Highly Selective Carbonylation of CH3Cl to Acetic Acid Catalyzed by Pyridine‐Treated MOR Zeolite. (15th June 2022)

• Record Type: Journal Article
• Authors: Fang, Xudong; Wen, Fuli; Ding, Xiangnong; Liu, Hanbang; Chen, Zhiyang; Liu, Zhaopeng; Liu, Hongchao; Zhu, Wenliang; Liu, Zhongmin
• Is Part Of: Angewandte Chemie. Volume 134:Number 31(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-06-15
• Subjects: Carbon Monoxide -- Carbonylation -- Chloromethane -- Methane Conversion -- Mordenite; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202203859
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: The selective conversion of methane to high value‐added chemicals under mild conditions is of great significance for the commercially viable and sustainable utilization of methane but remains a formidable challenge. Herein, we report a strategy for efficiently converting methane to acetic acid via CH3 Cl as an intermediate. Up to 99.3 % acetic acid and methyl acetate (AA+MA) selectivity was achieved over pyridine‐pretreated MOR (MOR‐8) under moderate conditions of 523 K and 2.0 MPa. Water, conventionally detrimental to carbonylation reaction over zeolite catalysts, was conducive to the production of AA in the current reaction system. In the 100 h continuous test with the MOR‐8 catalyst, the average AA+MA selectivity remained over 98 %. AA was formed by carbonylation of methoxy groups within 8‐membered rings of MOR followed by hydrolysis. This strategy provided an approach for highly efficient utilization of methane to oxygenates under mild reaction conditions. Abstract : An innovative reaction strategy for the transformation of methane into acetic acid via CH3 Cl carbonylation over H‐zeolites is reported. A 99.3 % acetic acid (AA) and methyl acetate (MA) selectivity was obtained over pyridine‐pretreated MOR at 523 K and 2.0 MPa. This strategy enables efficient conversion of methane into oxygenates under mild conditions.