TETRAHEDRON:
ASYMMETRY
Tetrahedron: Asymmetry 13 (2002) 333–337 Pergamon
A soluble polymer-bound Evans’ chiral auxiliary: synthesis,
characterization and use in cycloaddition reactio
GiovanniDesimoni,
a
Giuseppe Faita,
a,
* Alessandro Galbiati,
b
Dario Pasini,
a,
* Paolo Quadrelli
a
and
Fabio Rancati
a
a
Department of Organic Chemistry, University of Pavia-Viale Taramelli, 10 -I -27100
Pavia,Italy
b
NPT s.r.l.-Viale Zanotti, 90 -I -27027
Gropello Cairoli (
PV ) , Italy
Received 13 February 2002; accepted 6 March 2002
Abstract—The synthesis of novel soluble polymer-supported optically-active oxazolidinone (Evans’ chiral auxiliary) with
chiral monomer/styrene ratios is described. The polymer was obtained in high yields and then functionalized with trans-
anhydrideto givea high loading polymer(2.42 mmol/g). The reactivity wastested in the1,3-dipolarcycloaddition with
diphenylnitrone under catalyzed and uncatalyzed conditions. The cycloadducts could be obtained in high purities and fair yields
after reductive cleavage. The stereoselectivity is parallelto that obtained with the model substrate under classicalsolution
conditions. © 2002 Elsevier Science Ltd. All rights reserved.
Crosslinked,insolublepolymersupportsfor organic
synthesis have recently witnessed a resurgence of inter-
est for applications in combinatorial chemistry.
1
Most
recently,a variety of catalystsfor enantioselective
organic synthesis on insoluble supports have appeared
in the literature.
2
Tuning of the reactivity of the sup-
ported organic compounds in the unavoidably hetero-
geneous-phase reactions, as well as the detection and
analysis of the functionalized, supported products can,
however,be extremelyproblematic.Severalgroups
have recently explored the use of soluble linear poly-
meric,
3
dendritic
4
and precipiton
5
supports. The advan-
tagesof solid-phase synthesis are retained,since the
macromolecular supportis easily removed from the
reaction mixture via precipitation from an appropriate
solvent,but the synthetic pathway can be carried out
undermore convenient homogeneous solution condi-
tions, with easiercharacterization ofthe covalently
bound substrates.
Chiral 3-substituted1,3-oxazolidin-2-ones, originally
introduced by Evans,
6a
act as chiralauxiliaries in sev-
eral CC bond forming reactions as well as in metal-
catalyzed cycloaddition reactions between a variety of
1,3-dipoles and dienes, with good control of diastereo-
and enantioselectivity.
6
Typically, the catalyticpro-
cesses involve the dissolution in organic solvents of the
metalsalts (added as a heterogeneous solid) as a result
of coordination ofthe metalcation to the 1,3-dicar-
bonylmoiety in the chiralauxiliary.Grafting of this
chiral auxiliary to Merrifield and Wang resins has
already been achieved by us
7
and other groups,
8
but the
metal-catalyzed reactions of these resin-supported aux-
iliaries have shown some differences in stereoselectivity
in comparison to the solution-phase reactions.
7a
A car-
rier for the cation was found to be necessary in solid-
phase chemistry to allow interaction of the Lewis acid
with the grafted coordinating substrate and to simulate
classical catalysis conditions in solution, with the Wang
supportshowing highersensitivity to saltconcentra-
tions than the Merrifield resin-supported auxiliary.
7b
Herein, we communicate the synthesis, characteriza-
tion, and functionalization of a novel, soluble polymer-
supported optically-active oxazolidinone. Since the two
most common support strategies developed for soluble
macromolecular supportsare polyethylene glycol and
polystyrene-based,
3c
we chosethe latter in order to
avoid competitiveinteractionsbetweenthe oxygen
atoms of the polymer chains and the Lewis acidic metal
cation. Furthermore, polystyrene supports are removed
by precipitation in polar organic solvents in which all
the excess reagents should remain soluble. Preliminary
investigations on the reactivity of the soluble polymer-
* Correspondingauthors. Tel.: +39-0382-507866; fax: +39-0382-
507323; (G.F.) tel.: +39-0382-507312; fax: 39-0382-507323 (D.P.);
e-mail: faita@chifis.unipv.it; pasini@chifis.unipv.it
0957-4166/02/$ - see front matter © 2002 Elsevier Science Ltd. All rights reserved.
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