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PreprintCC BYChemRxiv

Disrupting Surface Oxo Availability Suppresses Ru Dissolution in RuO ₂ Electrocatalysts

  • Charles B. Musgrave1,2,3
  • Mengjie Liu1,2,3
  • Jaerim Kim1,2,3
  • Shih-Ching Huang4,5
  • Dániel Hetey6,7
  • Matej Zlatar6
  • Connor R. McCormick1,2,3
  • Yuyin Li1,2,3
  • Yan-Gu Lin4,5,8,9
  • Serhiy Cherevko6
  • Edward H. Sargent1,2,3
9 affiliations
  1. 1Department of Electrical and Computer Engineering
  2. 2Northwestern University
  3. 3Department of Chemistry
  4. 4Scientific Research Division
  5. 5National Synchrotron Radiation Research Center
  6. 6Forschungszentrum Jülich GmbH, Cauerstr. 1, Erlangen, Germany, 91058
  7. 7Department of Chemical and Biological Engineering, Friedrich-Alexander-University, Egerlandstraße 1, Erlangen, Germany, 91058
  8. 8Department of Materials Science and Engineering
  9. 9National Yang Ming Chiao Tung University
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Abstract

Ru loss from RuO 2 in acidic oxygen evolution requires availability of surface oxo (*O) for eruption of surface Ru to form adsorbed *RuO 4 . Screening 20 dopants on *O-covered RuO 2 (110) (DFT) gave a trend linking *RuO 4 formation to dopant-dependent *O activity. Durability testing (CP, ICP-MS) followed this trend for Mo- and Ta-RuO 2 . Zn- and Hf-RuO 2 retained more Ru than predicted; in situ near-ambient pressure XPS and online ICP-MS reveal that the two do so by different means. Zn inhibits Ru overoxidation while Hf welcomes it, yet both inhibit Ru eruption. Surface-modulated models in which Zn dissolution leaves a cation vacancy and Hf bears a surface *OH both exhibit enhanced Ru retention (DFT): cation vacancies electronically reduce neighboring Ru and lack *O, whereas Hf’s *OH permits Ru overoxidation but inhibits its eruption. Both catalysts retain high activity (LSV) through a Ru-centered oxygen evolution pathway (GC-DFT). These findings reveal how dopants can enhance Ru retention by disrupting *O participation, regardless of Ru oxidation state, all while maintaining high oxygen evolution activity.

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Cite

BibTeXRIS
BibTeX
@misc{musgrave2026disrupting,
  title = {{Disrupting Surface Oxo Availability Suppresses Ru Dissolution in RuO ₂ Electrocatalysts}},
  author = {Charles B. Musgrave and Mengjie Liu and Jaerim Kim and Shih-Ching Huang and Dániel Hetey and Matej Zlatar and Connor R. McCormick and Yuyin Li and Yan-Gu Lin and Serhiy Cherevko and Edward H. Sargent},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15011005/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011005/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Disrupting Surface Oxo Availability Suppresses Ru Dissolution in RuO ₂ Electrocatalysts
AU  - Charles B. Musgrave
AU  - Mengjie Liu
AU  - Jaerim Kim
AU  - Shih-Ching Huang
AU  - Dániel Hetey
AU  - Matej Zlatar
AU  - Connor R. McCormick
AU  - Yuyin Li
AU  - Yan-Gu Lin
AU  - Serhiy Cherevko
AU  - Edward H. Sargent
PY  - 2026
DA  - 2026/10/25
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15011005/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011005/v1
AB  - Ru loss from RuO 2 in acidic oxygen evolution requires availability of surface oxo (*O) for eruption of surface Ru to form adsorbed *RuO 4 . Screening 20 dopants on *O-covered RuO 2 (110) (DFT) gave a trend linking *RuO 4 formation to dopant-dependent *O activity. Durability testing (CP, ICP-MS) followed this trend for Mo- and Ta-RuO 2 . Zn- and Hf-RuO 2 retained more Ru than predicted; in situ near-ambient pressure XPS and online ICP-MS reveal that the two do so by different means. Zn inhibits Ru overoxidation while Hf welcomes it, yet both inhibit Ru eruption. Surface-modulated models in which Zn dissolution leaves a cation vacancy and Hf bears a surface *OH both exhibit enhanced Ru retention (DFT): cation vacancies electronically reduce neighboring Ru and lack *O, whereas Hf’s *OH permits Ru overoxidation but inhibits its eruption. Both catalysts retain high activity (LSV) through a Ru-centered oxygen evolution pathway (GC-DFT). These findings reveal how dopants can enhance Ru retention by disrupting *O participation, regardless of Ru oxidation state, all while maintaining high oxygen evolution activity.
ER  -