Highly Selective Carbonylation of CH3Cl to Acetic Acid Catalyzed by Pyridine-Treated MOR Zeolite

Author: Time:2022-06-02 Click:

Methane, the main component of natural gas, shale gas and flammable ice, is not only a clean and inexpensive chemical feedstock with abundant reserves, but also an alternative energy vector to petroleum. Nevertheless, the low efficiency of methane utilization has remained unresolved due to the high C-H band energy (439.3 kJ mol-1) and low polarizability of a methane molecule

Recently, a research team led by Prof. LIU Zhongmin and Prof. ZHU Wenliang developed a novel route for directly transforming CH3Cl to acetic acid through a carbonylation reaction using acidic zeolites as the catalyst.


Highly Selective Carbonylation of CH3Cl to Acetic Acid Catalyzed by Pyridine-Treated MOR Zeolite

 (Image by FANG Xudong)

The researchers used pyridine-treated MOR as catalysts to achieve high acetic acid and methyl acetate selectivity.They first demonstrated that the coupling of CH3Cl with CO and H2O occurred over acidic zeolites especially one-dimensional with 8-member ring(8 MR) or 10-member ring (10 MR). In particular, the high selectivity of acetic acid and methyl acetate reaching 99.3% could be obtained over pyridine-treated MOR under the optimized conditions, which was superior to that of Rh/AC under CH3I-free conditions. The Bronsted acid sites in 8MR has been proven to be the main active site for chloromethane carbonylation.

Moreover, with multiple characterizations, such as in situ DRIFT and isotope labeling experiments, the reaction mechanism was proposed, which includes the chemical adsorption of CH3Cl, the formation of acetyl groups, and the hydrolysis of acetyl groups.

“Our study would present enormous potential and advantages in the efficient and practical transformation of methane into oxygenates in the future.” said Prof. ZHU.

The study was supported by the National Natural Science Foundation of China,the Strategic Priority Research Program of CAS, the Dalian High-Level Talent Innovation Support Program, and National Special Support Program for High-Level Talents. (Text by FANG Xudong and LIU Hongchao)


Selective Carbonylation of CH3Cl to Acetic Acid Catalyzed by Pyridine-Treated MOR Zeolite. Xudong Fang,Fuli Wen,Xiangnong Ding,Hanbang Liu,Zhiyang Chen,Zhaopeng Liu,Hongchao Liu,Wenliang Zhu*,Zhongmin Liu, Angew. Chem. Int. Ed.,e202203859,2022.

Email:heshasha@dicp.ac.cn   Copyright Division of Low-Carbon Catalysis and Engineering,DICP, CAS