Journal
ORGANOMETALLICS
Volume 41, Issue 19, Pages 2678-2687Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.organomet.2c00261
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Funding
- National Science Foundation [CHE-2154878]
- North Carolina Biotechnology Center grant: NCBC [2019-IDG-1010]
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A new family of air-stable Re and Mn complexes with bidentate NNS ligands was introduced, and their performance and reaction mechanism as aldehyde hydrogenation catalysts were studied.
A new family of air-stable Re and Mn complexes bearing bidentate NNS (ENENES) ligands with the general formula E(CH2)2NH(CH)2SR (E =-NC4H8O or-NC5H10, R = Ph or thiophenyl) is introduced. All Re and Mn complexes were catalysts for the hydrogenation of aldehydes. The Mn catalysts were active at milder conditions. A rhenium-hydride complex, featuring cis Re-H and N- H moieties, was isolated to provide an insight into the mechanism for this reaction. DFT (B3PW91-D3) and experimental data suggest that there are two pathways for this system, with and without the presence of the base (t-BuOK). The pathway that included t-BuOK was lower in energy, providing a greater driving force for the overall reaction.
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