羰基化
吡啶
催化作用
沸石
醋酸
化学
选择性
甲烷
醋酸甲酯
氧合物
醋酸酐
水解
有机化学
一氧化碳
作者
Xudong Fang,Fuli Wen,Xiangnong Ding,Hanbang Liu,Zhiyang Chen,Zhao‐Peng Liu,Hongchao Liu,Wenliang Zhu,Zhongmin Liu
标识
DOI:10.1002/ange.202203859
摘要
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 CH 3 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.
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