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

Xiao-Jue Bai, Caoyu Yang and Zhiyong Tang ()
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Xiao-Jue Bai: National Center for Nanoscience and Technology
Caoyu Yang: National Center for Nanoscience and Technology
Zhiyong Tang: National Center for Nanoscience and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-50706-1

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