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首页> 外文期刊>ACS applied materials & interfaces >Toward Metal Organic Framework-Based Solar Cells: Enhancing Directional Exciton Transport by Collapsing Three-Dimensional Film Structures
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Toward Metal Organic Framework-Based Solar Cells: Enhancing Directional Exciton Transport by Collapsing Three-Dimensional Film Structures

机译：迈向基于金属有机框架的太阳能电池：通过折叠三维薄膜结构来增强定向激子传输。

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Owing to their ability to act as light-harvesting scaffolds, porphyrin-containing metal-organic frameworks (MOFs) are in the forefront of research on the application of highly ordered molecular materials to problems in solar-energy conversion. In this work, solvent-assisted linker exchange (SALE) is performed on a pillared paddlewheel porphyrin containing MOF thin film to collapse a 3D framework to a 2D framework. The change in dimensionality of the framework is confirmed by a decrease in the film thickness, the magnitude of which is in agreement with crystallographic parameters for related bulk materials. Furthermore, NMR spectroscopy performed on the digested sample suggests a similar change in geometry is achieved in bulk MOF samples. The decreased distance between the porphyrin chromophores in the 2D MOF film compared to the 3D film results in enhanced energy transfer through the film. The extent of energy transport was probed by assembling MOF thin film where the outermost layers are palladium porphyrin (P2) units, which act as energy traps and fluorescence quenchers. Steady-state emission spectroscopy together with time-resolved emission spectroscopy indicates that excitons can travel through about 9-11 layers (porphyrin layers) in 2D films, whereas in 3D films energy transfer occurs through no more than about 6-8 layers. The results are difficult to understand if only changes in MOF interlayer spacing are considered but become much more understandable if dipole-dipole coupling distances are considered.
机译：含卟啉的金属有机骨架（MOF）由于具有光收集支架的功能，因此在研究将高度有序的分子材料应用于太阳能转换问题方面处于研究的最前沿。在这项工作中，在含MOF薄膜的带柱桨轮卟啉上进行溶剂辅助接头交换（SALE），以将3D框架折叠为2D框架。框架尺寸的变化由膜厚度的减小证实，膜厚度的减小与相关块状材料的晶体学参数一致。此外，对消化后的样品进行的NMR光谱分析表明，在批量MOF样品中实现了相似的几何形状变化。与3D膜相比，2D MOF膜中的卟啉生色团之间的距离减小，导致通过膜的能量传递增强。通过组装MOF薄膜（其中最外层是用作能量陷阱和荧光猝灭剂的钯卟啉（P2）单元）来探测能量传输的程度。稳态发射光谱和时间分辨发射光谱表明，激子可以穿过2D膜中的约9-11层（卟啉层），而在3D膜中，能量转移发生时不超过约6-8层。如果仅考虑MOF层间间距的变化，结果将难以理解，但如果考虑偶极-偶极耦合距离，结果将变得更加容易理解。

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