ELSEVIER Synthetic Metals 74 (1995) 99-102
SWTiiETII[
IMITIS
Poly(cyclopentadienylene vinylene)s: synthesis via ROMP, chemical and
physical properties
Michael Schimetta ", G(inther Leising b, Franz Stelzer a
a Christian Doppler Laboratoriumfiir Katalytische Polymerisation, Institutfiir Chemische Technologie Organischer Stoffe, Technische Universitdt Graz,
Stremayrgasse 16, A-8010 Graz, Austria
b lnstitutfiir FestkOrperphysik, Technische Universitiit Graz, Petersgasse 16/11, A-8010 Graz, Austria
Received 7 December 1994; revised 10 June 1995; accepted 12 June 1995
Abstract
Norbornene derivatives, bearing different substituents, were polymerized via ring-opening metathesis polymerization (ROMP). This paper
mainly reports on possibilities of controlling the stereochemistry of the polymerization reaction to give stereoregular precursors to conjugated
polymers. The precursor polymers were then converted to the corresponding conjugated polymers through thermal or base-induced elimination.
Monomers used for the polymerization were norbornenebis(methylcarbonate), norbomenebis(S-methyldithiocarbonate) and benzonorbor-
nadienes substituted with isopropylidene, methylbenzylidene, phenylbenzylidene andp-fluorophenyl-p-fluorobenzylidene groups at the bridge
carbon. Resulting polymers were then converted to poly(cyclopentadienylene vinylene) or more rigid highly substituted
poly(cyclopentadienylene vinylene)-bearing exocyclic double bonds. Characterization was carded out by spectroscopic methods on thin
films (photoluminescence, IR, UV-Vis-NIR, ~H and ~3CNMR spectroscopy).
Keywords: Poly (cyclopentadienylene vinylene)s; Synthesis; Metathesis polymerization
1. Introduction
Use of precursor polymers is one common way to conju-
gated polymers. Polyacetylene via a precursor polymer was
first achieved by an elegant route established by Feast and
co-workers [ 1-3] that showed some useful features [4]. A
way to poly(p-phenylene) (PPP) via thermal acid extrusion
of acetates was first shown by ICI workers [5,6]. The major
disadvantages of this route were the price and commercial
availability of the monomer and the limited control over ster-
eochemistry. Similar routes were applied for the synthesis of
poly(phenylene vinylene) [7] and poly(cyclopenta-
dienylene vinylene) [8,9].
Theoretical studies on conjugated polymers [ 10,11 ]
showed a dependence of the bandgap on the conformation of
the conjugated polymer. Therefore, it was interesting to syn-
thesize precursor polymers with high tacticity and well-
defined stereoregularity. Ring-opening metathesis
polymerization (ROMP) of norbornene derivatives bearing
sterically demanding substituents proved to be a way to these
well-defined precursor polymers. Variation of substituents
(as shown below) from acetate to dixanthate in positions 2
and 3 of norbornenediol or from methyl- to p-fluorophenyl
benzylidenebenzonorbornadienes allowed the control of the
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stereochemistry of the polymerization and the electrical and
optical properties of the conjugated polymer.
R2
la-d 2a-d
R1, P~ = a) methyl, methyl F~ = a) acetate, b) benzoate,
b) methyl, phenyl, e) carbonate, d) xanthate
e) phenyl, phenyl
d) pfluorophenyl,p-fluorophenyl
Thermal elimination of esters as a precursor route to con-
jugated polymers usually was applied to esters like acetates
or benzoates. Precursor polymers with these functional
groups [9] usually showed glass transitions between 50 and
100 °C and decomposed at temperatures above 300 °C. At
these temperatures, uncontrolled side reactions (crosslink-
ing, oxidation, degradation, etc.) occurred that did not allow
formation of high conjugation lengths. So it was attempted
to reduce the temperature of elimination into the region of
the glass transition by substitution with S-methyldithiocar-
bonate ( = dixanthate) groups. The literature indicated little