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Perylene-Based Coordination Polymers: Synthesis, Fluorescent J-Aggregates, and Electrochemical Properties
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-05-08 , DOI: 10.1021/acs.inorgchem.3c00540 Gonçalo Valente 1 , María Esteve-Rochina 2 , Sergio P C Alves 3 , José M G Martinho 3 , Enrique Ortí 2 , Joaquín Calbo 2 , Filipe A Almeida Paz 1 , João Rocha 1 , Manuel Souto 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-05-08 , DOI: 10.1021/acs.inorgchem.3c00540 Gonçalo Valente 1 , María Esteve-Rochina 2 , Sergio P C Alves 3 , José M G Martinho 3 , Enrique Ortí 2 , Joaquín Calbo 2 , Filipe A Almeida Paz 1 , João Rocha 1 , Manuel Souto 1
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The incorporation of electroactive organic building blocks into coordination polymers (CPs) and metal–organic frameworks (MOFs) offers a promising approach for adding electronic functionalities such as redox activity, electrical conductivity, and luminescence to these materials. The incorporation of perylene moieties into CPs is, in particular, of great interest due to its potential to introduce both luminescence and redox properties. Herein, we present an innovative synthesis method for producing a family of highly crystalline and stable coordination polymers based on perylene-3,4,9,10-tetracarboxylate (PTC) and various transition metals (TMs = Co, Ni, and Zn) with an isostructural framework. The crystal structure of the PTC-TM CPs, obtained through powder X-ray diffraction and Rietveld refinement, provides valuable insights into the composition and organization of the building blocks within the CP. The perylene moieties are arranged in a herringbone pattern, with short distances between adjacent ligands, which contributes to the dense and highly organized framework of the material. The photophysical properties of PTC-Zn were thoroughly studied, revealing the presence of J-aggregation-based and monomer-like emission bands. These bands were experimentally identified, and their behavior was further understood through the use of quantum-chemical calculations. Solid-state cyclic voltammetry experiments on PTC-TMs showed that the perylene redox properties are maintained within the CP framework. This study presents a simple and effective approach for synthesizing highly stable and crystalline perylene-based CPs with tunable optical and electrochemical properties in the solid state.
中文翻译：
基于苝的配位聚合物：合成、荧光 J-聚集体和电化学性质
将电活性有机结构单元结合到配位聚合物 (CP) 和金属有机骨架 (MOF) 中，为向这些材料添加电子功能（如氧化还原活性、导电性和发光）提供了一种很有前途的方法。将苝部分结合到 CP 中尤其令人感兴趣，因为它有可能同时引入发光和氧化还原特性。在此，我们提出了一种创新的合成方法，用于生产基于 perylene-3,4,9,10-tetracarboxylate (PTC) 和各种过渡金属（TMs = Co、Ni 和 Zn）的一系列高度结晶且稳定的配位聚合物，其中同构框架。PTC-TM的晶体结构通过粉末 X 射线衍射和 Rietveld 精修获得的 CP 为了解 CP 中构建块的组成和组织提供了宝贵的见解。苝部分以人字形排列，相邻配体之间的距离很短，这有助于材料的致密和高度有序的框架。对PTC-Zn的光物理特性进行了深入研究，揭示了基于 J 聚集和类单体的发射带的存在。这些带是通过实验确定的，并且通过使用量子化学计算进一步了解了它们的行为。PTC-TM的固态循环伏安法实验表明苝的氧化还原特性在 CP 框架内得以保持。本研究提出了一种简单有效的方法来合成高度稳定的结晶苝基 CP，其在固态下具有可调的光学和电化学性质。
更新日期：2023-05-08
中文翻译：
基于苝的配位聚合物：合成、荧光 J-聚集体和电化学性质
将电活性有机结构单元结合到配位聚合物 (CP) 和金属有机骨架 (MOF) 中，为向这些材料添加电子功能（如氧化还原活性、导电性和发光）提供了一种很有前途的方法。将苝部分结合到 CP 中尤其令人感兴趣，因为它有可能同时引入发光和氧化还原特性。在此，我们提出了一种创新的合成方法，用于生产基于 perylene-3,4,9,10-tetracarboxylate (PTC) 和各种过渡金属（TMs = Co、Ni 和 Zn）的一系列高度结晶且稳定的配位聚合物，其中同构框架。PTC-TM的晶体结构通过粉末 X 射线衍射和 Rietveld 精修获得的 CP 为了解 CP 中构建块的组成和组织提供了宝贵的见解。苝部分以人字形排列，相邻配体之间的距离很短，这有助于材料的致密和高度有序的框架。对PTC-Zn的光物理特性进行了深入研究，揭示了基于 J 聚集和类单体的发射带的存在。这些带是通过实验确定的，并且通过使用量子化学计算进一步了解了它们的行为。PTC-TM的固态循环伏安法实验表明苝的氧化还原特性在 CP 框架内得以保持。本研究提出了一种简单有效的方法来合成高度稳定的结晶苝基 CP，其在固态下具有可调的光学和电化学性质。
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