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Rapid, Mild, and Catalytic Synthesis of 2D and 3D COFs with Promising Supercapacitor Applications
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-12-12 , DOI: 10.1021/acsaem.3c01913
Amir Khojastehnezhad 1 , Khaled Rhili 1 , Mohammad K. Shehab 2 , Hichem Gamraoui 1 , Zhiyuan Peng 1 , Ahmad Samih ElDouhaibi 3 , Rachid Touzani 4 , Belkheir Hammouti 5 , Hani M. El-Kaderi 2 , Mohamed Siaj 1
Affiliation  

An approach based on Keggin heteropoly acids (HPAs) has been presented for the mild and fast synthesis of five different structures of imine and azine-linked two-dimensional (2D) and three-dimensional (3D) covalent organic frameworks (COFs). Traditionally, these crystalline materials have been synthesized via the Schiff base polycondensation reaction between different aldehydes and amines under harsh conditions and in the presence of acetic acid. Herein, two different Keggin-type heteropolyacids (HPAs) have been exploited as catalysts which are both Bronsted and Lewis acids to speed up the synthesis of 2D and 3D COFs and improve their materials quality. The catalyst led to the preparation of the imine and azine-linked COFs with high crystallinity and porosity under mild conditions and short reaction time. According to the results, the amine building blocks with two amine functional groups formed the COFs with higher crystallinity, porosity, and yield compared to amine with three functional groups and nonplanar structures. On this basis, under mild reaction conditions, a 2D COF named TAPA-TPT was successfully prepared with high crystallinity and good porosity. The developed TAPA-TPT COF exhibits a very good performance when used in supercapacitor applications. This COF showed excellent specific capacitance of 205 F g–1 at a current density of 0.5 A g–1, which is a very attractive value for supercapacitors. This study provides a synthetic approach that can lead to large-scale production of COF materials for energy harvesting.

中文翻译:

快速、温和催化合成 2D 和 3D COF 具有广阔的超级电容器应用前景

提出了一种基于 Keggin 杂多酸 (HPA) 的方法,用于温和快速合成五种不同结构的亚胺和吖嗪连接的二维 (2D) 和三维 (3D) 共价有机框架 (COF)。传统上,这些结晶材料是通过不同醛和胺之间在恶劣条件下和乙酸存在下的席夫碱缩聚反应合成的。在此,两种不同的Keggin型杂多酸(HPA)被用作催化剂,它们都是布朗斯台德酸和路易斯酸,以加速2D和3D COF的合成并提高其材料质量。该催化剂可以在温和的条件和较短的反应时间下制备出具有高结晶度和孔隙率的亚胺和吖嗪连接的COF。结果表明,与具有三个官能团和非平面结构的胺相比,具有两个胺官能团的胺结构单元形成的COF具有更高的结晶度、孔隙率和产率。在此基础上,在温和的反应条件下,成功制备了结晶度高、孔隙率好的二维COF,命名为TAPA-TPT。所开发的TAPA-TPT COF在超级电容器应用中表现出非常好的性能。这种COF在0.5 A g –1的电流密度下表现出205 F g –1的优异比电容,这对于超级电容器来说是一个非常有吸引力的值。这项研究提供了一种合成方法,可以大规模生产用于能量收集的 COF 材料。
更新日期:2023-12-12
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