期刊
NATURE CHEMISTRY
卷 3, 期 4, 页码 287-290出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1001
关键词
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资金
- Robert A. Welch Foundation [F-0038]
- Texas Higher Education Coordinating Board [01849]
- University of Texas Center for Green Chemistry and Catalysis
- National Science Foundation [CHE-1021640]
- Natural Sciences and Engineering Research Council of Canada
- German Research Foundation
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1021640] Funding Source: National Science Foundation
Methanol is an abundant (35 million metric tons per year), renewable chemical feedstock, yet its use as a one-carbon building block in fine chemical synthesis is highly underdeveloped. Using a homogeneous iridium catalyst developed in our laboratory, methanol engages in a direct C-C coupling with allenes to furnish higher alcohols that incorporate all-carbon quaternary centres, free of stoichiometric by-products. A catalytic mechanism that involves turnover-limiting methanol oxidation, a consequence of the high energetic demand of methanol dehydrogenation, is corroborated through a series of competition kinetics experiments. This process represents the first catalytic C-C coupling of methanol to provide discrete products of hydrohydroxymethylation.
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