Catalytic, oxidative condensation of CH4 to CH3COOH in one step via CH activation
Catalytic, oxidative condensation of CH4 to CH3COOH in one step via CH activation
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DOI：
10.1126/science.1086466
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发表时间：
2003-08-08
期刊：
影响因子：
56.9
通讯作者：
Jones, CJ
中科院分区：
文献类型：
--
作者：
Periana, RA;Mironov, O;Jones, CJ
乙酸是一种重要的石油化工产品，目前主要由甲烷（或煤）通过甲醇羰基化的三步法生产。本文报道了在180 ℃下，在液态硫酸中，两个甲烷分子直接选择性氧化缩合生成乙酸的反应。碳-13同位素标记研究表明，乙酸的两个碳都来自甲烷。该反应由钯催化，并且结果与通过串联催化发生的反应一致，所述串联催化涉及甲烷C-H活化以生成Pd-CH 3物质，然后用甲醇进行有效的氧化羰基化，由甲烷原位生成，以产生乙酸。
Acetic acid is an important petrochemical that is currently produced from methane ( or coal) in a three-step process based on carbonylation of methanol. We report a direct, selective, oxidative condensation of two methane molecules to acetic acid at 180 degreesC in liquid sulfuric acid. Carbon-13 isotopic labeling studies show that both carbons of acetic acid originate from methane. The reaction is catalyzed by palladium, and the results are consistent with the reaction occurring by tandem catalysis, involving methane C-H activation to generate Pd-CH3 species, followed by efficient oxidative carbonylation with methanol, generated in situ from methane, to produce acetic acid.