Catalytic, Oxidative Condensation of CH₄ to CH₃COOH in One Step via CH Activation
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$180\textdegree C$in liquid sulfuric acid. Carbon-13...
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| Veröffentlicht in: | Science (American Association for the Advancement of Science) 2003-08, Vol.301 (5634), p.814-818 |
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| container_issue | 5634 |
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| container_title | Science (American Association for the Advancement of Science) |
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| creator | Periana, Roy A. Mironov, Oleg Taube, Doug Bhalla, Gaurav Jones, C. J. |
| description | 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$180\textdegree C$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$Pd-CH_3$species, followed by efficient oxidative carbonylation with methanol, generated in situ from methane, to produce acetic acid. |
| doi_str_mv | 10.1126/science.1086466 |
| format | Article |
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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$Pd-CH_3$species, followed by efficient oxidative carbonylation with methanol, generated in situ from methane, to produce acetic acid.</description><identifier>ISSN: 0036-8075</identifier><identifier>EISSN: 1095-9203</identifier><identifier>DOI: 10.1126/science.1086466</identifier><identifier>PMID: 12907796</identifier><identifier>CODEN: SCIEAS</identifier><language>eng</language><publisher>Washington, DC: American Association for the Advancement of Science</publisher><subject>Carboxylic acids ; Catalysis ; Catalysts ; Chemistry ; Condensation ; Crystals ; Exact sciences and technology ; General and physical chemistry ; Methane ; Molecules ; Oxidation ; Polymers ; Sulfuric acids ; Theory of reactions, general kinetics. Catalysis. 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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$Pd-CH_3$species, followed by efficient oxidative carbonylation with methanol, generated in situ from methane, to produce acetic acid.</description><subject>Carboxylic acids</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Condensation</subject><subject>Crystals</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Methane</subject><subject>Molecules</subject><subject>Oxidation</subject><subject>Polymers</subject><subject>Sulfuric acids</subject><subject>Theory of reactions, general kinetics. Catalysis. 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| ispartof | Science (American Association for the Advancement of Science), 2003-08, Vol.301 (5634), p.814-818 |
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| source | American Association for the Advancement of Science; Jstor Complete Legacy |
| subjects | Carboxylic acids Catalysis Catalysts Chemistry Condensation Crystals Exact sciences and technology General and physical chemistry Methane Molecules Oxidation Polymers Sulfuric acids Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolites |
| title | Catalytic, Oxidative Condensation of CH₄ to CH₃COOH in One Step via CH Activation |
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