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Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition

Author

Listed:
  • Yunpeng Long

    (Tsinghua University)

  • Xiao Zhu

    (Tsinghua University)

  • Chuan Gao

    (Tsinghua University)

  • Wenzhe Si

    (Tsinghua University)

  • Junhua Li

    (Tsinghua University)

  • Yue Peng

    (Tsinghua University)

Abstract

Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions of long-range order and alterations in electronic structure. However, the mechanisms of molecule activation and spin states at interfaces remain elusive. Herein, we present a Co3O4 spinel-based catalyst featuring crystalline-amorphous interfaces. Characterization analyses confirm that tetrahedral Co2+ is selectively etched from bulk spinel, forming amorphous CoO islands on the surface. The resultant symmetry breaking in the coordination field induces a reconstruction of the Co3+ 3 d orbitals, leading to high-spin states. In CO oxidation, the interface serves as novel active sites with a lower energy barrier, facilitated by lattice oxygen activation. In N2O decomposition, the interface promotes reassociation of dissociated oxygen through quantum spin exchange interactions. This work provides a straightforward approach to modulating the spin state of interfaces and elucidates their role in molecule activations.

Suggested Citation

  • Yunpeng Long & Xiao Zhu & Chuan Gao & Wenzhe Si & Junhua Li & Yue Peng, 2025. "Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56487-5
    DOI: 10.1038/s41467-025-56487-5
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    References listed on IDEAS

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    1. Sihong Wang & Qu Jiang & Shenghong Ju & Chia-Shuo Hsu & Hao Ming Chen & Di Zhang & Fang Song, 2022. "Identifying the geometric catalytic active sites of crystalline cobalt oxyhydroxides for oxygen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Juan Wang & Lili Han & Bolong Huang & Qi Shao & Huolin L. Xin & Xiaoqing Huang, 2019. "Amorphization activated ruthenium-tellurium nanorods for efficient water splitting," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    3. Xin Zhang & Haoyin Zhong & Qi Zhang & Qihan Zhang & Chao Wu & Junchen Yu & Yifan Ma & Hang An & Hao Wang & Yiming Zou & Caozheng Diao & Jingsheng Chen & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin , 2024. "High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Arno Bergmann & Elias Martinez-Moreno & Detre Teschner & Petko Chernev & Manuel Gliech & Jorge Ferreira de Araújo & Tobias Reier & Holger Dau & Peter Strasser, 2015. "Reversible amorphization and the catalytically active state of crystalline Co3O4 during oxygen evolution," Nature Communications, Nature, vol. 6(1), pages 1-9, December.
    5. Davis, Steven J & Lewis, Nathan S. & Shaner, Matthew & Aggarwal, Sonia & Arent, Doug & Azevedo, Inês & Benson, Sally & Bradley, Thomas & Brouwer, Jack & Chiang, Yet-Ming & Clack, Christopher T.M. & Co, 2018. "Net-Zero Emissions Energy Systems," Institute of Transportation Studies, Working Paper Series qt7qv6q35r, Institute of Transportation Studies, UC Davis.
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