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Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction

Author

Listed:
  • Jihyun Baek

    (Stanford University)

  • Md Delowar Hossain

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Pinaki Mukherjee

    (Stanford University)

  • Junghwa Lee

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Kirsten T. Winther

    (SLAC National Accelerator Laboratory)

  • Juyoung Leem

    (Stanford University)

  • Yue Jiang

    (Stanford University)

  • William C. Chueh

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Michal Bajdich

    (SLAC National Accelerator Laboratory)

  • Xiaolin Zheng

    (Stanford University)

Abstract

Developing stable and efficient electrocatalysts is vital for boosting oxygen evolution reaction (OER) rates in sustainable hydrogen production. High-entropy oxides (HEOs) consist of five or more metal cations, providing opportunities to tune their catalytic properties toward high OER efficiency. This work combines theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Density functional theory confirms that randomly mixed metal sites show thermodynamic stability, with intermediate adsorption energies displaying wider distributions due to mixing-induced equatorial strain in active metal-oxygen bonds. The rapid sol-flame method is employed to synthesize HEO, comprising five 3d-transition metal cations, which exhibits superior OER activity and durability under alkaline conditions, outperforming lower-entropy oxides, even with partial surface oxidations. The study highlights that the enhanced activity of HEO is primarily attributed to the mixing of multiple elements, leading to strain effects near the active site, as well as surface composition and coverage.

Suggested Citation

  • Jihyun Baek & Md Delowar Hossain & Pinaki Mukherjee & Junghwa Lee & Kirsten T. Winther & Juyoung Leem & Yue Jiang & William C. Chueh & Michal Bajdich & Xiaolin Zheng, 2023. "Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41359-7
    DOI: 10.1038/s41467-023-41359-7
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