A Complex Oxide Containing Inherent Peroxide Ions for Catalyzing Oxygen Evolution Reactions in Acid
Proton exchange membrane water electrolyzers powered by sustainable energy represent a cutting-edge technology for renewable hydrogen generation, while slow anodic oxygen evolution reaction (OER) kinetics still remains a formidable obstacle that necessitates basic comprehension for facilitating electrocatalysts' design. Here, we report a low-iridium complex oxide La<sub>1.2</sub>Sr<sub>2.7</sub>IrO<sub>7.33</sub> with a unique hexagonal structure consisting of isolated Ir(V)O<sub>6</sub> octahedra and true peroxide O<sub>2</sub><sup>2-</sup> groups as a highly active and stable OER electrocatalyst under acidic conditions. Remarkably, La<sub>1.2</sub>Sr<sub>2.7</sub>IrO<sub>7.33</sub>, containing 59 wt % less iridium relative to the benchmark IrO<sub>2</sub>, shows about an order of magnitude higher mass activity, 6-folds higher intrinsic activity than the latter, and also surpasses the state-of-the-art Ir-based oxides ever reported. Combined electrochemical, spectroscopic, and density functional theory investigations reveal that La<sub>1.2</sub>Sr<sub>2.7</sub>IrO<sub>7.33</sub> follows the peroxide-ion participation mechanism under the OER condition, where the inherent peroxide ions with accessible nonbonded oxygen states are responsible for the high OER activity. This discovery offers an innovative strategy for designing advanced catalysts for various catalytic applications.
Authors
- Zhiwei Hu (ORCID: https://orcid.org/0000-0003-0324-2227)
- Daqin Guan (ORCID: https://orcid.org/0000-0001-5393-2301)
- Chuan Zhou (ORCID: https://orcid.org/0000-0002-6162-9748)
- Hainan Sun (ORCID: https://orcid.org/0000-0003-1589-3860)
- Zongping Shao (ORCID: https://orcid.org/0000-0002-4538-4218)
- Yinlong Zhu (ORCID: https://orcid.org/0000-0002-9207-2452)
- Zihan Shen (ORCID: https://orcid.org/0000-0002-5368-8190)
- Jie Dai (ORCID: https://orcid.org/0000-0001-9470-5172)
- Chih‐Wen Pao (ORCID: https://orcid.org/0000-0001-7681-4391)
- Vanessa K. Peterson (ORCID: https://orcid.org/0000-0002-5442-0591)
- Yu Chen (ORCID: https://orcid.org/0000-0001-7145-3873)
- Yu Li (ORCID: https://orcid.org/0000-0003-1430-7989)
- Mengran Li (ORCID: https://orcid.org/0000-0001-7858-0533)
- Wei Zhou (ORCID: https://orcid.org/0000-0003-0322-095X)
- Xixi Wang (ORCID: https://orcid.org/0000-0003-0829-7745)
- Jiayi Tang (ORCID: https://orcid.org/0000-0003-0725-6239)
- Wei-Hsiang Huang (ORCID: https://orcid.org/0000-0002-4796-6609)
- Chien‐Te Chen
Institutions
- Australian Nuclear Science and Technology Organisation (AU)
- Nanjing Tech University (CN)
- Korea Advanced Institute of Science and Technology (KR)
- The University of Melbourne (AU)
- Shanghai Jiao Tong University (CN)
- Curtin University (AU)
- National Synchrotron Radiation Research Center (TW)
- Max Planck Institute for Chemical Physics of Solids (DE)
- Suzhou Research Institute (CN)
- Institute of Process Engineering (CN)
- Monash University (AU)
- Nanjing University of Aeronautics and Astronautics (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-11-25
- DOI
- https://doi.org/10.1021/jacs.4c11477
- Citations
- 42
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 4.30
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Natural Science Foundation of Jiangsu Province
- National Postdoctoral Program for Innovative Talents