Cited by 547Electrocatalysts for Energy ConversionCatalytic Processes in Materials ScienceCO2 Reduction Techniques and Catalysts

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Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation

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Wang, Yi, Yang, Rong, Ding, Yajun, Zhang, Bo, Li, Hao, Bai, Bing, Li, Mingrun, Cui, Yi, Xiao, Jianping, Wu, Zhong-Shuai·2023·Nature Communications

DOI 10.1038/s41467-023-37008-8PMC PMC10015077

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Abstract

Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance for H 2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy of Rh doping and surface oxygen vacancies to precisely regulate unconventional OER reaction path via the Ru–O–Rh active sites of Rh-RuO 2 , simultaneously boosting intrinsic activity and stability. The stabilized low-valent catalyst exhibits a remarkable performance, with an overpotential of 161 mV at 10 mA cm −2 and activity retention of 99.2% exceeding 700 h at 50 mA cm −2 . Quasi in situ/operando characterizations demonstrate the recurrence of reversible oxygen species under working potentials for enhanced activity and durability. It is theoretically revealed that Rh-RuO 2 passes through a more optimal reaction path of lattice oxygen mediated mechanism-oxygen vacancy site mechanism induced by the synergistic interaction of defects and Ru–O–Rh active sites with the rate-determining step of *O formation, breaking the barrier limitation (*OOH) of the traditional adsorption evolution mechanism.

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Fig. 1 Synthesis and morphology characterization of Rh-RuO2/G nanosheets. a Preparation schematic. b SEM image. c TEM image. d HAADF-STEM image (inset shows the SEAD pattern). e, f AFM image (e) and corresponding height profiles (f). g Elemental mapping analysis of Rh-RuO2/G.CC BY · PubMed Central

Fig. 2 Compositional structure analysis of Rh-RuO2/G nanosheets. a XRD pattern of Rh-RuO2/G. b Raman spectra, c O 1s XPS spectra, and d H2-TPR spectra of Rh-RuO2/G and RuO2/G. e Ru K-edge XANES spectra and f Fourier transformed EXAFS spectra of Ru-edge for Rh-RuO2/G, RuO2/G, Ru foil, RuCl3 solution, and commercial RuO2.CC BY · PubMed Central

Fig. 3 Electrocatalytic performance of Rh-RuO2/G, RuO2/G, and commercial RuO2 catalysts in 0.5 M H2SO4 solution with 95% iR compensation. a LSV polarization curves. b Overpotentials at a current density of 10 mA cm−2 and 100 mA cm−2. c Tafel plots. d The TOF curve of Rh-RuO2/G compared with reported representative catalysts. e The galvanostatic curves at a current density of 10 mA cm−2 and 50 mA cm−2.CC BY · PubMed Central

Fig. 4 Quasi in situ NAP-XPS, ex-situ XAFS, and operando DEMS measurements probing dynamic evolution of electronic structure on Rh-RuO2/G catalyst during OER reaction. a, b The quasi in situ O 1s (a) and Ru 3p3/2 (b) XPS spectra recorded of the resultant Rh-RuO2/G during the multipotential steps. c Variation of OV/OL ratio from quasi in situ XPS measurement. d Ex-situ XANES spectra for Rh-RuO2/G and RuO2/G at 1.5 V for 8 h during OER. Inset: magnified pre-edge XANES region. e DEMS signals of 36O2, 34O2, and 32O2 for Rh-RuO2/G in H218O aqueous sulfuric acid electrolyte within four times of LSV at 1.1–1.9 V (vs. RHE).CC BY · PubMed Central

Fig. 5 DFT calculation of the OER reaction mechanism to elucidate intrinsic activity and stability of Rh-RuO2. a–c A two-dimensional activity map for AEM mechanism (a), LOM-OVSM mechanism (b), and LOM-SMSM (c) mechanism based on OER. The adsorption energies of *OH (*OH_OV or *OH_SM) and *O (*O_OV or *O_SM) are applied to be two independent descriptors. A 0.2 eV error bar is shown to describe the theoretical uncertainty. d Comparisons between calculated overpotential and experiment overpotential relationship. e A two-dimensional stability map for d and d-OV. f Charge density difference analysis for d and d-OV slab.CC BY · PubMed Central

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Authors: Wang, Y., Yang, R., Ding, Y., Zhang, B., Li, H., Bai, B., Li, M., Cui, Y., Xiao, J., & Wu, Z.-S.
Affiliations: Dalian Institute of Chemical Physics (CN)
Tianjin University (CN)
University of Science and Technology of China (CN)
Corresponding author: Xiao, Jianping
Wu, Zhong-Shuai
ORCID: Wang, Yi
Yang, Rong
Ding, Yajun
Zhang, Bo
Bai, Bing
Cui, Yi
Xiao, Jianping
Wu, Zhong-Shuai
Venue: Nature Communications
Publisher: Springer Science and Business Media LLC
Published: 2023-03-14
Volume: 14
Issue: 1
Pages: 1412-1412
ISSN: 2041-1723 (ISSN-L)
DOI: 10.1038/s41467-023-37008-8
PMC: PMC10015077
OpenAlex: W4324141467
Cited by: 547
References: 69
Citations by year: 2026: 144 · 2025: 216 · 2024: 146 · 2023: 41
FWCI: 26.13
Type: journal article
Language: en
Open access: gold
doi.org
Licence: cc-by
creativecommons.org/licenses/by/4.0 (tdm)
creativecommons.org/licenses/by/4.0 (vor)
Locations: Nature Communications (publishedVersion, cc-by)
PubMed Central (publishedVersion, cc-by)
PubMed (publishedVersion)
RePEc: Research Papers in Economics (submittedVersion)
DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders: Salt Science Research Foundation (BL14W1)
National Natural Science Foundation of China (91945302, 22125903, 51872283, 22172156, 2019RT09, 22172156, 22125 903, 51872283)
Chinese Academy of Sciences (DNL202016, DNL202003, DNL202019, XDB36030200, 2019RT09)
Dalian Institute of Chemical Physics (DICP I2020032, I2020032)
Dalian National Laboratory for Clean Energy (DNL202019, DNL-YL A202205, DNL202016, DNL 202003, DICP I2020032)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords: oxygen evolution reaction, RuO2 electrocatalyst, rhodium doping, oxygen vacancies, acidic water oxidation, proton exchange membrane electrolyzer, hydrogen production, lattice oxygen mechanism, reaction mechanism, catalyst stability, operando characterization

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Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation

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