Stabilizing isolated rhodium cations by MFI zeolite for heterogeneous methanol carbonylation

···材料科学与工程学院-中文···

论文题目:Stabilizing isolated rhodium cations by MFI zeolite for heterogeneous methanol carbonylation

论文作者:Weixiang Shang, Mingyang Gao, Yuchao Chai, Guangjun Wu,
Naijia Guan, Landong Li*

发表期刊:ACS Catalysis, 11(12), 7249-7256, 2021    

Abstract: 

Methanol carbonylation is known as a classic reaction of homogeneous  catalysis with large-scale industrial applications. The heterogenization  of homogeneous catalysts is being pursued to address the issues of  catalyst deactivation and separation encountered in homogeneous systems.  Herein, we report the strategy of stabilizing isolated rhodium cations  by MFI zeolite to construct highly active Rh@MFI zeolite catalysts for  heterogeneous methanol carbonylation. The formation of a  zeolitestabilized [Rh(CO)(2)I-2] analogue during the reaction has been  identified to catalyze methanol carbonylation. Moreover, the structure  of the zeolite can significantly promote methanol carbonylation within  channels through electronic confinment. As a result, a state of the art  turnover frequency of 3950 mol(acetyl)/(mol(Rh) h) is achieved with the  Rh@ZSM-5 catalyst at a low reaction temperature of 423 K. This work  presents a simple and general approach toward the heterogenization of  homogeneous catalysts for targeted chemical transformations.

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