Catalytic, oxidative condensation of CH4 to CH3COOH in one step via CH activation

被引：362

作者：

Periana, RA ^{[1
]}

Mironov, O ^{[1
]}

Taube, D ^{[1
]}

Bhalla, G ^{[1
]}

Jones, CJ ^{[1
]}

机构：

[1] Univ So Calif, Dept Chem, Loker Hydrocarbon Inst, Los Angeles, CA 90089 USA

来源：

SCIENCE | 2003年 / 301卷 / 5634期

关键词：

D O I：

10.1126/science.1086466

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页码：814 / 818

页数：5

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