Rationalizing Acidic Oxygen Evolution Reaction over IrO 2 : Essential Role of Hydronium Cation

Mou, Tianyou; Bushiri, Daniela A.; Esposito, Daniel V.; Chen, Jingguang G.; Liu, Ping

doi:10.1002/ange.202409526

Title: Rationalizing Acidic Oxygen Evolution Reaction over IrO ₂ : Essential Role of Hydronium Cation

Journal Article · 04 September 2024 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202409526 · OSTI ID:2514496

Mou, Tianyou ^[1]; Bushiri, Daniela A. ^[2]; Esposito, Daniel V. ^[2];

^[3]; Liu, Ping ^[1]

Chemistry Division Brookhaven National Laboratory 11973 Upton NY USA
Department of Chemical Engineering Columbia University 10027 New York NY USA
Chemistry Division Brookhaven National Laboratory 11973 Upton NY USA, Department of Chemical Engineering Columbia University 10027 New York NY USA

Abstract The development of active, stable, and more affordable electrocatalysts for acidic oxygen evolution reaction (OER) is of great importance for the practical application of electrolyzers and the advancement of renewable energy conversion technologies. Currently, IrO ₂ is the only catalyst with high stability and activity, but a high cost. Further optimization of the catalyst is limited by the lack of understanding of catalytic behaviors at the acid‐IrO ₂ interface. Here, in strong interaction with the experiment, we develop an explicit model based on grand‐canonical density function theory (GC‐DFT) calculations to describe acidic OER over IrO ₂ . Compared to the explicit models reported previously, hydronium cations (H ₃ O ⁺ ) are introduced at the electrochemical interface in the current model. As a result, a variation in stable IrO ₂ surface configuration under the OER operating condition from previously proposed complete *O‐coverage to a mixture coverage of *OH and *O is revealed, which is well supported by in situ Raman measurements. In addition, the accuracy of predicted overpotential is increased in comparison with the experimentally measured. More importantly, an alteration of the potential limiting step from previously identified *O→*OOH to *OH→*O is observed, which opens new opportunities to advance the IrO ₂ ‐based catalysts for acidic OER.

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Sponsoring Organization:: USDOE

OSTI ID:: 2514496

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 48 Vol. 136; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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