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Snap-Fit Assembly of Multicomponent Pt(II) Metallacages Enabling Through-Space Electron Transfer and Enhanced
Jikun Li1, Shijin Jian1, Zilin Zhou1
1State Key Laboratory for Porous Metal Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Shaanxi International Research Center for Soft Matter, Xi'an Key Laboratory of Sustainable Polymer Materials, School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China.
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The rational design of heteroleptic metallacages from multiple ligands remains a significant challenge in supramolecular chemistry due to the tendency for thermodynamic mixtures and poorly defined assemblies. Herein, we demonstrate a snap-fit-inspired self-assembly strategy for the construction of heteroleptic platinum(II) cages containing three types of organic ligands. An asymmetric tetracarboxylate ligand acts as a multifaceted connector, guiding the two distinct tetrapyridyl panels to snap into place around the Pt(II) vertices, yielding a type of box-shaped metallacage with reduced constitutional symmetry. Spatial combination of electron-rich anthracene or dimethoxybenzene donors with electron-deficient perylene diimide acceptors within a single metallacage facilitates efficient through-space photoinduced electron transfer and charge separation. As a result, the metallacages promote the generation of superoxide radical anions and enable photocatalytic benzimidazole formation from o-phenylenediamine and aromatic aldehydes via a condensation-oxidative cyclization sequence. This snap-fit assembly concept provides a modular and programmable approach to multicomponent metallacages and enables deliberate control over intramolecular electronic communication for supramolecular photocatalysis.
