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Sophisticated Design of Covalent Organic Frameworks with Controllable Bimetallic Docking for a Cascade Reaction

机译:可控双金属对接反应的共价有机骨架的精密设计

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摘要

Precise control of the number and position of the catalytic metal ions in heterogeneous catalysts remains a big challenge. Here we synthesized a series of two-dimensional (2D) covalent organic frameworks (COFs) containing two different types of nitrogen ligands, namely imine and bipyridine, with controllable contents. For the first time, the selective coordination of the two nitrogen ligands of the 2D COFs to two different metal complexes, chloro(1,5-cyclooctadiene)rhodium(I) (Rh(COD) Cl) and palladium(II) acetate (Pd(OAc)(2)), has been realized using a programmed synthetic procedure. The bimetallically docked COFs showed excellent catalytic activity in a one-pot addition-oxidation cascade reaction. The high surface area, controllable metal-loading content, and predesigned active sites make them ideal candidates for their use as heterogeneous catalysts in a wide range of chemical reactions.
机译:精确控制非均相催化剂中催化金属离子的数量和位置仍然是一个巨大的挑战。在这里,我们合成了一系列二维(2D)共价有机骨架(COF),其中包含两种不同类型的氮配体,即亚胺和联吡啶,含量可控。首次将2D COF的两个氮配体与两种不同的金属络合物(氯(1,5-环辛二烯)铑(I)(Rh(COD)Cl)和乙酸钯(II))进行选择性配位(OAc)(2)),已使用编程的合成程序实现。双金属对接的COF在一锅加成-氧化级联反应中显示出出色的催化活性。高表面积,可控制的金属负载量以及预先设计的活性位点使其成为在各种化学反应中用作多相催化剂的理想候选者。

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