Crystalline metal−organic frameworks (MOFs) are candidates for heterogeneous photo(electro)catalysts performing as synthetic analogs of photosynthetic light-harvesting complexes (LHCs). For this, one would need a modular system where the photogenerated molecular excitons can be efficiently manipulated as needed. A photo(electro)chemical transformation in the ambient condition is quite challenging as the substrate activation must be done within the nano-(sub-nano-)second lifetime of the excited photosensitizer (PS*), and molecular diffusion comes into the picture. Solving this problem, we can think of ways to efficiently migrate/displace the exciton instead of molecular diffusion of the PS*. In MOFs, the precisely assembled linkers (organic chromophores) around the topology-defined pores offer a plethora of opportunities with unique photophysical properties that are reminiscence of LHCs. Like the spatially dispersed excitons can be directionally and efficiently displaced, depending on the topology, of course. We will describe, with several MOF structures, the underline linker, and the assembly criteria to make superior MOF-based photosensitizer, and their electronic properties to efficiently split the energy (i.e., excitons) into redox equivalents.

Manipulating singlet excitons in MOFs for efficient heterogeneous photo(electro)catalysis

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