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      The synergistic effect of Hf-O-Ru bonds and oxygen vacancies in Ru/HfO 2 for enhanced hydrogen evolution

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          Abstract

          Ru nanoparticles have been demonstrated to be highly active electrocatalysts for the hydrogen evolution reaction (HER). At present, most of Ru nanoparticles-based HER electrocatalysts with high activity are supported by heteroatom-doped carbon substrates. Few metal oxides with large band gap (more than 5 eV) as the substrates of Ru nanoparticles are employed for the HER. By using large band gap metal oxides substrates, we can distinguish the contribution of Ru nanoparticles from the substrates. Here, a highly efficient Ru/HfO 2 composite is developed by tuning numbers of Ru-O-Hf bonds and oxygen vacancies, resulting in a 20-fold enhancement in mass activity over commercial Pt/C in an alkaline medium. Density functional theory (DFT) calculations reveal that strong metal-support interaction via Ru-O-Hf bonds and the oxygen vacancies in the supported Ru samples synergistically lower the energy barrier for water dissociation to improve catalytic activities.

          Abstract

          Although ruthenium nanomaterials have proven to be effective catalysts for H 2 evolution, there is still room for activity improvements. Here, authors develop an efficient Ru/HfO 2 electrocatalyst with tuned Ru-O-Hf bonds and oxygen vacancies that shows high activities for alkaline H 2 evolution.

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          Towards the computational design of solid catalysts.

          J K Nørskov, T Bligaard, J Rossmeisl … (2009)
          Over the past decade the theoretical description of surface reactions has undergone a radical development. Advances in density functional theory mean it is now possible to describe catalytic reactions at surfaces with the detail and accuracy required for computational results to compare favourably with experiments. Theoretical methods can be used to describe surface chemical reactions in detail and to understand variations in catalytic activity from one catalyst to another. Here, we review the first steps towards using computational methods to design new catalysts. Examples include screening for catalysts with increased activity and catalysts with improved selectivity. We discuss how, in the future, such methods may be used to engineer the electronic structure of the active surface by changing its composition and structure.
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            High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst.

            Yan Jiao, Ying Chen, Yao Zheng … (2016)
            Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.
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              Correlating the hydrogen evolution reaction activity in alkaline electrolytes with the hydrogen binding energy on monometallic surfaces

              Wenchao Sheng, Yushan Yan, Jingguang G Chen … (2013)
              Article 0 comments Cited 237 times – based on 0 reviews     Review now
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                Author and article information

                Contributors
                Qing Qin:
                ORCID: http://orcid.org/0000-0003-3204-924X
                qinqing@qust.edu.cn
                Xien Liu:
                ORCID: http://orcid.org/0000-0002-4947-0631
                liuxien@qust.edu.cn
                Jaephil Cho:
                ORCID: http://orcid.org/0000-0002-3890-1432
                jpcho@unist.ac.kr
                Journal
                Journal ID (nlm-ta): Nat Commun
                Journal ID (iso-abbrev): Nat Commun
                Title: Nature Communications
                Publisher: Nature Publishing Group UK (London )
                ISSN (Electronic): 2041-1723
                Publication date (Electronic): 11 March 2022
                Publication date PMC-release: 11 March 2022
                Publication date Collection: 2022
                Volume: 13
                Electronic Location Identifier: 1270
                Affiliations
                [1 ]GRID grid.412610.0, ISNI 0000 0001 2229 7077, College of Chemical Engineering, , Qingdao University of Science and Technology, ; Qingdao, China
                [2 ]GRID grid.42687.3f, ISNI 0000 0004 0381 814X, Department of Energy Engineering, Department of Energy and Chemical Engineering, , Ulsan National Institute of Science and Technology (UNIST), ; Ulsan, South Korea
                [3 ]GRID grid.35030.35, ISNI 0000 0004 1792 6846, Department of Chemistry, , City University of Hong Kong, ; Hong Kong, China
                [4 ]GRID grid.49100.3c, ISNI 0000 0001 0742 4007, Beamline Research Division, Pohang Accelerator Laboratory (PAL), ; Pohang, South Korea
                Author information
                http://orcid.org/0000-0002-1301-8627
                http://orcid.org/0000-0002-2366-6898
                http://orcid.org/0000-0003-3204-924X
                http://orcid.org/0000-0002-4947-0631
                http://orcid.org/0000-0002-3890-1432
                Article
                Publisher ID: 28947
                DOI: 10.1038/s41467-022-28947-9
                PMC ID: 8917135
                PubMed ID: 35277494
                SO-VID: 17ec04c7-c6ae-4b9f-8945-f20dc5b0e684
                Copyright © © The Author(s) 2022
                License:

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                Date received : 15 July 2021
                Date accepted : 15 February 2022
                Categories
                Subject: Article
                Custom metadata
                issue-copyright-statement © The Author(s) 2022

                ScienceOpen disciplines: Uncategorized
                Keywords: hydrogen energy,materials for energy and catalysis,electrocatalysis
                Data availability:
                ScienceOpen disciplines: Uncategorized
                Keywords: hydrogen energy, materials for energy and catalysis, electrocatalysis

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