A zero-valent palladium cluster-organic framework

Xiyue Liu, James N. McPherson (), Carl Emil Andersen, Mike S. B. Jørgensen, René Wugt Larsen, Nathan J. Yutronkie, Fabrice Wilhelm, Andrei Rogalev, Mónica Giménez-Marqués, Guillermo Mínguez Espallargas, Christian R. Göb and Kasper S. Pedersen ()
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Xiyue Liu: Technical University of Denmark
James N. McPherson: Technical University of Denmark
Carl Emil Andersen: Technical University of Denmark
Mike S. B. Jørgensen: Technical University of Denmark
René Wugt Larsen: Technical University of Denmark
Nathan J. Yutronkie: European Synchrotron Radiation Facility (ESRF)
Fabrice Wilhelm: European Synchrotron Radiation Facility (ESRF)
Andrei Rogalev: European Synchrotron Radiation Facility (ESRF)
Mónica Giménez-Marqués: Universidad de Valencia, Paterna
Guillermo Mínguez Espallargas: Universidad de Valencia, Paterna
Christian R. Göb: Rigaku Europe SE
Kasper S. Pedersen: Technical University of Denmark

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

Abstract: Abstract Acquiring spatial control of nanoscopic metal clusters is central to their function as efficient multi-electron catalysts. However, dispersing metal clusters on surfaces or in porous hosts is accompanied by an intrinsic heterogeneity that hampers detailed understanding of the chemical structure and its relation to reactivities. Tethering pre-assembled molecular metal clusters into polymeric, crystalline 2D or 3D networks constitutes an unproven approach to realizing ordered arrays of chemically well-defined metal clusters. Herein, we report the facile synthesis of a {Pd3} cluster-based organometallic framework from a molecular triangulo-Pd3(CNXyl)6 (Xyl = xylyl; Pd3) cluster under chemically mild conditions. The formally zero-valent Pd3 cluster readily engages in a complete ligand exchange when exposed to a similar, ditopic isocyanide ligand, resulting in polymerization into a 2D coordination network (Pd3-MOF). The structure of Pd3-MOF could be unambiguously determined by continuous rotation 3D electron diffraction (3D-ED) experiments to a resolution of ~1.0 Å (>99% completeness), showcasing the applicability of 3D-ED to nanocrystalline, organometallic polymers. Pd3-MOF displays Pd03 cluster nodes, which possess significant thermal and aerobic stability, and activity towards hydrogenation catalysis. Importantly, the realization of Pd3-MOF paves the way for the exploitation of metal clusters as building blocks for rigidly interlocked metal nanoparticles at the molecular limit.

Date: 2024
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DOI: 10.1038/s41467-024-45363-3

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