3 years ago

Encapsulation of a Quinhydrone Cofactor in the Inner Pocket of Cobalt Triangular Prisms: Combined Light-Driven Reduction of Protons and Hydrogenation of Nitrobenzene

Encapsulation of a Quinhydrone Cofactor in the Inner Pocket of Cobalt Triangular Prisms: Combined Light-Driven Reduction of Protons and Hydrogenation of Nitrobenzene
Liang Zhao, Chunying Duan, Cheng He, Jing Zhang, Jianwei Wei
The design of artificial systems that mimic highly evolved and finely tuned natural photosynthetic systems has attracted intensive research interest. A new system was formulated that encapsulates a quinhydrone (QHQ) cofactor in metal–organic hosts based on inspiration from the redox relays of photosystem II. The M6L3 triangular prism hosts provided a special redox-modulated environment for the cofactor localized within the pocket, and the proximity effects of the host–guest interactions facilitated the formation of charge-transfer complexes that are typically very difficult to form in normal homogeneous systems. Extensive electron delocalization and well-controlled redox potential were induced to decrease the overpotential of the metal sites for proton reduction. The excellent activity and stability of the supramolecular systems allow the tandem reductions being combined to efficiently reduce nitrobenzene using active H-sources from the light activation of water. Through encapsulation of quinhydrone in redox-active molecular flasks, a strategy for constructing host–guest charge-transfer complexes was developed. It features the redox-modulated environment of the metal–organic host and the proximity effects of the host–guest interactions. The system echoes enzymes in the transformation of nitrobenzene with light.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201707676

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