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Encapsulation of a Quinhydrone Cofactor in the Inner Pocket of Cobalt Triangular Prisms: Combined Light‐Driven Reduction of Protons and Hydrogenation of Nitrobenzene
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-11-02 , DOI: 10.1002/anie.201707676
Liang Zhao 1 , Jianwei Wei 1 , Jing Zhang 1 , Cheng He 1 , Chunying Duan 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-11-02 , DOI: 10.1002/anie.201707676
Liang Zhao 1 , Jianwei Wei 1 , Jing Zhang 1 , Cheng He 1 , Chunying Duan 1
Affiliation
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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.
中文翻译:
钴三角棱镜内袋中的醌醌辅助因子的封装:质子的光驱动还原与硝基苯加氢的结合
模仿高度进化和微调的自然光合系统的人工系统的设计引起了广泛的研究兴趣。根据光系统II的氧化还原继电器的启发,制定了一个新系统,该系统将喹–酮(QHQ)辅因子封装在金属有机主体中。M 6 L 3三角棱镜主体为位于袋中的辅因子提供了特殊的氧化还原调节环境,主体与客体相互作用的邻近效应促进了电荷转移络合物的形成,而这些电荷转移络合物通常很难在正常的均相系统中形成。诱导了广泛的电子离域和良好控制的氧化还原电势,以减少金属位点用于质子还原的过电势。超分子系统具有出色的活性和稳定性,可将串联还原反应结合起来,从而利用水的光活化产生的活性H源有效地还原硝基苯。
更新日期:2017-11-02
中文翻译:
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钴三角棱镜内袋中的醌醌辅助因子的封装:质子的光驱动还原与硝基苯加氢的结合
模仿高度进化和微调的自然光合系统的人工系统的设计引起了广泛的研究兴趣。根据光系统II的氧化还原继电器的启发,制定了一个新系统,该系统将喹–酮(QHQ)辅因子封装在金属有机主体中。M 6 L 3三角棱镜主体为位于袋中的辅因子提供了特殊的氧化还原调节环境,主体与客体相互作用的邻近效应促进了电荷转移络合物的形成,而这些电荷转移络合物通常很难在正常的均相系统中形成。诱导了广泛的电子离域和良好控制的氧化还原电势,以减少金属位点用于质子还原的过电势。超分子系统具有出色的活性和稳定性,可将串联还原反应结合起来,从而利用水的光活化产生的活性H源有效地还原硝基苯。