Alsudairy Ziad, Campbell Allea, Zheng Qi, Harrod Chelsea, Brown Normanda, Saintilma Allison, Maligal-Ganesh Raghu V, Ingram Conrad, Li Xinle
Department of Chemistry, Clark Atlanta University, Atlanta, Georgia, 30314, United States.
Department of Chemistry, College of Science, Qassim University, Buraidah, 51452, Saudi Arabia.
Chemistry. 2024 Dec 18;30(71):e202402513. doi: 10.1002/chem.202402513. Epub 2024 Nov 7.
Metal-encapsulated covalent organic frameworks (metal/COFs) represent an emerging paradigm in heterogeneous catalysis. However, the time-intensive (usually 4 or more days) and tedious multi-step synthesis of metal/COFs remains a significant stumbling block for their broad application. To address this challenge, we introduce a facile microwave-assisted in situ metal encapsulation strategy to cooperatively combine COF formation and in situ palladium(II) encapsulation in one step. With this unprecedented approach, we synthesize a diverse range of palladium(II)-encapsulated COFs (termed Mw-Pd/COF) in the air within just an hour. Notably, this strategy is scalable for large-scale production (~0.5 g). Leveraging the high crystallinity, porosity, and structural stability, one representative Mw-Pd/COF exhibits remarkable activity, functional group tolerance, and recyclability for the Suzuki-Miyaura coupling reaction at room temperature, surpassing most previously reported Pd(II)/COF catalysts with respect to catalytic performance, preparation time, and synthetic ease. This microwave-assisted in situ metal encapsulation strategy opens a facile and rapid avenue to construct metal/COF hybrids, which hold enormous potential in a multitude of applications including heterogeneous catalysis, sensing, and energy storage.
金属封装的共价有机框架材料（金属/共价有机框架材料）代表了多相催化领域中一种新兴的模式。然而，金属/共价有机框架材料耗时较长（通常为4天或更长时间）且繁琐的多步合成方法仍然是其广泛应用的一个重大障碍。为应对这一挑战，我们引入了一种简便的微波辅助原位金属封装策略，将共价有机框架材料的形成与钯（II）的原位封装一步协同完成。通过这种前所未有的方法，我们仅在一小时内就在空气中合成了多种钯（II）封装的共价有机框架材料（称为Mw-Pd/COF）。值得注意的是，该策略可扩展用于大规模生产（约0.5克）。利用其高结晶度、孔隙率和结构稳定性，一种具有代表性的Mw-Pd/COF在室温下对铃木-宫浦偶联反应表现出显著的活性、官能团耐受性和可回收性，在催化性能、制备时间和合成简便性方面超过了大多数先前报道的钯（II）/共价有机框架材料催化剂。这种微波辅助原位金属封装策略为构建金属/共价有机框架材料杂化体开辟了一条简便快捷的途径，这类杂化体在多相催化、传感和能量存储等众多应用中具有巨大潜力。
