Li Yingguo, He Jialun, Lu Guilong, Wang Chensheng, Fu Mengmeng, Deng Juan, Yang Fu, Jiang Danfeng, Chen Xiao, Yu Ziyi, Liu Yan, Yu Chao, Cui Yong
School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212003, China.
State Key Laboratory of Materials-oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 211816, China.
Nat Commun. 2024 Aug 15;15(1):7044. doi: 10.1038/s41467-024-51431-5.
Microflow catalysis is a cutting-edge approach to advancing chemical synthesis and manufacturing, but the challenge lies in developing efficient and stable multiphase catalysts. Here we showcase incorporating amine-containing metal-organic cages into automated microfluidic reactors through covalent bonds, enabling highly continuous flow catalysis. Two FeL tetrahedral cages bearing four uncoordinated amines were designed and synthesized. Post-synthetic modifications of the amine groups with 3-isocyanatopropyltriethoxysilane, introducing silane chains immobilized on the inner walls of the microfluidic reactor. The immobilized cages prove highly efficient for the reaction of anthranilamide with aldehydes, showing superior reactivity and recyclability relative to free cages. This superiority arises from the large cavity, facilitating substrate accommodation and conversion, a high mass transfer rate and stable covalent bonds between cage and microreactor. This study exemplifies the synergy of cages with microreactor technology, highlighting the benefits of heterogenous cages and the potential for future automated synthesis processes.
微流催化是推动化学合成与制造的前沿方法，但挑战在于开发高效且稳定的多相催化剂。在此，我们展示了通过共价键将含胺金属有机笼引入自动化微流反应器，实现高度连续的流动催化。设计并合成了两个带有四个未配位胺的FeL四面体笼。用3-异氰酸酯基丙基三乙氧基硅烷对胺基进行后合成修饰，引入固定在微流反应器内壁的硅烷链。固定化的笼对邻氨基苯甲酰胺与醛的反应证明非常高效，相对于游离笼显示出优异的反应活性和可回收性。这种优越性源于大的空腔，有利于底物容纳和转化、高传质速率以及笼与微反应器之间稳定的共价键。本研究例证了笼与微反应器技术的协同作用，突出了异质笼的优势以及未来自动化合成过程的潜力。
