Well-defined discrete metal-organic cages have been widely explored in the field of supramolecular catalysis. However, these metal-organic cages have been rarely explored as heterogeneous catalysts for one-pot reactions. Herein, we present the first successful confinement self-assembly of (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO)-containing metal-organic cages within amino-functionalized mesoporous carbon to realize a new family of bifunctional heterogeneous catalyst (Cage@FDU-ED) for one-pot reactions. The orthogonal features of the isolated catalytically active sites within the obtained bifunctional catalyst lead to enhanced catalytic activities, selectivity, and recyclability with the overall transformation yielding up to 96% conversion. These results demonstrate that continuous chemical transformation with high efficiency is possible through careful design of catalytic sites in both metal-organic cages and mesoporous matrix isolatedly. This study paves a new way toward metal-organic cages as a promising platform for heterogeneous sequential reactions.

在超分子催化领域中已经广泛探索了定义明确的离散金属有机笼。但是，这些金属有机笼子很少被用作一锅反应的多相催化剂。在这里，我们介绍了氨基官能化介孔碳内含（2,2,6,6-四甲基哌啶-1-基）氧基（TEMPO）的金属有机笼的首次成功的封闭自组装，以实现一个新的双官能团非均相催化剂（Cage @ FDU-ED）进行一锅反应。所获得的双功能催化剂中分离的催化活性位点的正交特征导致增强的催化活性，选择性和可回收性，总转化率可达到96％。这些结果表明，通过精心设计分离的金属有机笼和中孔基质中的催化位点，可以实现连续高效的化学转化。这项研究为金属有机笼子铺平了道路，将其作为异质顺序反应的有前途的平台。