Redox-Active M8L6 Cubic Hosts with Tetraphenylethylene Faces Encapsulate Organic Dyes for Light-Driven H-2 Production

Redox-Active M8L6 Cubic Hosts with Tetraphenylethylene Faces Encapsulate Organic Dyes for Light-Driven H-2 Production
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具有四苯乙烯面的氧化还原活性 M8L6 立方主体封装有机染料,用于光驱动 H-2 生产

DOI:
10.1002/chem.201601447
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发表时间:
2016
期刊:
Chemistry - A European Journal
影响因子:
--
通讯作者:
Duan Chunying
Duan Chunying
中科院分区:
其他
文献类型:
--
作者:
Yang Linlin;Jing Xu;He Cheng;Chang Zhiduo;Duan Chunying

文献摘要

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The design of artificial systems that mimic highly evolved and finely tuned natural enzymes is a promising subject of intensive research. The assembly ofO‐symmetric cubic structures with an Fe8L6formula was reported through the direct combination of aC4‐symmetric tetraphenylethylene‐based ligand with aC3‐symmetric tris(bipyridine)iron node. The robust metal–organic cubes are rich in π‐electron density and provide favorable interactions with planar polycyclic aromatic hydrocarbons. Within the confined space of the host, the aromatic hydrocarbons molecules are forced closer to the redox active host, and the photoinduced electron transfer (PET) is modified into a pseudo‐intramolecular pathway. These iron vertices within the cubes exhibit suitable redox potential for electrochemical reduction of protons and the well‐modified PET is further tailored to create artificial systems for light‐driven hydrogen evolution from water through the encapsulation of fluorescein dyes. Control experiments based on a mononuclear compound resembling the iron corner of the octahedron suggest an enzymatic dynamic behavior. The new, well‐elucidated reaction pathways and the increased molarity of the reaction within the confined space render these supramolecular systems superior to other relevant systems.