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CO Reduction to CH₃OSiMe₃: Electrophile-Promoted Hydride Migration at a Single Fe Site

Deegan, Meaghan M. and Peters, Jonas C. (2017) CO Reduction to CH₃OSiMe₃: Electrophile-Promoted Hydride Migration at a Single Fe Site. Journal of the American Chemical Society, 139 (7). pp. 2561-2564. ISSN 0002-7863. PMCID PMC5509333. doi:10.1021/jacs.6b12444.

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One of the major challenges associated with developing molecular Fischer–Tropsch catalysts is the design of systems that promote the formation of C–H bonds from H₂ and CO while also facilitating the release of the resulting CO-derived organic products. To this end, we describe the synthesis of reduced iron-hydride/carbonyl complexes that enable an electrophile-promoted hydride migration process, resulting in the reduction of coordinated CO to a siloxymethyl (L_nFe-CH₂OSiMe₃) group. Intramolecular hydride-to-CO migrations are extremely rare, and to our knowledge the system described herein is the first example where such a process can be accessed from a thermally stable M(CO)(H) complex. Further addition of H₂ to L_nFe-CH₂OSiMe₃ releases CH_₃OSiMe₃, demonstrating net four-electron reduction of CO to CH₃OSiMe₃ at a single Fe site.

Item Type:Article
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URLURL TypeDescription Information CentralArticle
Deegan, Meaghan M.0000-0002-7633-2074
Peters, Jonas C.0000-0002-6610-4414
Additional Information:© 2017 American Chemical Society. Received: December 2, 2016; Published: February 3, 2017. This work was supported by the NIH (GM070757) and the Gordon and Betty Moore Foundation. We thank Larry Henling and Mike Takase for assistance with crystallography. The authors declare no competing financial interest.
Funding AgencyGrant Number
Gordon and Betty Moore FoundationUNSPECIFIED
Issue or Number:7
PubMed Central ID:PMC5509333
Record Number:CaltechAUTHORS:20170213-121746843
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Official Citation:CO Reduction to CH3OSiMe3: Electrophile-Promoted Hydride Migration at a Single Fe Site Meaghan M. Deegan and Jonas C. Peters Journal of the American Chemical Society 2017 139 (7), 2561-2564 DOI: 10.1021/jacs.6b12444
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:74242
Deposited By: George Porter
Deposited On:13 Feb 2017 21:02
Last Modified:05 Apr 2022 17:52

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