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Enantioselective Synthesis of Pyroglutamic Acid Esters from Glycinate via Carbonyl Catalysis

Jiguo Ma, Qinghai Zhou, Guanshui Song, Yongchang Song, Guoqing Zhao, Kuiling Ding, Baoguo Zhao

2021Angewandte Chemie International Edition63 citationsDOI

Abstract

-free glycinates with relatively weak electrophiles such as α,β-unsaturated esters still remains a big challenge in organic synthesis. With chiral pyridoxal 5 d as a carbonyl catalyst, direct asymmetric conjugated addition at the α-C of glycinate 1 a with α,β-unsaturated esters 2 has been successfully realized, to produce various chiral pyroglutamic acid esters 4 in 14-96 % yields with 81-97 % ee's after in situ lactamization. The trans and cis diastereomers can be obtained at the same time by chromatography and both of them can be easily converted into chiral 4-substituted pyrrolidin-2-ones such as Alzheimer's drug Rolipram (11) with the same absolute configuration via tert-butyl group removal and subsequent Barton decarboxylation.

Topics & Concepts

Enantioselective synthesisPyroglutamic acidChemistryElectrophileDecarboxylationDiastereomerCatalysisOrganic chemistryAmino acidBiochemistryChemical Synthesis and AnalysisAsymmetric Synthesis and CatalysisFluorine in Organic Chemistry