Pergamon
Tetrahedron 54 (1998) 10449-10456
TETRAHEDRON
First Enantioselective Synthesis of
(+)-(3R,3aS,6aS)-3-Hydroxy-3,3a,4,6a-tetrahydrocyclopenta[blfuran-2-one
- a Versatile Chiral Heterocyclic Building Block
Steffen Kudis and Giinter Heimchen*
Organisch-Chemisches Institut der Umversit~t Heidelberg,Im Neuenheirner Feld 270, D-69120Heidelberg,Germany
Received 2 February 1998; accepted 11 February 1998
Abstract: Asymmetric Pd-catalyzed allylic alkylations of 2-acetoxymalonates with 2-cyclopentenyl
chloride are described. With the cymantrene based phosphinooxazoline 2 as chiral ligand enantio-
meric excess of> 99 % and > 90 % yield were obtained. Alkylation products were transformed in
three steps to ( + )-(3 R,3aS, 6aS)- 3-hydroxy- 3,3a, 4, 6a-tetrahydrocyclopenta [b]furan- 2-one (l a) in up
to 52 % yield. © 1998ElsevierScienceLtd. All rights reserved.
The bicyclic lactone I a (Scheme 1) is a versatile building block for syntheses of a variety of important
natural products, e.g. brefeldin A, 'a mevinolin) aristeromycin and carbodine, 4 5'-homo-carbocyclic nucleo-
sides, 5 carbocyclic analogs of polyoxins and nikkomycins, 6 the anti-HIV agent carbovir7 and the antitumor
agents sesbanimide A and B. s The key building block la has so far been prepared by enzyme catalyzed
kinetic resolution of the racemic compound which was obtained via Diels-Alder reaction of cyclopentadiene
and glyoxylic acid. 9 In view of the importance of the lactone la a catalytic asymmetric synthesis appears
highly desirable.
OH H OH
U ~ 4 " 3
HO .... ) s 0
6 - v 1
H H
Brefeldin A
Scheme 1
(+ )-(3R,3aS,6aS)-la
* Corresponding author. Email: en4@ix.urz.uni-heidelberg.de. Fax: 0049 6221 544205.
0040-4020/98l$ - see front matter © 1998 Elsevier Science Ltd. All rights reserved.
Plh S0040-4020(98)00497-9