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Acceptorless dehydrogenation of small molecules through cooperative base metal catalysis

Author(s): West, Julian G.; Huang, David; Sorensen, Erik J.

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Abstract: The dehydrogenation of unactivated alkanes is an important transformation both in industrial and biological systems. Recent efforts towards this reaction have revolved around high temperature, organometallic C–H activation by noble metal catalysts that produce alkenes and hydrogen gas as the sole products. Conversely, natural desaturase systems proceed through stepwise hydrogen atom transfer at physiological temperature; however, these transformations require a terminal oxidant. Here we show combining tetra-n-butylammonium decatungstate (TBADT) and cobaloxime pyridine chloride (COPC) can catalytically dehydrogenate unactivated alkanes and alcohols under near-UV irradiation at room temperature with hydrogen as the sole by-product. This noble metal-free process follows a nature-inspired pathway of high- and low-energy hydrogen atom abstractions. The hydrogen evolution ability of cobaloximes is leveraged to render the system catalytic, with cooperative turnover numbers up to 48 and yields up to 83%. Our results demonstrate how cooperative base metal catalysis can achieve transformations previously restricted to precious metal catalysts.
Publication Date: Dec-2015
Electronic Publication Date: 11-Dec-2015
Citation: West, Julian G., Huang, David, Sorensen, Erik J. (2015). Acceptorless dehydrogenation of small molecules through cooperative base metal catalysis. Nature Communications, 6 (1), 10.1038/ncomms10093
DOI: doi:10.1038/ncomms10093
EISSN: 2041-1723
Pages: 6.10093:1-7
Type of Material: Journal Article
Journal/Proceeding Title: Nature Communications
Version: Final published version. This is an open access article.



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