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DOE OSTI · 3372181

Confinement Reconstruction Unlocks Stable Ru Single Atom-Doped IrO x Anodes for Long-Term High-Rate CO 2 Electrolysis

Wang, Lei [Univ. of Waterloo, ON (Canada)]·López-Estrada, Omar [Univ. of Calgary, AB (Canada)]·Lu, Siyan [Univ. of Waterloo, ON (Canada)]·Du, Cheng [Univ. of Waterloo, ON (Canada)]·Soni, Aman [Univ. of Calgary, AB (Canada)]·Wang, Xiyang [Univ. of Waterloo, ON (Canada)] (ORCID:0000000275916676)·Wang, Maoyu [Argonne National Laboratory (ANL), Lemont, IL (United States)]·Wang, Hsiaotsu [Canadian Light Source, Saskatoon, SK (Canada); Tamkang Univ., New Taipei City (Taiwan)]·Singh, Zuihar [Univ. of Waterloo, ON (Canada)]·Tirado, Ariel [Canadian Light Source, Saskatoon, SK (Canada)]·Billinghurst, Brant [Canadian Light Source, Saskatoon, SK (Canada)]·Wei, Wei [Univ. of Waterloo, ON (Canada)]·Zhang, Baizhou [Univ. of Waterloo, ON (Canada)]·Chen, Zuolong [Univ. of Waterloo, ON (Canada)]·Wang, Jian [Canadian Light Source, Saskatoon, SK (Canada)] (ORCID:0000000151847023)·Zhou, Jigang [Canadian Light Source, Saskatoon, SK (Canada)]·Sun, Cheng-Jun [Argonne National Laboratory (ANL), Lemont, IL (United States)]·Zhou, Hua [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000196428674)·Smith, Rodney D.L. [Univ. of Waterloo, ON (Canada)] (ORCID:0000000312099653)·Kendall, Brian [Univ. of Waterloo, ON (Canada)]·Sinton, David [Univ. of Toronto, ON (Canada)]·Siahrostami, Samira [Simon Fraser Univ., Burnaby, BC (Canada)] (ORCID:0000000211924634)·Wu, Yimin A. [Univ. of Waterloo, ON (Canada)] (ORCID:0000000238078431)
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Abstract

IrO 2 is a commonly employed anode catalyst for CO 2 electrolysis in membrane electrode assembly (MEA) systems. However, under high current densities, its structural reconstruction leads to activity loss and stability degradation, limiting the industrial viability of CO 2 electrolysis. In this work, we demonstrated a confinement reconstruction strategy to precisely regulate the structural evolution during electrolysis. Ethylene glycol serves as a structural modulator, protecting the catalyst surface, suppressing soluble species formation, and promoting ordered structural evolution. Single-atom Ru acts as a stability enhancer, forming robust Ir–O–Ru bridging structures that facilitate an ordered transformation from a 4-fold [RuO 4 ]/[IrO 4 ] to a 6-fold symmetry [RuO 6 ]/[IrO 6 ] octahedral framework, thereby enhancing structural rigidity and long-term stability. As a result, in MEA-based CO 2 electrolysis, the catalyst achieves a stable operation at 200 mA cm –2 for 480 h, maintaining a CO selectivity above 80%. Theoretical calculations further elucidate that the enhanced stability originates from the suppression of oxygen vacancy formation, making the lattice-oxygen-mediated mechanism (LOM) potentially less favorable. This work provides insights into the structural evolution of the OER catalysts under high-current-density conditions, paving the way for large-scale CO 2 electrolysis commercialization.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYCO2 reductionElectrocatalysisMEAneutral electrolyteoxygen evolution reactionstabilitystructural reconstruction

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Wang, Lei [Univ. of Waterloo, ON (Canada)], López-Estrada, Omar [Univ. of Calgary, AB (Canada)], Lu, Siyan [Univ. of Waterloo, ON (Canada)], Du, Cheng [Univ. of Waterloo, ON (Canada)], Soni, Aman [Univ. of Calgary, AB (Canada)], Wang, Xiyang [Univ. of Waterloo, ON (Canada)] (ORCID:0000000275916676), Wang, Maoyu [Argonne National Laboratory (ANL), Lemont, IL (United States)], Wang, Hsiaotsu [Canadian Light Source, Saskatoon, SK (Canada); Tamkang Univ., New Taipei City (Taiwan)], Singh, Zuihar [Univ. of Waterloo, ON (Canada)], Tirado, Ariel [Canadian Light Source, Saskatoon, SK (Canada)], Billinghurst, Brant [Canadian Light Source, Saskatoon, SK (Canada)], Wei, Wei [Univ. of Waterloo, ON (Canada)], Zhang, Baizhou [Univ. of Waterloo, ON (Canada)], Chen, Zuolong [Univ. of Waterloo, ON (Canada)], Wang, Jian [Canadian Light Source, Saskatoon, SK (Canada)] (ORCID:0000000151847023), Zhou, Jigang [Canadian Light Source, Saskatoon, SK (Canada)], Sun, Cheng-Jun [Argonne National Laboratory (ANL), Lemont, IL (United States)], Zhou, Hua [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000196428674), Smith, Rodney D.L. [Univ. of Waterloo, ON (Canada)] (ORCID:0000000312099653), Kendall, Brian [Univ. of Waterloo, ON (Canada)], Sinton, David [Univ. of Toronto, ON (Canada)], Siahrostami, Samira [Simon Fraser Univ., Burnaby, BC (Canada)] (ORCID:0000000211924634), Wu, Yimin A. [Univ. of Waterloo, ON (Canada)] (ORCID:0000000238078431). 2026-01-05. Confinement Reconstruction Unlocks Stable Ru Single Atom-Doped IrO x Anodes for Long-Term High-Rate CO 2 Electrolysis. https://doi.org/10.1021/acscatal.5c06756

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