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The first catalytic inverse-electron demand hetero-Diels–Alder reaction of nitrosoalkenes using pyrrolidine as an organocatalyst
Tobias C. Wabnitz,Steen Saaby,Karl Anker Jørgensen
Organic & Biomolecular Chemistry Pub Date : 02/16/2004 00:00:00 , DOI:10.1039/B316518C
Abstract

The first catalytic inverse-electron demand hetero-Diels–Alder reaction of nitroso alkenes has been developed. Nitroso alkenes were generated in situ from α-halooximes and underwent [4 + 2]-cycloadditions with enamines as dienophiles formed from aldehydes and pyrrolidine (10 mol%) as an organocatalyst. The presence of a suitable heterogeneous buffer system was found to be essential and best results were obtained with sodium acetate trihydrate. The resulting 5,6-dihydro-4H-oxazines were obtained in moderate to good yields under mild reaction conditions. A catalytic cycle has been proposed and evidence for the cycloaddition mechanism has been obtained. Moderate asymmetric induction (42% ee) was observed when a chiral secondary amine was used.

Graphical abstract: The first catalytic inverse-electron demand hetero-Diels–Alder reaction of nitroso alkenes using pyrrolidine as an organocatalyst
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