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A Highly Active Bidentate Magnesium Catalyst for Amine‐Borane Dehydrocoupling: Kinetic and Mechanistic Studies

Ried, Alexander; Taylor, Laurence; Geer, Ana; Williams, Huw; Lewis, William; Blake, Alexander; Kays, Deborah Lorraine

Authors

Alexander Ried

Ana Geer

William Lewis

Alexander Blake

DEBORAH KAYS deborah.kays@nottingham.ac.uk
Professor of Inorganic Chemistry



Abstract

A magnesium complex (1) featuring a bidentate aminopyridinato ligand is a remarkably selective catalyst for the dehydrocoupling of amine-boranes. This reaction proceeds to completion with low catalyst loadings (1 mol%) under mild conditions (60 °C), exceeding previously reported s-block systems in terms of selectivity, rate, and turnover number (TON). Mechanistic studies by in situNMR analysis reveals the reaction to be firstorder in both catalyst and substrate. A reaction mechanism is proposed to account for these findings, with the high TON of the catalyst attributed to the bidentate nature of the ligand, which allows for reversible deprotonation of the substrate and regeneration of 1as a stable resting state.

Journal Article Type Article
Publication Date May 10, 2019
Journal Chemistry – A European Journal
Print ISSN 0947-6539
Electronic ISSN 1521-3765
Publisher Wiley
Peer Reviewed Peer Reviewed
Volume 25
Issue 27
Pages 6840-6846
APA6 Citation Ried, A., Taylor, L., Geer, A., Williams, H., Lewis, W., Blake, A., & Kays, D. L. (2019). A Highly Active Bidentate Magnesium Catalyst for Amine‐Borane Dehydrocoupling: Kinetic and Mechanistic Studies. Chemistry - A European Journal, 25(27), 6840-6846. https://doi.org/10.1002/chem.201901197
DOI https://doi.org/10.1002/chem.201901197
Keywords dehydrocoupling; magnesium; hydrogen storage; amido ligands; homogeneous catalysis
Publisher URL https://onlinelibrary.wiley.com/doi/abs/10.1002/chem.201901197

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