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Development and mechanistic investigation of the manganese(iii) salen-catalyzed dehydrogenation of alcohols
Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark..
Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-1553-4027
Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark..ORCID iD: 0000-0002-2576-1004
2019 (English)In: Chemical Science, ISSN 2041-6520, E-ISSN 2041-6539, Vol. 10, no 4, p. 1150-1157Article in journal (Refereed) Published
Abstract [en]

The first example of a manganese(III) catalyst for the acceptorless dehydrogenation of alcohols is presented. N,N'-Bis(salicylidene)-1,2-cyclohexanediaminomanganese(III) chloride (2) has been shown to catalyze the direct synthesis of imines from a variety of alcohols and amines with the liberation of hydrogen gas. The mechanism has been investigated experimentally with labelled substrates and theoretically with DFT calculations. The results indicate a metal-ligand bifunctional pathway in which both imine groups in the salen ligand are first reduced to form a manganese(III) amido complex as the catalytically active species. Dehydrogenation of the alcohol then takes place by a stepwise outer-sphere hydrogen transfer generating a manganese(III) salan hydride from which hydrogen gas is released.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2019. Vol. 10, no 4, p. 1150-1157
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Chemical Sciences
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URN: urn:nbn:se:kth:diva-244112DOI: 10.1039/c8sc03969kISI: 000457342200020Scopus ID: 2-s2.0-85060677462OAI: oai:DiVA.org:kth-244112DiVA, id: diva2:1289762
Note

QC 20190219

Available from: 2019-02-19 Created: 2019-02-19 Last updated: 2019-02-19Bibliographically approved

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Ahlquist, Mårten S. G.

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