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Optimizing Hydrogen Binding on Ru Sites with RuCo Alloy Nanosheets for Efficient Alkaline Hydrogen Evolution
Open accessAbstract
Ruthenium (Ru)‐based catalysts, with considerable performance and desirable cost, are becoming highly interesting candidates to replace platinum (Pt) in the alkaline hydrogen evolution reaction (HER). The hydrogen binding at Ru sites (Ru−H) is an important factor limiting the HER activity. Herein, density functional theory (DFT) simulations show that the essence of Ru−H binding energy is the strong interaction between the orbital of Ru and the 1s orbital of H. The charge transfer between Ru sites and substrates (Co and Ni) causes the appropriate downward shift of the ‐band center of Ru, which results in a Gibbs free energy of 0.022 eV for H* in the RuCo system, much lower than the 0.133 eV in the pure Ru system. This theoretical prediction has been experimentally confirmed using RuCo alloy‐nanosheets (RuCo ANSs). They were prepared via a fast co‐precipitation method followed with a mild electrochemical reduction. Structure characterizations reveal that the Ru atoms are embedded into the Co substrate as isolated active sites with a planar symmetric and Z‐direction asymmetric coordination structure, obtaining an optimal modulated electronic structure. Hydrogen sensor and temperature program desorption (TPD) tests demonstrate the enhanced Ru−H interactions in RuCo ANSs compared to those in pure Ru nanoparticles. As a result, the RuCo ANSs reach an ultra‐low overpotential of 10 mV at 10 mA cm −2 and a Tafel slope of 20.6 mV dec −1 in 1 M KOH, outperforming that of the commercial Pt/C. This holistic work provides a new insight to promote alkaline HER by optimizing the metal‐H binding energy of active sites.
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“traditional supports on the micrometer scale are usually not compatible with the catalysts on the nanoscale and therefore do not contribute considerably to the intrinsic catalytic activity.”
From An energy-saving support made of silver nanowire aerogel for hydrogen evolution reaction (2023) · cites this paper as [31]
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Recent Advances in Electrocatalytic Hydrogen Evolution Using Nanoparticles
Zhu, J., Hu, L., Zhao, P., Lee, L. Y. S., & Wong, K.-Y. (2020) · Chemical Reviews · doi:10.1021/acs.chemrev.9b00248 · Cited by 3,133
High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst
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Self-citationSu, J., Yang, Y., Xia, G., Chen, J., Jiang, P., & Chen, Q. (2017) · Nature Communications · doi:10.1038/ncomms14969 · Cited by 845
Recent Advances and Prospective in Ruthenium-Based Materials for Electrochemical Water Splitting
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Self-citationUltrahigh-Loading of Ir Single Atoms on NiO Matrix to Dramatically Enhance Oxygen Evolution Reaction
Wang, Q., Huang, X., Zhao, Z. L., Wang, M., Xiang, B., Li, J., Feng, Z., Xu, H., & Gu, M. D. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.9b12642 · Cited by 663
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Metadata
- Authors
- Cai, C., Liu, K., Zhu, Y., Li, P., Wang, Q., Liu, B., Chen, S., Li, H., Zhu, L., Li, H., Fu, J., Chen, Y., Pensa, E., Hu, J., Lu, Y., Chan, T., Cortés, E., & Liu, M.
- Affiliations
- Central South University (CN)
- Southern University of Science and Technology (CN)
- Ludwig-Maximilians-Universität München (DE)
- Zhengzhou University (CN)
- National Synchrotron Radiation Research Center (TW)
- Corresponding author
- Cortés, Emiliano
- Liu, Min
- ORCID
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2021-12-07
- Volume
- 61
- Issue
- 4
- Pages
- e202113664-e202113664
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- PMC
- PMC9300137
- OpenAlex
- W3217607620
- Cited by
- 213
- References
- 60
- Citations by year
- 2026: 32 · 2025: 40 · 2024: 43 · 2023: 54 · 2022: 43 · 2021: 1
- FWCI
- 6.61
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Angewandte Chemie International Edition (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- Spiral (Imperial College London) (submittedVersion, cc-by)
- Funders
- European Commission (ERC-STG 802989)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- alkaline hydrogen evolution reaction, ruthenium catalysts, metal-hydrogen interaction, charge transfer, band center shift, platinum-free electrocatalysts, co-precipitation synthesis, electrochemical reduction, hydrogen adsorption, overpotential
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