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Direct observation of accelerating hydrogen spillover via surface-lattice-confinement effect

Author

Listed:
  • Yijing Liu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Rankun Zhang

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    Dalian University of Technology)

  • Le Lin

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Yichao Wang

    (University of Chinese Academy of Sciences
    Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Changping Liu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Rentao Mu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Qiang Fu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

Abstract

Uncovering how hydrogen transfers and what factors control hydrogen conductivity on solid surface is essential for enhancing catalytic performance of H-involving reactions, which is however hampered due to the structural complexity of powder catalysts, in particular, for oxide catalysts. Here, we construct stripe-like MnO(001) and grid-like Mn3O4(001) monolayers on Pt(111) substrate and investigate hydrogen spillover atop. Atomic-scale visualization demonstrates that hydrogen species from Pt diffuse unidirectionally along the stripes on MnO(001), whereas it exhibits an isotropic pathway on Mn3O4(001). Dynamic surface imaging in H2 atmosphere reveals that hydrogen diffuses 4 times more rapidly on MnO than the case on Mn3O4, which is promoted by one-dimension surface-lattice-confinement effect. Theoretical calculations indicate that a uniform and medium O-O distance favors hydrogen diffusion while low-coordinate surface O atom inhibits it. Our work illustrates the surface-lattice-confinement effect of oxide catalysts on hydrogen spillover and provides a promising route to improve the hydrogen spillover efficiency.

Suggested Citation

  • Yijing Liu & Rankun Zhang & Le Lin & Yichao Wang & Changping Liu & Rentao Mu & Qiang Fu, 2023. "Direct observation of accelerating hydrogen spillover via surface-lattice-confinement effect," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36044-8
    DOI: 10.1038/s41467-023-36044-8
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    References listed on IDEAS

    as
    1. Carlos Hernández Mejía & Tom W. Deelen & Krijn P. Jong, 2018. "Activity enhancement of cobalt catalysts by tuning metal-support interactions," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    2. Mingwu Tan & Yanling Yang & Ying Yang & Jiali Chen & Zhaoxia Zhang & Gang Fu & Jingdong Lin & Shaolong Wan & Shuai Wang & Yong Wang, 2022. "Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
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    Cited by:

    1. Chengsheng Yang & Sicong Ma & Yongmei Liu & Lihua Wang & Desheng Yuan & Wei-Peng Shao & Lunjia Zhang & Fan Yang & Tiejun Lin & Hongxin Ding & Heyong He & Zhi-Pan Liu & Yong Cao & Yifeng Zhu & Xinhe Ba, 2024. "Homolytic H2 dissociation for enhanced hydrogenation catalysis on oxides," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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