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Continuous-flow organic transformations using immobilized catalysts are crucial for green and sustainable chemistry. Cross-linked polymer ligands offer high stability, ease of recovery through filtrat...ion, and thus enhance performance in continuous-flow reactions via transition-metal catalysis. Additionally, the cross-linking structure of the polymer support creates a unique reaction platform that controls the coordination behavior of the supported ligands and stabilizes the metal catalysts. However, insights into the material-based design for preparing highly active and durable immobilized metal catalysts are still limited. In this report, we propose a straightforward approach to boost both selective mono-coordination and effective stabilization of metal complexes. We developed threefold cross-linked polystyrene-triphenylphosphine hybrid monoliths with cross-linking structures adjusted by varying the content of divinylbenzene as co-cross-linker. The coordination behaviors and metal-support interactions of these monoliths were evaluated, highlighting the importance of co-cross-linker content in site-isolating phosphine units and stabilizing metal centers via arene-metal interactions on the polystyrene network. By optimizing the cross-linking structure, the monolith catalysts demonstrated exceptionally high catalytic activity and durability in Pd-catalyzed C-Cl transformations, such as Suzuki-Miyaura cross-couplings and Buchwald-Hartwig aminations in continuous flow. This underscores the utility of our monolith system in challenging transition-metal catalysis.続きを見る
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Mendeley出力
