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Enabling long-distance hydrogen spillover in nonreducible metal-organic frameworks for catalytic reaction

Author

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  • Xiao-Jue Bai

    (National Center for Nanoscience and Technology)

  • Caoyu Yang

    (National Center for Nanoscience and Technology
    University of Chinese Academy of Sciences)

  • Zhiyong Tang

    (National Center for Nanoscience and Technology
    University of Chinese Academy of Sciences)

Abstract

Hydrogen spillover is an extraordinary effect in heterogeneous catalysis and hydrogen storage, which refers to the surface migration of metal particle-activated hydrogen atoms over the solid supports. Historical studies on this phenomenon have mostly been limited to reducible metal oxides where the long-distance proton-electron coupled migration mechanism has been established, yet the key question remains on how to surmount short-distance and defect-dependent hydrogen migration on nonreducible supports. By demerging hydrogen migration and hydrogenation reaction, here we demonstrate that the hydrogen spillover in nonreducible metal-organic frameworks (MOFs) can be finely modulated by the ligand functional groups or embedded water molecules, enabling significant long-distance (exceed 50 nm) movement of activated hydrogen. Furthermore, using sandwich nanostructured MOFs@Pt@MOFs as catalysts, we achieve highly selective hydrogenation of N-heteroarenes via controllable hydrogen spillover from Pt to MOFs-shell. We anticipate that this work will enhance the understanding of hydrogen spillover and shed light on de novo design of MOFs supported catalysts for many important reactions involving hydrogen.

Suggested Citation

  • Xiao-Jue Bai & Caoyu Yang & Zhiyong Tang, 2024. "Enabling long-distance hydrogen spillover in nonreducible metal-organic frameworks for catalytic reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50706-1
    DOI: 10.1038/s41467-024-50706-1
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