The structural and chemical tunability of metal-organic frameworks (MOFs) makes them promising platforms for single-site heterogeneous catalysts. Our group has been investigating MOF assembly from metallolinkers based on catalytically-active transition metal diphosphine pincer complexes. The immobilized pincer complexes benefit from site isolation and exhibit marked improvements in catalytic activity and stability compared to homogeneous analogues. This presentation will discuss our recent efforts to use postsynthetic modification reactions to append pincer complexes at the metal nodes or amine linker sites of mesoporous MOFs such as NU-1000 and MIL-101-NH2(Al). This approach offers greater versatility for catalyst design than direct synthesis from metallolinkers. Solvent-assisted ligand incorporation (SALI) has been used to attach PNNNP-Pd pincer complexes at the Zr-based metal nodes of NU-1000. The catalyst loading can be varied from 0.16-0.57 equivalents per node by controlling the postsynthetic reaction conditions. Ongoing studies are focused on investigating the reactivity and catalytic activity of these new materials.

Designing MOFs with immobilized pincer complexes

ACS Spring 2022

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