Synergy of Electrostatic and π-π Interactions in the Realization of Nanoscale Artificial Photosynthetic Model Systems.,Angewandte Chemie International Edition

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Synergy of Electrostatic and π-π Interactions in the Realization of Nanoscale Artificial Photosynthetic Model Systems.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-07-11 , DOI: 10.1002/anie.202006014
Eduardo Anaya-Plaza _{1,

2} , Jan Joseph ₃ , Stefan Bauroth ₃ , Maximilian Wagner ₃ , Christian Dolle ₃ , Michael Sekita ₃ , Franziska Gröhn ₃ , Erdmann Spiecker ₃ , Timothy Clark ₃ , Andrés de la Escosura _{1,

4} , Dirk M Guldi ₃ , Tomás Torres _{1,

4,

5}

Affiliation

In the scientific race to build up photoactive electron donor‐acceptor systems with increasing efficiencies, little is known about the interplay of their building blocks when integrated into supramolecular nanoscale arrays, particularly in aqueous environments. Here, we describe an aqueous donor‐acceptor ensemble whose emergence as a nanoscale material renders it remarkably stable and efficient. We have focused on a tetracationic zinc phthalocyanine (ZnPc) featuring pyrenes, which shows an unprecedented mode of aggregation, driven by subtle cooperation between electrostatic and π–π interactions. Our studies demonstrate monocrystalline growth in solution and a symmetry‐breaking intermolecular charge transfer between adjacent ZnPcs upon photoexcitation. Immobilizing a negatively charged fullerene (C₆₀) as electron acceptor onto the monocrystalline ZnPc assemblies was found to enhance the overall stability, and to suppress the energy‐wasting charge recombination found in the absence of C₆₀. Overall, the resulting artificial photosynthetic model system exhibits a high degree of preorganization, which facilitates efficient charge separation and subsequent charge transport.

中文翻译：

静电和π-π相互作用在纳米级人工光合模型系统实现中的协同作用。

在建立效率不断提高的光敏电子供体-受体系统的科学竞赛中，人们对它们的构建模块在集成到超分子纳米级阵列中时的相互作用知之甚少，特别是在水环境中。在这里，我们描述了一种水性供体-受体整体，其作为纳米级材料的出现使其非常稳定和高效。我们专注于以芘为特征的四阳离子锌酞菁（ZnPc），它表现出前所未有的聚集模式，由静电和π-π相互作用之间的微妙合作驱动。我们的研究证明了溶液中的单晶生长以及光激发时相邻 ZnPc 之间对称性破坏的分子间电荷转移。研究发现，将带负电的富勒烯 (C ₆₀ ) 作为电子受体固定到单晶 ZnPc 组件上可以增强整体稳定性，并抑制在不存在 C ₆₀的情况下发现的浪费能量的电荷重组。总体而言，所得的人工光合作用模型系统表现出高度的预组织性，这有利于有效的电荷分离和随后的电荷传输。

更新日期：2020-07-11

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