Templating Photodimerization of
trans-Cinnamic Acids with
Cucurbit[8]uril and γ-Cyclodextrin
Mahesh Pattabiraman, Arunkumar Natarajan, Lakshmi S. Kaanumalle, and
V. Ramamurthy*
Department of Chemistry, Tulane UniVersity, New Orleans, Louisiana 70118
murthy@tulane.edu
Received October 15, 2004 (Revised Manuscript Received December 29, 2004)
ABSTRACT
Cucurbit[8]uril and γ-cyclodextrin are able to align two olefin molecules in a head-head fashion within their large cavities. Excitation of such
templated olefins results in syn head-head cyclobutanes in nearly quantitative yields. The methodology revealed here works with trans-
cinnamic acids that do not dimerize either in solution or in the solid state and with the ones that yield only anti head-tail dimer in the solid
state.
The reactions of trans-cinnamic acids are examples of [2 +
2] photodimerization that have been investigated extensively
since 1889.
1
Some of these acids exhibit a dual behavior on
photolysis dependent on the reaction medium. While in
solution trans-cis isomerization occurs exclusively, on
photolysis of the crystal these acids react to give dimeric
products under conditions where the two reactive CdC bonds
are within the topochemically stipulated distance (<4.2 Å)
and parallel (Scheme 1).
2,3
Most of the current efforts in
solid-state photochemistry are devoted to establishing reliable
strategies that would steer molecules so as to obtain a crystal
structure that would favor photodimerization.
4
In this paper,
we establish the utility of cucurbit[8]uril (CB[8])
5
and
γ-cyclodextrin (γ-CD) in templating photodimerization of a
variety of trans-cinnamic acids to a single isomer (syn head-
head dimer) both in solution and the solid state. Remarkably,
the methodology reported here with CB[8] and γ-CD is
general and works with a number of cinnamic acids that do
not dimerize (γ-packing) and also with the ones that give
anti head-tail dimers (R-packing) in solid state. Since
CB[8] is known to include mostly cationic guest molecules,
until now its scope as a reaction medium has been limited.
Photodimerization of C
2
-symmetric trans-diaminostilbene
hydrochloride within CB[8] has recently been reported.
6
As
far as we are aware, neither neutral olefins nor olefins with
different substituents have been included and aligned within
CB[8]. We show in this report that CB[8] can include neutral
(1) (a) Liebermann, C. Chem. Ber. 1989, 122, 124. (b) Liebermann, C.
Chem. Ber. 1989, 122, 782.
(2) (a) Cohen, M. D.; Schmidt, G. M. J. J. Chem. Soc. 1964, 1996. (b)
Cohen, M. D.; Schmidt, G. M. J. J. Chem. Soc. 1964, 2000. (c) Schmidt,
G. M. J. J. Chem. Soc. 1964, 2014.
(3) Ramamurthy, V.; Venkatesan, K. Chem. ReV. 1987, 87, 433.
(4) (a) Toda, F. Acc. Chem. Res. 1995, 28, 480. (b) Ito, Y.; Kitada, T.;
Horiguchi, M. Tetrahedron 2003, 59, 7323. (c) Ito, Y.; Borecka, B.; Totter,
J.; Scheffer, J. R. Tetrahedron Lett. 1995, 36, 6083. (d) MacGillivray, L.
R.; Reid, J. L.; Ripmeester, J. A. J. Am. Chem. Soc. 2000, 122, 7817. (e)
Gao, X.; Friscic, T.; MacGillivray, L. R. Angew. Chem., Int. Ed. 2003, 43,
232. (f) Papaefstahiou, G. S.; Zhong, Z.; Geng, L.; MacGillivray, L. R. J.
Am. Chem. Soc. 2004, 126, 9158. (g) Caronna, T.; Liantonio, R.; Logothetis,
T. A.; Metrangolo, P.; Pilati, T.; Resnati, G. J. Am. Chem. Soc. 2004, 126,
4500. (h) Shan, N.; Jones, W. Tetrahedron Lett. 2003, 44, 3687.
(5) (a) Mock, W. L. Top. Curr. Chem. 1995, 175, 1. (b) Day, A.; Arnold,
A. P.; Blanch, R. J.; Sunshall, B. J. Org. Chem. 2001, 66, 8094. (c) Kim,
J.; Jung, I.-S.; Kim, S.-Y.; Lee, E.; Kang, J.-K.; Sakamoto, S.; Yamaguchi,
K.; Kim, K. J. Am. Chem. Soc. 2000, 122, 540.
ORGANIC
LETTERS
2005
Vol. 7, No. 4
529-532
10.1021/ol047866k CCC: $30.25 © 2005 American Chemical Society
Published on Web 01/21/2005