ArticleNature chemistry2022
Structure, reactivity and catalytic properties of manganese-hydride amidate complexes.
Article in Nature chemistry, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 15 papers.
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15 citing papers in PubMed.
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- Low-Valent Transition Metalate Anions in Synthesis, Small Molecule Activation, and Catalysis.Chemical reviews · 2024Review
- A 13-million turnover-number anionic Ir-catalyst for a selective industrial route to chiral nicotine.Nature communications · 2023Article
- Designing New Magnesium Pincer Complexes for Catalytic Hydrogenation of Imines andJournal of the American Chemical Society · 2023Article
- Efficient Hydrogenation of N-Heterocycles Catalyzed by NNP-Manganese(I) Pincer Complexes at Ambient Temperature.Chemistry (Weinheim an der Bergstrasse, Germany) · 2023Article
- ReNeGate: A Reaction Network Graph-Theoretical Tool for Automated Mechanistic Studies in Computational Homogeneous Catalysis.Journal of chemical theory and computation · 2022Article
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6 authors.
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Abstract
The high efficiency of widely applied Noyori-type hydrogenation catalysts arises from the N-H moiety coordinated to a metal centre, which stabilizes rate-determining transition states through hydrogen-bonding interactions. It was proposed that a higher efficiency could be achieved by substituting an N-M' group (M' = alkali metals) for the N-H moiety using a large excess of metal alkoxides (M'OR); however, such a metal-hydride amidate intermediate has not yet been isolated. Here we present the synthesis, isolation and reactivity of a metal-hydride amidate complex (HMn-NLi). Kinetic studies show that the rate of hydride transfer from HMn-NLi to a ketone is 24-fold higher than that of the corresponding amino metal-hydride complex (HMn-NH). Moreover, the hydrogenation of N-alkyl-substituted aldimines was realized using HMn-NLi as the active catalyst, whereas HMn-NH is much less effective. These results highlight the superiority of M/NM' bifunctional catalysis over the classic M/NH bifunctional catalysis for hydrogenation reactions.
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