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首页> 外文期刊>Chemistry: A European journal >A charge-stabilizing, multimodular, ferrocene-bis(triphenylamine)-zinc- porphyrin-fullerene polyad
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A charge-stabilizing, multimodular, ferrocene-bis(triphenylamine)-zinc- porphyrin-fullerene polyad

机译：电荷稳定的多模块二茂铁-双（三苯胺）-锌-卟啉-富勒烯多聚体

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摘要

A novel multimodular donor-acceptor polyad featuring zinc porphyrin, fullerene, ferrocene, and triphenylamine entities was designed, synthesized, and studied as a charge-stabilizing, photosynthetic-antenna/reaction-center mimic. The ferrocene and fullerene entities, covalently linked to the porphyrin ring, were distantly separated to accomplish the charge-separation/hole-migration events leading to the creation of a long-lived charge-separated state. The geometry and electronic structures of the newly synthesized compound was deduced by B3LYP/3-21G(*) optimization, while the energy levels for different photochemical events was established using data from the optical absorption and emission, and electrochemical studies. Excitation of the triphenylamine entities revealed singlet-singlet energy transfer to the appended zinc porphyrin. As predicted from the energy levels, photoinduced electron transfer from both the singlet and triplet excited states of the zinc porphyrin to fullerene followed by subsequent hole migration involving ferrocene was witnessed from the transient absorption studies. The charge-separated state persisted for about 8.5 μs and was governed by the distance between the final charge-transfer product, that is, a species involving a ferrocenium cation and a fullerene radical anion, with additional influence from the charge-stabilizing triphenylamine entities located on the zinc-porphyrin macrocycle. Step-by-step events: Occurrence of sequential energy and electron transfer leading to the generation of a long-lived charge-separated state is demonstrated in a novel multimodular donor-acceptor supramolecular system comprised of different photo and redox entities as a photosynthetic-antenna/reaction-center mimic (see figure; EnT=energy transfer, CS=charge separation, HS=hole shift, CR=charge recombination).
机译：设计，合成并研究了以卟啉锌，富勒烯，二茂铁和三苯胺实体为特征的新型多模块供体-受体多聚体，作为电荷稳定的光合天线/反应中心模拟物。共价连接至卟啉环的二茂铁和富勒烯实体被远距离分离，以完成电荷分离/空穴迁移事件，从而导致了长寿命的电荷分离状态。通过B3LYP / 3-21G（*）优化推导了新合成化合物的几何结构和电子结构，同时利用光吸收和发射以及电化学研究的数据确定了不同光化学事件的能级。三苯胺实体的激发表明单重态-单重态能量转移至所附的卟啉锌。根据能级预测，从瞬态吸收研究中可以看出，光致电子从卟啉锌的单重态和三重态激发态转移到富勒烯，随后空穴迁移涉及二茂铁。电荷分离状态持续约8.5μs，并受最终电荷转移产物（即涉及二茂铁阳离子和富勒烯自由基阴离子的物质）之间的距离支配，并受位于其中的电荷稳定三苯胺实体的影响在锌卟啉大环上。循序渐进的事件：在新型多模态供体-受体超分子系统中证明了发生顺序能量和电子转移，导致长寿命的电荷分离状态的产生，该系统由不同的光和氧化还原实体组成，作为光合天线/反应中心模拟（参见图; EnT =能量转移，CS =电荷分离，HS =空穴移位，CR =电荷重组）。

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