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Cited by 503Electrocatalysts for Energy ConversionCO2 Reduction Techniques and CatalystsCatalytic Processes in Materials Science

Electronic Structure Engineering of Single‐Atom Ru Sites via Co–N4 Sites for Bifunctional pH‐Universal Water Splitting

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Rong, Chengli, Shen, Xiangjian, Wang, Yuan, Thomsen, Lars, Zhao, Tingwen, Li, Yibing, Lu, Xunyu, Amal, Rose +1 more·2022·Advanced Materials
DOI 10.1002/adma.202110103
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Abstract

The development of bifunctional water‐splitting electrocatalysts that are efficient and stable over a wide range of pH is of great significance but challenging. Here, an atomically dispersed Ru/Co dual‐sites catalyst is reported anchored on N‐doped carbon (Ru/Co–N–C) for outstanding oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in both acidic and alkaline electrolytes. The Ru/Co–N–C catalyst requires the overpotential of only 13 and 23 mV for HER, 232 and 247 mV for OER to deliver a current density of 10 mA cm geo −2 in 0.5 m H 2 SO 4 and 1 m KOH, respectively, outperforming benchmark catalysts Pt/C and RuO 2 . Theoretical calculations reveal that the introduction of Co–N4 sites into Ru/Co–N–C efficiently modify the electronic structure of Ru by enlarging Ru–O covalency and increasing Ru electron density, which in turn optimize the bonding strength between oxygen/hydrogen intermediate species with Ru sites, thereby enhancing OER and HER performance. Furthermore, the incorporation of Co–N4 sites induces electron redistribution around Ru–N4, thus enhancing corrosion–resistance of Ru/Co–N–C during acid and alkaline electrolysis. The Ru/Co–N–C has been applied in a proton exchange membrane water electrolyzer and steady operation is demonstrated at a high current density of 450 mA cm geo −2 for 330 h.

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  • Another challenge for Pt-based electrocatalysts is the constraint of stability in acidic environment due to substantial decay performance in proton solvation during HER.

    “Another challenge for Pt-based electrocatalysts is the constraint of stability in acidic environment due to the substantial decay performance in proton solvation during HER.[9]”

    From Constructing Novel High‐Entropy Alloy Aerogels Platform for pH‐Universal Hydrogen Evolution Reaction with High Electrocatalytic Activity and Stability (2026) · cites this paper as [9]

    The Electrochemical Performance of HER section reports severe activity decay for commercial Pt/C during tests in acidic and alkaline electrolytes, supporting the stability concern in acid. It attributes the decay to dissolution of Pt surface atoms and agglomeration of Pt particles, not to proton solvation. No page number is available in our copy. (LLM, conf=0.88)

    Experimental — accuracy not yet measured

  • Ru- and Ir-based catalysts are the best oxygen evolution reaction electrocatalysts.

    “Ru- and Ir-based catalysts are the best oxygen evolution reaction (OER) electrocatalysts”

    From Carbon Aerogels Loaded with Noble Metal Nanocrystal Electrocatalysts for Efficient Full Water Splitting (2023) · cites this paper as [8]

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Cited by

Sorted by citations

Authors
Rong, C., Shen, X., Wang, Y., Thomsen, L., Zhao, T., Li, Y., Lu, X., Amal, R., & Zhao, C.
Affiliations
  • UNSW Sydney (AU)
  • Zhengzhou University (CN)
  • Australian Nuclear Science and Technology Organisation (AU)
Corresponding author
Zhao, Chuan
ORCID
Venue
Advanced Materials
Publisher
Wiley
Published
2022-04-24
Volume
34
Issue
21
Pages
e2110103-e2110103
ISSN
  • 0935-9648 (ISSN-L)
  • 1521-4095
DOI
10.1002/adma.202110103
OpenAlex
W4224447374
Cited by
503
References
1
Citations by year
2026: 74 · 2025: 124 · 2024: 143 · 2023: 122 · 2022: 40
FWCI
19.32
Type
journal article
Language
en
Open access
Licence
Locations
  • Advanced Materials (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • Figshare (submittedVersion, cc-by)
Funders
  • Australian Research Council (FT170100224, DP210103892, IC200100023)
  • National Natural Science Foundation of China (21873086)
  • Zhengzhou University
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
Keywords
bifunctional electrocatalysts, water splitting, single-atom catalysts, ruthenium, nitrogen-doped carbon, oxygen evolution reaction, hydrogen evolution reaction, pH-universal electrocatalysis, electronic structure engineering, corrosion resistance, proton exchange membrane electrolyzer, electrocatalyst stability

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