Repozytorium

Structures of highly twisted amides relevant to amide N—C cross-coupling: evidence for ground-state amide destabilization.

Autorzy

Vittorio Pace

Wolfgang Holzer

Guangrong Meng

Shicheng Shi

Roger Lalancette

Roman Szostak

Michal Szostak

Rok wydania

2016

Czasopismo

Chemistry-A European Journal

Numer woluminu

22

Strony

14494-14498

DOI

10.1002/chem.201603543

Kolekcja

Naukowa

Język

Angielski

Typ publikacji

Artykuł

Streszczenie

Herein, we show that acyclic amides that have recently enabled a series of elusive transition-metal-catalyzed N−C activation/cross-coupling reactions are highly twisted around the N−C(O) axis by a new destabilization mechanism of the amide bond. A unique effect of the N-glutarimide substituent, leading to uniformly high twist (ca. 90°) irrespective of the steric effect at the carbon side of the amide bond has been found. This represents the first example of a twisted amide that does not bear significant steric hindrance at the α-carbon atom. The 15N NMR data show linear correlations between electron density at nitrogen and amide bond twist. This study strongly supports the concept of amide bond ground-state twist as a blueprint for activation of amides toward N−C bond cleavage. The new mechanism offers considerable opp

Słowa kluczowe

amides, N−C activation, rotation, steric hindrance, twisted amides

Adres publiczny

http://dx.doi.org/10.1002/chem.201603543

Strona internetowa wydawcy

onlinelibrary.wiley.com

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