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La-Metal-Organic Framework incorporating Fe3O4 nanoparticles, post-synthetically modified with Schiff base and Pd. A highly active, magnetically recoverable, recyclable catalyst for CC cross-couplings at low Pd loadings
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-03-16 , DOI: 10.1016/j.jcat.2018.02.026
Gang Xiong , Xiao-Ling Chen , Li-Xin You , Bao-Yi Ren , Fu Ding , Ileana Dragutan , Valerian Dragutan , Ya-Guang Sun

Unprecedented post-synthetic modification (PSM) applied on a new La-MOF containing Fe3O4 nanoparticles (NPs), via Schiff base build-up (with pyridine-2-carboxaldehyde) and PdCl2 coordination, proved to be an advantageous strategy to produce a superior heterogeneous catalyst for Suzuki-Miyaura CC bond formation. The Fe3O4@La-MOF-Schiff base-Pd ensemble (characterized by PXRD, EDS, TEM, HAADF-STEM, VSM, TGA) showed very active, quite stable, magnetically recoverable and reusable in coupling of bromo- or iodoaryls with arylboronic acids, affording practically quantitative yields of biaryls (>99%) and high TONs and TOFs. The catalyst has been recycled up to 12 times without significant loss of the catalytic activity. A synergistic cooperativity between Pd and the oxophilic La nodes, through the organic linker, is responsible for enhancing the catalyst activity and stability.



中文翻译:

包含Fe 3 O 4纳米粒子的La-Metal-Organic框架,经过Schiff碱和Pd合成后修饰。高活性,可磁回收,可循环利用的催化剂,可在低Pd负载下进行C C交叉偶联

前所未有的合成后修饰(PSM)通过Schiff碱堆积(与吡啶-2-甲醛)和PdCl 2配位作用于包含Fe 3 O 4纳米颗粒(NPs)的新型La-MOF ,被证明是一种有利的策略生产铃木-宫浦C C键形成的优异多相催化剂。铁3 O 4@ La-MOF-Schiff碱-钯系化合物(由PXRD,EDS,TEM,HAADF-STEM,VSM,TGA表征)在溴或碘代芳基与芳基硼酸的偶联中表现出非常活跃,非常稳定,可磁回收和可重复使用的特性,从而提供了联芳基(> 99%)以及高TON和TOF的实际定量收率。催化剂已循环使用多达12次,而催化活性没有明显损失。通过有机连接基,Pd和亲氧性La节点之间的协同协同作用可增强催化剂的活性和稳定性。

更新日期:2018-03-16
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