Stabilizing Isolated Rhodium Cations by MFI Zeolite for Heterogeneous Methanol Carbonylation
Weixiang Shang, Mingyang Gao, Yuchao Chai, Guangjun Wu, Naijia Guan, Landong Li
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 zeolite-stabilized [Rh(CO)2I2] 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 molacetyl/(molRh 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.