By incorporating the electron transfer pairs in both the ground and excited states into redox active Werner-typed metal-organic hosts with electronic acceptor/donor guest molecules, Prof. Duan’s group has developed a promising protocol to mimic natural enzymatic systems in the redox transformations within a confined environment. The host-guest supramolecular systems fixed and isolated the donor-acceptor counter-pair with a short through-space separation, and without a through-bond electron transfer route. The confined electron transfer behavior was different from both the classical intermolecular or intramolecular photoinduced electron transfer processes that comply with Rehm-Weller or Marcus theory. It was proposed that this novel electron transfer behavior was helpful to stabilize the charge-separation pair, which enhanced the redox transformations in the ground and excited states. The intrinsic communication between the chromophore guest and the Werner host is the direct confined photoinduced electron transfer from the excited state of the chromophore to the host cage, which provided a meaningful insight into the nature of metabolism of substance and energy in the biological systems. Through the mimic of the reactive site of nicotinamide adenine dinucleotide (NADH), the redox-active metal-organic host facilitated the confined electron transfer process from the reactive sites of the NADH models to the substrate for mimicking the biological hydrogenation in the inner space of the host. The host-guest chemistry within the chromophore-containing Werner-typed hosts permitted additional thermodynamic activation and revision of the electron transfer pathway for chemical reactions. The regioselective and stereoselective photoinduced electron transfer processes in the host are at in the early infant stage, however, they were important in forging the organic reactions with cascade steps or special selectivity.

New paradigm of photocatalysis: Confined electron transfer for supramolecular catalysis within Werner-typed hosts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.