaces promote interfacial water dissociation. Moreover, compared to low-valence Ru(0) surfaces, high-valence Ru(n+) surfaces have more moderate adsorption energies for interfacial water, *H, and *OH. They, therefore, facilitate the activity. Our findings demonstrate the regulation of valence state on interfacial water, intermediates, and finally the catalytic activity, which provide guidelines for the rational design of high-efficiency catalysts.Here, the authors simultaneously capture dynamic Raman spectral evidence of Ru surfaces, interfacial water, *H and *OH intermediates, and the interactions between them, demonstrating the regulation of Ru valence state on interfacial water and intermediates for catalytic activity improvement. |
| ArticleNumber | 5289 |
| Author | Radjenovic, Petar Wang, Xue Wang, Xiao-Ting Li, Shu-Min Zhao, Yu Zhang, Yu-Jin Le, Jia-Bo Chen, Xing Li, Jian-Feng Lin, Xiu-Mei Wang, Yao-Hui Dong, Jin-Chao |
| Author_xml | – sequence: 1 givenname: Xing surname: Chen fullname: Chen, Xing organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 2 givenname: Xiao-Ting surname: Wang fullname: Wang, Xiao-Ting organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 3 givenname: Jia-Bo surname: Le fullname: Le, Jia-Bo organization: Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences – sequence: 4 givenname: Shu-Min surname: Li fullname: Li, Shu-Min organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 5 givenname: Xue surname: Wang fullname: Wang, Xue organization: Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences – sequence: 6 givenname: Yu-Jin surname: Zhang fullname: Zhang, Yu-Jin organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 7 givenname: Petar surname: Radjenovic fullname: Radjenovic, Petar organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 8 givenname: Yu surname: Zhao fullname: Zhao, Yu organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 9 givenname: Yao-Hui surname: Wang fullname: Wang, Yao-Hui organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University – sequence: 10 givenname: Xiu-Mei orcidid: 0000-0001-9692-8855 surname: Lin fullname: Lin, Xiu-Mei email: xiu-mei.lin@xmu.edu.cn organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University, Department of Chemistry and Environment Science, Fujian Province University Key Laboratory of Analytical Science, Minnan Normal University – sequence: 11 givenname: Jin-Chao orcidid: 0000-0001-7776-6360 surname: Dong fullname: Dong, Jin-Chao email: jcdong@xmu.edu.cn organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM) – sequence: 12 givenname: Jian-Feng orcidid: 0000-0003-1598-6856 surname: Li fullname: Li, Jian-Feng email: Li@xmu.edu.cn organization: College of Energy, College of Chemistry and Chemical Engineering, College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Xiamen University, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM) |
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| Snippet | Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to be... Abstract Ruthenium exhibits comparable or even better alkaline hydrogen evolution reaction activity than platinum, however, the mechanistic aspects are yet to... |
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| SubjectTerms | 140/133 639/638/161 639/638/161/886 639/638/542/969 Adsorption Catalysis Catalysts Catalytic activity Chemistry Electrolytes Electrons Humanities and Social Sciences Hydrogen Hydrogen evolution reactions Intermediates Laboratories multidisciplinary Nanoparticles Raman spectroscopy Ruthenium Science Science (multidisciplinary) Valence Work functions |
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| Title | Revealing the role of interfacial water and key intermediates at ruthenium surfaces in the alkaline hydrogen evolution reaction |
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