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H NMR Study of the Kinetics of Substituted Aniline
Polymerization. I. Homopolymerization of
2-Methoxyaniline
IDA MAV, MAJDA Z
ˇ
IGON
National Institute of Chemistry, Laboratory for Polymer Chemistry and Technology, Hajdrihova 19, POB 3430,
1000 Ljubljana, Slovenia
Received 2 January 2001; accepted 30 April 2001
Published online 00 Month 2001
ABSTRACT: We studied the kinetics of the oxidative chemical homopolymerization of
2-methoxyaniline (OMA) in aqueous acid solutions by monitoring OMA depletion with
1
H NMR spectroscopy. We used the same semiempirical kinetic model used for aniline
(ANI) homopolymerization to evaluate the experimental data. The reaction kinetics of
OMA homopolymerization was similar to that of ANI, although we obtained longer
induction and propagation times for OMA. This was attributed to steric hindrance of
the bulky methoxy substituent during the coupling reaction. Furthermore, it was
suggested that a lower OMA polymerization rate could also be related to a lower
concentration of nonprotonated OMA molecules in the reaction solution due to a higher
pK
a
value for OMA than for ANI. This may also explain the lower OMA end conversion
(90%) compared with that of ANI (96%). The OMA end conversion was not influenced
substantially by reaction conditions; it was lower than 90% only when high acid or low
oxidant (oxidant-deficient oxidant/OMA ratio) concentrations were applied. Because
the oxidant took an active part in polymerization, it markedly influenced the polymer-
ization rate, especially the initiation rate. The OMA initiation and propagation rates
increased with increasing oxidant and initial monomer concentrations and with the
reaction temperature, but there was no uniform trend in the correlation between the
homopolymerization rate and acid concentration. The activation energies of the OMA
initiation and propagation were 57 and 10 kJ/mol, respectively. © 2001 John Wiley & Sons,
Inc. J Polym Sci Part A: Polym Chem 39: 2471–2481, 2001
Keywords: aniline derivative; 2-methoxyaniline; chemical polymerization; reaction
conditions; kinetics;
1
H NMR
INTRODUCTION
The polymerization mechanisms of aniline (ANI)
and its derivatives are very complex and have
been studied intensively by many groups. The
polymerization mechanisms and reaction kinetics
have been investigated mostly by electrochemical
polymerization, that is, by cyclic voltammetry in
aqueous solutions.
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It is generally agreed that
the initiation reaction (induction period) involves
the oxidation of neutral (nonprotonated) ANI
monomers to radical cations, whose radical cou-
pling leads to the formation of dimeric species:
p-aminodiphenylamine, N-phenyl-p-phenylenedi-
amine, or benzidine. The oxidation of dimeric spe-
cies, as well as subsequently formed oligomers
and polymers, all with lower oxidation potentials
than ANI, occurs immediately after their forma-
tion. An electrophilic attack on the ANI monomer
by oxidized species would accomplish a growth
Correspondence to: I. Mav (E-mail: ida.mav@ki.si)
Journal of Polymer Science: Part A: Polymer Chemistry, Vol. 39, 2471–2481 (2001)
© 2001 John Wiley & Sons, Inc.
2471