Fang Xudong, Wen Fuli, Ding Xiangnong, Liu Hanbang, Chen Zhiyang, Liu Zhaopeng, Liu Hongchao, Zhu Wenliang, Liu Zhongmin
National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2022 Aug 1;61(31):e202203859. doi: 10.1002/anie.202203859. Epub 2022 Jun 15.
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 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.
在温和条件下将甲烷选择性转化为高附加值化学品对于甲烷的商业可行和可持续利用具有重要意义,但仍然是一项艰巨的挑战。在此,我们报道了一种通过CHCl作为中间体将甲烷高效转化为乙酸的策略。在523 K和2.0 MPa的温和条件下,吡啶预处理的丝光沸石(MOR-8)上乙酸和乙酸甲酯(AA+MA)的选择性高达99.3%。传统上对沸石催化剂上的羰基化反应有害的水,在当前反应体系中有利于AA的生成。在使用MOR-8催化剂的100小时连续测试中,AA+MA的平均选择性保持在98%以上。AA是由MOR八元环内的甲氧基羰基化然后水解形成的。该策略为在温和反应条件下将甲烷高效转化为含氧化合物提供了一种方法。