Modulating Hydrogen Adsorption via Charge Transfer at the Semiconductor–Metal Heterointerface for Highly Efficient Hydrogen Evolution Catalysis
Abstract
Designing and synthesizing highly efficient and stable electrocatalysts for hydrogen evolution reaction (HER) is important for realizing the hydrogen economy. Tuning the electronic structure of the electrocatalysts is essential to achieve optimal HER activity, and interfacial engineering is an effective strategy to induce electron transfer in a heterostructure interface to optimize HER kinetics. In this study, ultrafine RhP 2 /Rh nanoparticles are synthesized with a well-defined semiconductor-metal heterointerface embedded in N,P co-doped graphene (RhP 2 /Rh@NPG) via a one-step pyrolysis. RhP 2 /Rh@NPG exhibits outstanding HER performances under all pH conditions. Electrochemical characterization and first principles density functional theory calculations reveal that the RhP 2 /Rh heterointerface induces electron transfer from metallic Rh to semiconductive RhP 2 , which increases the electron density on the Rh atoms in RhP 2 and weakens the hydrogen adsorption on RhP 2 , thereby accelerating the HER kinetics. Moreover, the interfacial electron transfer activates the dual-site synergistic effect of Rh and P of RhP 2 in neutral and alkaline environments, thereby promoting reorganization of interfacial water molecules for faster HER kinetics.
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Metallic Rh species are present in Co AG-Rh500.
“As for the Rh 3d core spectrum (Fig. 2d), the binding energies of 307.2 eV and 311.9 eV are attributed to Rh0 3d5/2 and Rh0 3d3/2, respectively, which suggests the presence of metallic Rh species [44].”
From Better than Pt in all-pH media: A charge transfer modulating hydrogen adsorption in cobalt-rhodium alloy aerogel to boost hydrogen evolution (2023) · cites this paper as [44]
Cites
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Liu, X., Wang, X., Li, K., Tang, J., Zhu, J., Chi, J., Lai, J., & Wang, L. (2024) · Angewandte Chemie International Edition · doi:10.1002/anie.202316319 · Cited by 110 · see citing works
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- Authors
- Liu, Y., Ding, J., Li, F., Su, X., Zhang, Q., Guan, G., Hu, F., Zhang, J., Wang, Q., Jiang, Y., Liu, B., & Yang, H. B.
- Affiliations
- Chinese Academy of Sciences (CN)
- Nanyang Technological University (SG)
- Shenzhen University (CN)
- Suzhou University of Science and Technology (CN)
- Corresponding author
- Hu, Fangxin
- Liu, Bin
- Yang, Hong Bin
- ORCID
- Venue
- Advanced Materials
- Publisher
- Wiley
- Published
- 2022-12-03
- Volume
- 35
- Issue
- 1
- Pages
- e2207114-e2207114
- ISSN
- 0935-9648 (ISSN-L)
- 1521-4095
- OpenAlex
- W4303432692
- Cited by
- 193
- References
- 3
- Citations by year
- 2026: 30 · 2025: 60 · 2024: 57 · 2023: 46
- FWCI
- 7.34
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Advanced Materials (publishedVersion)
- PubMed (publishedVersion)
- DR-NTU (Nanyang Technological University) (submittedVersion)
- Funders
- National Natural Science Foundation of China (22075195)
- Agency for Science, Technology and Research (AME IRG A20E5c0080)
- Suzhou University of Science and Technology
- 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 › Advanced Photocatalysis Techniques
- Keywords
- hydrogen evolution reaction, electrocatalysts, interfacial electron transfer, hydrogen adsorption, rhodium nanoparticles, pyrolysis synthesis, electronic structure modulation
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