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Cited by 183Electrocatalysts for Energy ConversionCatalytic Processes in Materials ScienceAdvanced oxidation water treatment

Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation

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Ji, Qianqian, Tang, Bing, Zhang, Xilin, Wang, Chao, Tan, Hao, Zhao, Jie, Liu, Ruiqi, Sun, Mei +5 more·2024·Nature Communications
DOI 10.1038/s41467-024-52471-7PMC PMC11405856
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Abstract

The microscopic reaction pathway plays a crucial role in determining the electrochemical performance. However, artificially manipulating the reaction pathway still faces considerable challenges. In this study, we focus on the classical acidic water oxidation based on RuO2 catalysts, which currently face the issues of low activity and poor stability. As a proof-of-concept, we propose a strategy to create local structural symmetry but oxidation-state asymmetric Mn4-δ-O-Ru4+δ active sites by introducing Mn atoms into RuO2 host, thereby switching the reaction pathway from traditional adsorbate evolution mechanism to oxide path mechanism. Through advanced operando synchrotron spectroscopies and density functional theory calculations, we demonstrate the synergistic effect of dual-active metal sites in asymmetric Mn4-δ-O-Ru4+δ microstructure in optimizing the adsorption energy and rate-determining step barrier via an oxide path mechanism. This study highlights the importance of engineering reaction pathways and provides an alternative strategy for promoting acidic water oxidation. Microscopic reaction pathways are crucial for electrochemical performance, but manipulating them remains challenging. Here, the authors report an approach that involves integrating Mn into RuO2 catalysts to switch the reaction mechanism of the oxygen evolution reaction from a traditional single metal-site adsorbate evolution mechanism to a different dual-metal-site oxide path mechanism.

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  • The average valence for the Ru species in Ru-RuOx/GA-2 is situated between Ru0 and Ru4+.

    “indicating that the average valence for the Ru species in Ru–RuOx/GA-2 is situated between Ru0 and Ru4+.1,45”

    From Interface strain engineering of a Ru–RuO <sub> <i>x</i> </sub> /graphene aerogel composite boosts HER, OER and ORR applications (2026) · cites this paper as [45]

    The Results section on structural characterization reports a Ru oxidation state of +4.46 for Mn0.2RuO2, a different material. A search for Ru–RuOx/GA-2 and its average Ru valence found no passage addressing the claimed material; the Mn0.2RuO2 result does not establish its valence. (LLM, conf=0.76)

    Experimental — accuracy not yet measured

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Cited by

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Authors
Ji, Q., Tang, B., Zhang, X., Wang, C., Tan, H., Zhao, J., Liu, R., Sun, M., Liu, H., Jiang, C., Zeng, J., Cai, X., & Yan, W.
Affiliations
  • Shenzhen University (CN)
  • University of Science and Technology of China (CN)
  • Henan Normal University (CN)
  • Xiamen University (CN)
  • Chinese Academy of Sciences (CN)
Corresponding author
  • Cai, Xingke
  • Yan, Wensheng
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2024-09-16
Volume
15
Issue
1
Pages
8089-8089
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-024-52471-7
PMC
PMC11405856
OpenAlex
W4402580280
Cited by
183
References
1
Citations by year
2026: 93 · 2025: 84 · 2024: 6
FWCI
12.20
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by-nc-nd)
  • PubMed Central (publishedVersion, cc-by-nc-nd)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • Salt Science Research Foundation
  • National Natural Science Foundation of China (12305364, 52373266, 12275271)
  • University of Science and Technology of China
  • National Synchrotron Radiation Laboratory
  • National Key Research and Development Program of China (2021YFA1600800, 2023YFF0716100)
  • Beijing Synchrotron Radiation Facility
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 › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
Keywords
acidic water oxidation, oxygen evolution reaction, RuO2 catalyst, adsorbate evolution mechanism, rate-determining step, adsorption energy, electrocatalyst stability

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