Influence of Temperature on the Ultrasonic Degradation of
Poly(vinyl acetate) and Poly(vinyl chloride)
Sujay Chattopadhyay, Giridhar Madras
Department of Chemical Engineering, Indian Institute of Science, Bangalore— 560012, India
Received 7 February 2002; accepted 1 October 2002
ABSTRACT: This study investigates the effect of temper-
ature on the ultrasonic degradation of polyvinyl acetate and
polyvinyl chloride in chlorobenzene. The time evolution of
molecular weight distribution was determined using gel
permeation chromatography. Continuous distribution kinet-
ics was used to obtain the degradation rate coefficients. The
rate coefficients decrease with increasing temperature, and
this is attributed to the increase of vapor pressure and the
decrease of kinematic viscosity. The degradation rate coef-
ficient also changes sharply near the glass transition temper-
ature, indicating that this factor may play a role in the
degradation process. © 2003 Wiley Periodicals, Inc. J Appl Polym
Sci 88: 2818 –2822, 2003
Key words: degradation; gel permeation chromatography;
glass transition; viscosity; effect of temperature
INTRODUCTION
Ultrasound has been used in a variety of applications
like homo- and copolymerization,
1
emulsification,
2
and organic reactions.
3
One of the main applications
of ultrasound has been in the area of polymer degra-
dation. The literature has been summarized in the
review articles by Basedow
4
and Price.
5
The study of
ultrasound initiated degradation is interesting from
both practical and academic viewpoints.
6
Ultrasonic depolymerization is mainly caused by the
mechanical forces that arise due to the propagation of
ultrasonic waves. These forces are directly associated
with cavitation, which is the nucleation, growth, and
collapse of vapor-filled bubbles in the liquid.
7
Microjets,
formed during the collapse of a bubble, transmits the
shear force on to the polymer chain.
8
Unlike photo or
thermal, the process of chain breakage is nonrandom
and happens specifically at nearly the mid point of the
chain. An explanation put forth by Thomas
8
is that the
polymer molecule gradually changes its shape (in a
shear field) from that of a sphere to a cylinder and then
this breaks at the midpoint.
Several investigations
9,10
have focused on the physics
of shear breakage and the factors that influence the cav-
itation. Other than the solvent polymer parameters like
the Flory–Huggins and the Huggins constant that play a
minor role, the main parameters are the vapor pressure
and kinematic viscosity of the solution.
11
Unlike thermal
degradation, an increase of temperature leads to reduced
rate coefficients. Price
5
cites the work of Schmid and
Beuttenmuller, who investigated the degradation of ni-
trocellulose dissolved in n-butyl acetate and of polysty-
rene in toluene at 40 –120°C. The results indicated that
the degradation proceeded more slowly and yielded
higher limiting molecular weights at higher tempera-
tures. Thomas and Alexander
12
investigated ultrasonic
degradation of cellulose nitrate in a series of alkyl ace-
tates from 0 to 85°C and observed an optimum temper-
ature. The reduced degradation observed at both higher
and lower temperatures was explained by ineffective
cavitation. Malhotra
13
investigated ultrasonic degrada-
tion of hydroxypropyl cellulose in water, ethanol, and
tetrahydrofuran at various temperatures. It was con-
cluded that for cavitation to occur there must be a critical
radius that is dependent on the wavelength and inten-
sity of sound, density, viscosity, and surface tension of
the solvent. Recently, Price
14
investigated the degrada-
tion of polystyrene in toluene also reported decreasing
rate coefficients with increasing temperature.
To our knowledge, we are unaware of any study on
the ultrasonic degradation of polyvinyl acetate (PVAc)
and polyvinyl chloride (PVC) over an extensive tem-
perature range. The objective of this study is to inves-
tigate the degradation of these polymers in chloroben-
zene. The variation of the rate coefficients with tem-
perature is attributed to the change in the kinematic
viscosity and vapor pressure.
EXPERIMENTAL
Ultrasound degradation experiments
PVAc (prepared by bulk polymerization) and PVC
(Aldrich Chemicals) were used for the experiments.
The solvent chlorobenzene (S. D. Fine Chemicals) was
Correspondence to: G. Madras (giridhar@chemeng.iisc.
ernet.in).
Journal of Applied Polymer Science, Vol. 88, 2818 –2822 (2003)
© 2003 Wiley Periodicals, Inc.