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Molecule-based solid-state materials with long lifetimes could enable longer migration distances for excitons, which are beneficial for vast applications in optoelectronic field. Herein, we report a hexanuclear zinc cluster based MOF exhibits highly enhanced phosphorescence about 2 orders of magnitude in comparison with the pristine phosphor ligand. The combination of both experimental and computational results suggest that the {Zn6} cluster is very important for adjusting molecular conformations, packing arrangement, and photophysical properties of the organic phosphor ligands within the MOF matrix. Optoelectronic measurements reveal that the MOF-modified electrode is catalytically active to hydrogen evolution under light irradiation in neutral solution. Thus, our study provide an effective way to achieve low-cost metal-based phosphorescence MOF, expanding its further optoelectronic applications.

Oriented by the structure-directing effect of metal clusters, a novel trinuclear nickel-based MOF (Ni–BTC) exhibited highly denser crystal packing and π-conjugation degree, providing a platform for efficient charge carrier mobility between metal clusters through π-conjugated molecular bridges and long-term stability of an efficient oxygen evolution reaction.