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    Article

    Regulation of Oxide Pathway Mechanism for Sustainable Acidic Water Oxidation
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    • Xuejie Cao
      Xuejie Cao
      Key Laboratory of Advanced Energy Materials Chemistry, Ministry of Education State Key Laboratory of Advanced Chemical Power Sources Collaborative Innovation Center of Chemical Science and Engineering, TianjinCollege of Chemistry, Nankai University, Tianjin 300071, China
      More by Xuejie Cao
    • Hongye Qin
      Hongye Qin
      Key Laboratory of Advanced Energy Materials Chemistry, Ministry of Education State Key Laboratory of Advanced Chemical Power Sources Collaborative Innovation Center of Chemical Science and Engineering, TianjinCollege of Chemistry, Nankai University, Tianjin 300071, China
      More by Hongye Qin
    • Jinyang Zhang
      Jinyang Zhang
      Key Laboratory of Advanced Energy Materials Chemistry, Ministry of Education State Key Laboratory of Advanced Chemical Power Sources Collaborative Innovation Center of Chemical Science and Engineering, TianjinCollege of Chemistry, Nankai University, Tianjin 300071, China
      More by Jinyang Zhang
    • Xiaojie Chen
      Xiaojie Chen
      Key Laboratory of Advanced Energy Materials Chemistry, Ministry of Education State Key Laboratory of Advanced Chemical Power Sources Collaborative Innovation Center of Chemical Science and Engineering, TianjinCollege of Chemistry, Nankai University, Tianjin 300071, China
      More by Xiaojie Chen
    • Lifang Jiao*
      Lifang Jiao
      Key Laboratory of Advanced Energy Materials Chemistry, Ministry of Education State Key Laboratory of Advanced Chemical Power Sources Collaborative Innovation Center of Chemical Science and Engineering, TianjinCollege of Chemistry, Nankai University, Tianjin 300071, China
      *Email: [email protected]
      More by Lifang Jiao
      Orcidhttps://orcid.org/0000-0002-4676-997X
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 46, 32049–32058
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    https://doi.org/10.1021/jacs.4c12942
    Published November 12, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evolution mechanism, while the lattice-oxygen-mediated mechanism undermines stability. Here, we propose a heterogeneous dual-site oxide pathway mechanism (OPM) that avoids these limitations through direct dioxygen radical coupling. A combination of Lewis acid (Cr) and Ru to form solid solution oxides (CrxRu1–xO2) promotes OH adsorption and shortens the dual-site distance, which facilitates the formation of *O radical and promotes the coupling of dioxygen radical, thereby altering the OER mechanism to a Cr–Ru dual-site OPM. The Cr0.6Ru0.4O2 catalyst demonstrates a lower overpotential than that of RuO2 and maintains stable operation for over 350 h in a PEM water electrolyzer at 300 mA cm–2. This mechanism regulation strategy paves the way for an optimal catalytic pathway, essential for large-scale green hydrogen production.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c12942.

    • Experimental procedures, calculation details, EDS, XRD, Rietveld refinement analysis, optimal surface structures, morphology of as-prepared Cr0.6Ru0.4O2 catalyst and RuO2 catalyst, XPS , EXAFS oscillations, CV curves in KOH, Raman spectra, zeta potential, free energy diagrams, FTIR, DEMS, EIS, ECSA, chronoamperometry curves, ICP results, refined structural parameters, and calculated free energy of different mechanisms (PDF)

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    This article is cited by 20 publications.

    1. Jianghao Kang, Yunpeng Fang, Jie Yang, Luo Huang, Yu Chen, Deng Li, Jie Sun, Ruibin Jiang. Recent Development of Ir- and Ru-Based Electrocatalysts for Acidic Oxygen Evolution Reaction. ACS Applied Materials & Interfaces 2025, 17 (14) , 20519-20559. https://doi.org/10.1021/acsami.4c22918
    2. Sheng Zhao, Sung-Fu Hung, Yue Wang, Shaoxiong Li, Juan Yang, Wen-Jing Zeng, Ying Zhang, Hao-Hsiang Chang, Han-Yi Chen, Feng Hu, Linlin Li, Shengjie Peng. Dynamic Deprotonation Enhancement Triggered by Accelerated Electrochemical Delithiation Reconstruction during Acidic Water Oxidation. Journal of the American Chemical Society 2025, 147 (9) , 7993-8003. https://doi.org/10.1021/jacs.5c00493
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    5. Wei Xia, Jinyang Zhang, Guangyu Xu, Ting Jin, Qinglun Wang, Lifang Jiao. Recent advances and challenges in single-atom catalysts for proton exchange membrane water electrolysis. Next Materials 2025, 8 , 100553. https://doi.org/10.1016/j.nxmate.2025.100553
    6. Xinbin Ma, Zeyuan Wang, Baoshan Hou, Yanxing Xu, Ruijian Dong, Cuijuan Xuan. Interface engineering of Fe doped NiO/NiSe2 tailoring d-band center for enhanced oxygen evolution activity. Applied Surface Science 2025, 698 , 163087. https://doi.org/10.1016/j.apsusc.2025.163087
    7. Xiaoxiao Li, Yu Yan, Yuan Yao, Yang Liu. Oxygen radical coupling on short-range ordered V sites for enhanced oxygen evolution reaction activity. Applied Surface Science 2025, 694 , 162829. https://doi.org/10.1016/j.apsusc.2025.162829
    8. Bingyi Qu, Xiaohua Ma, Shaofeng Lou, Shuofeng Tian, Sudan Ma, Xi Cheng, Dongbin Yan, Xianxu Chu. Recent advances on engineering RuO2-based electrocatalysts for acidic oxygen evolution reaction: From the perspective of reaction mechanisms. Journal of Electroanalytical Chemistry 2025, 985 , 119075. https://doi.org/10.1016/j.jelechem.2025.119075
    9. Jie Yu, Haolin Cheng, Yan Fu, Jinli Zhang. Magnetic field oriented dual site S-Ni,FeOOH-M nanoarrays for enhanced oxygen evolution at high current densities. Chemical Engineering Journal 2025, 512 , 162390. https://doi.org/10.1016/j.cej.2025.162390
    10. Chanyuan Ji, Yun Jiang, Lei Guo, Jipeng Wang, Sheng Feng. Reactive species spillover effect for boosting electrocatalytic reaction. Chemical Engineering Journal 2025, 512 , 162560. https://doi.org/10.1016/j.cej.2025.162560
    11. Gege Su, Jiayi Yang, Jie Yin. Advancements in Electrocatalysts for Oxygen Evolution Reaction: A Review of Catalysts in Acidic Media. ChemElectroChem 2025, 12 (8) https://doi.org/10.1002/celc.202400559
    12. Yin'an Zhu, Fei Wu, Xiaozan Zhang, Yichao Lin, Linjuan Zhang, Ting‐Shan Chan, Qiuju Zhang, Liang Chen. Engineering Lattice Distortion in Ruthenium Oxide Enables Robust Acidic Water Oxidation via Direct O–O Coupling. Advanced Materials 2025, 10 https://doi.org/10.1002/adma.202500449
    13. Ying Liu, Yuanyuan Qin, Dawei Yu, Haiyue Zhuo, Churong Ma, Kai Chen. Enhance Water Electrolysis for Green Hydrogen Production with Material Engineering: A Review. The Chemical Record 2025, 2 https://doi.org/10.1002/tcr.202400258
    14. Xiaoqian Wei, Hanyu Gao, Tiantian Wang, Zijian Li, Yanru Geng, Guiping Zheng, Min Gyu Kim, Haeseong Jang, Xien Liu, Qing Qin. Neodymium-Doped Hollow Ir/IrO2 Nanospheres with Low Geometric Iridium Density Enable Excellent Acidic Water Oxidation Performance. Chinese Journal of Structural Chemistry 2025, 121 , 100600. https://doi.org/10.1016/j.cjsc.2025.100600
    15. Meihuan Liu, Xiaoyan Zhong, Xiaoxia Chen, Donghai Wu, Chenyu Yang, Shiyu Li, Chudi Ni, Yiwen Chen, Qinghua Liu, Hui Su. Unraveling Compressive Strain and Oxygen Vacancy Effect of Iridium Oxide for Proton‐Exchange Membrane Water Electrolyzers. Advanced Materials 2025, https://doi.org/10.1002/adma.202501179
    16. Zhaoyan Luo, Yinnan Qian, Zijie Yang, Lei Zhang, Qianling Zhang, Chuanxin He, Xiangzhong Ren. Water‐Hydroxide Trapping in Hollandite‐Type Iridium Oxide Enables Efficient Proton Exchange Membrane Water Electrolysis. Advanced Functional Materials 2025, 49 https://doi.org/10.1002/adfm.202500044
    17. Zhichao Yang, Yutian Ding, Wen Chen, Shuiping Luo, Daofan Cao, Xin Long, Lei Xie, Xincheng Zhou, Xinyi Cai, Ke Liu, Xian‐Zhu Fu, Jing‐Li Luo. Phase‐Engineered Bi‐RuO 2 Single‐Atom Alloy Oxide Boosting Oxygen Evolution Electrocatalysis in Proton Exchange Membrane Water Electrolyzer. Advanced Materials 2025, 37 (9) https://doi.org/10.1002/adma.202417777
    18. Yu Zhang, Wenwen Huang, Hehe Wei. Electrocatalytic Stability Over Ruthenium‐Based Catalysts for Proton Exchange Membrane Water Electrolysis. ChemCatChem 2025, 17 (5) https://doi.org/10.1002/cctc.202401707
    19. Rashid Mehmood, Fuxiang Zhang. Recent progress in understanding mechanism of electrochemical oxygen evolution reaction via operando/in situ characterizations. Chem Catalysis 2025, 355 , 101332. https://doi.org/10.1016/j.checat.2025.101332
    20. Guoxin Ma, Fei Wang, Rui Jin, Bingrong Guo, Haohao Huo, Yulong Dai, Zhe Liu, Jia Liu, Siwei Li. Dual Doping in Precious Metal Oxides: Accelerating Acidic Oxygen Evolution Reaction. International Journal of Molecular Sciences 2025, 26 (4) , 1582. https://doi.org/10.3390/ijms26041582
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 46, 32049–32058
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c12942
    Published November 12, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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