A general synthesis of unnatural α-amino acids by iron-catalysed olefin–olefin coupling via generated radicals (original) (raw)

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* Corresponding authors

a A. N. Nesmeyanov Institute of Organoelement Compounds of Russian Academy of Sciences, Vavilova Str. 28, 119991 Moscow, Russian Federation
E-mail: larionov@ineos.ac.ru

b Department of Inorganic Chemistry, Peoples’ Friendship University of Russia (RUDN University), Miklukho-Maklaya Str. 6, 117198 Moscow, Russian Federation

c Dmitry Mendeleev University of Chemical Technology of Russia, Miusskaya sq. 9, 125047 Moscow, Russian Federation

d Plekhanov Russian University of Economics, Stremyanny per. 36, 117997 Moscow, Russian Federation

Abstract

Herein, we report an efficient and practical protocol for the asymmetric synthesis of unnatural α-amino acids (AAs) with γ-tertiary and quaternary carbon centres via selective intermolecular iron-catalysed olefin–olefin coupling of a chiral Ni(II) complex of dehydroalanine Schiff base 2 ((S)-BPB-Ni-Δ-Ala) with different olefins. In all successful reactions, diastereomeric nickel complexes were typically obtained in a ratio of up to dr > 20 : 1. The desired products were isolated in 42–93% yields (18 examples). Exemplarily, the three Ni(II) complexes obtained were decomposed with aqueous HCl and the target unnatural α-amino acids were isolated with excellent enantioselectivities and yields of up to 83%. The chiral auxiliary (BPB = 2-(_N_-benzylprolyl)aminobenzophenone) was readily recycled and reused for the synthesis of the starting chiral Ni(II) complex 2. The developed protocol provided a facile access to the analogues of glutamic acid, leucine and phosphinothricin.

Graphical abstract: A general synthesis of unnatural α-amino acids by iron-catalysed olefin–olefin coupling via generated radicals

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Article information

DOI

https://doi.org/10.1039/C9QO00108E

Article type

Research Article

Submitted

23 Jan 2019

Accepted

15 Feb 2019

First published

18 Feb 2019

Download Citation

Org. Chem. Front., 2019,6, 1094-1099

Permissions

A general synthesis of unnatural α-amino acids by iron-catalysed olefin–olefin coupling via generated radicals

V. A. Larionov, N. V. Stoletova, V. I. Kovalev, A. F. Smol'yakov, T. F. Savel'yeva and V. I. Maleev,Org. Chem. Front., 2019, 6, 1094DOI: 10.1039/C9QO00108E

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