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Bridging the Homogeneous and Heterogeneous Catalysis by Supramolecular Metal-Organic Cages with Varied Packing Modes
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-16 , DOI: 10.1002/adma.202310061 Liang Kan 1 , Lei Zhang 1 , Long-Zhang Dong 1 , Xiao-Han Wang 1 , Run-Han Li 1 , Chenxing Guo 2 , Xiaopeng Li 2 , Yong Yan 1 , Shun-Li Li 1 , Ya-Qian Lan 1
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-16 , DOI: 10.1002/adma.202310061 Liang Kan 1 , Lei Zhang 1 , Long-Zhang Dong 1 , Xiao-Han Wang 1 , Run-Han Li 1 , Chenxing Guo 2 , Xiaopeng Li 2 , Yong Yan 1 , Shun-Li Li 1 , Ya-Qian Lan 1
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Integrating the advantages of homogeneous and heterogeneous catalysis has proved to be an optimal strategy for developing catalytic systems with high efficiency, selectivity, and recoverability. Supramolecular metal-organic cages (MOCs), assembled by the coordination of metal ions with organic linkers into discrete molecules, have performed solvent processability due to their tunable packing modes, endowing them with the potential to act as homogeneous or heterogeneous catalysts in different solvent systems. Here, the design and synthesis of a series of stable {Cu3} cluster-based tetrahedral MOCs with varied packing structures are reported. These MOCs, as homogeneous catalysts, not only show high catalytic activity and selectivity regardless of substrate size during the CO2 cycloaddition reaction, but also can be easily recovered from the reaction media through separating products and co-catalysts by one-step work-up. This is because that these MOCs have varied solubilities in different solvents due to the tunable packing of MOCs in the solid state. Moreover, the entire catalytic reaction system is very clean, and the purity of cyclic carbonates is as high as 97% without further purification. This work provides a unique strategy for developing novel supramolecular catalysts that can be used for homogeneous catalysis and recycled in a heterogeneous manner.
中文翻译：
不同填充方式的超分子金属有机笼连接均相和多相催化
整合均相和多相催化的优点已被证明是开发具有高效率、选择性和可回收性的催化体系的最佳策略。超分子金属有机笼（MOC）通过金属离子与有机连接体配位组装成离散分子，由于其可调节的堆积模式而具有溶剂可加工性，赋予它们在不同溶剂体系中作为均相或非均相催化剂的潜力。在此，报道了一系列具有不同堆积结构的稳定的基于{Cu 3 }簇的四面体MOC的设计和合成。这些MOC作为均相催化剂，不仅在CO 2环加成反应过程中无论底物尺寸如何都表现出高催化活性和选择性，而且可以通过一步后处理分离产物和助催化剂，轻松从反应介质中回收。这是因为由于固态 MOC 的堆积可调，这些 MOC 在不同溶剂中具有不同的溶解度。而且整个催化反应体系非常干净，无需进一步纯化，环状碳酸酯纯度高达97%。这项工作为开发新型超分子催化剂提供了一种独特的策略，该催化剂可用于均相催化并以非均相方式回收。
更新日期：2024-01-16
中文翻译：
不同填充方式的超分子金属有机笼连接均相和多相催化
整合均相和多相催化的优点已被证明是开发具有高效率、选择性和可回收性的催化体系的最佳策略。超分子金属有机笼（MOC）通过金属离子与有机连接体配位组装成离散分子，由于其可调节的堆积模式而具有溶剂可加工性，赋予它们在不同溶剂体系中作为均相或非均相催化剂的潜力。在此，报道了一系列具有不同堆积结构的稳定的基于{Cu 3 }簇的四面体MOC的设计和合成。这些MOC作为均相催化剂，不仅在CO 2环加成反应过程中无论底物尺寸如何都表现出高催化活性和选择性，而且可以通过一步后处理分离产物和助催化剂，轻松从反应介质中回收。这是因为由于固态 MOC 的堆积可调，这些 MOC 在不同溶剂中具有不同的溶解度。而且整个催化反应体系非常干净，无需进一步纯化，环状碳酸酯纯度高达97%。这项工作为开发新型超分子催化剂提供了一种独特的策略，该催化剂可用于均相催化并以非均相方式回收。
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