Non-isothermal Modelling and Optimisation Methodology of the Injection Moulding of Rubber Products

Non-isothermal Modelling and Optimisation Methodology of the

Injection Moulding of Rubber Products
A.V. Baranov
Gubkin State Oil and Gas University, Moscow, Russia
Received: 23 November 2015, Accepted: 6 January 2016

Summary
The process of injection moulding is regarded as a combination of separate operations linked by certain process
parameters. The first part of this study presents a mathematical model of the non-isothermal flow of rubber mixes
along mould sprue channels, taking into account all the main features of the injection moulding process. On the
basis of this model, an attempt is made to develop a methodology for optimising the injection stage. Diagrams
linking the main process parameters are plotted. The second part of the study is devoted to the final stage of
this cycle – the vulcanisation stage. The presented mathematical model of non-stationary heat conduction takes
into account the heat evolution from the chemical reaction of vulcanisation and the temperature dependence
of all thermophysical properties. On this basis, an attempt to develop optimisation methodology for this stage
is presented. Diagrams are plotted that link the main process parameters of the vulcanisation stage with the
previous stages of plasticisation and injection.

Keywords: Rubber mixes; Mathematical modelling; Non-Newtonian fluids; Injection moulding;

Vulcanisation

1. INTRODUCTION
The process of injection moulding
is one of the principal and most
progressive methods for moulding
of rubber products. However, the
advantages of injection moulding can
only be exploited fully if the process
has been fully optimised. The large
number of variable parameters results
in process control flexibility but creates
difficulties in process optimisation.
Experience now gained over many
years indicates that the actual efficiency
of the process and exploitation of its
advantages are ensured by optimising
the entire process and through correct
selection of the equipment and
mould construction. Therefore, in the
literature a great deal of attention has
been paid to this process of rubber mix
processing.
At present there are a fair number
of studies devoted to developing
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Smithers Information Ltd., 2017
mathematical models of the non-
isothermal flow of non-Newtonian
fluids in the sprue channels and mould
cavities during injection moulding1–9.
Different thermoplastics, rubber mixes,
highly filled thermosetting plastics,
and thermosetting plastics modified
with low-molecular-weight liquid
elastomers have been examined. In
many studies, the dependence of
viscosity on temperature, pressure, and
degree of transformation has been taken
into account. The presence of a moving
free surface (flow front) with so-called
‘fountain’ flow has been considered.
Both two-dimensional and three-
dimensional models have been used.
In solving such complex mathematical
models, use has been made of the
extremely costly finite difference/
element/volume methods. However,
most of these publications contain
no methodology for engineering
calculation of the optimum parameters
covering the entire process of injection
moulding. At the same time, the
approach proposed here to optimising
the given process dispenses with the
need to use such complex, expensive
and time-consuming programs.
This paper presents an attempt to model
the entire injection moulding process as
a combination of different operations –
plasticisation, injection, holding under
pressure, vulcanisation – following one
after another. The individual operations
have been regarded as independent
steps where the output parameter of the
previous step is the input parameter of
the next step.
2. INJECTION STAGE
In the present work an examination is
made of the injection (mould filling)
stage, as it is at this stage that the
quality of the obtained article depends
simultaneously on the features of
the injection moulding machine, the
mould construction, and the rubber
mix formulation. Optimisation of this
stage will lead to maximum throughput

Polymers & Polymer Composites, Vol. 25, No. 2, 2017 153


of the equipment, reduced substandard
production, and a reduction in
production waste. Rubber mixes are
highly viscous, and their flow in the
sprue channels of the mould occurs
under conditions of high pressure
gradients and considerable non-
isothermality, and is accompanied
with the occurrence of the chemical
reaction of vulcanisation. Therefore,
in the modelling of processes of
injection moulding of rubber mixes,
it is necessary to take into account
simultaneously the dependence of
mix viscosity on shear velocity,
temperature, pressure, and the degree
to which the vulcanisation reaction
proceeds. Furthermore, heat effects
from compressibility and dissipation
must be taken into account, as well as
the wall slip velocity10–12. During the
injection moulding of rubber mixes,
the moulding pressure can reach
200–250 MPa nowadays, which must
be taken into account in such processes.
Thus, with an increase in pressure to
150 MPa, the viscosity of different
mixes can increase 2–3-fold13. Analysis
of a whole number of studies indicates
an exponential dependence of viscosity
on pressure. Here, the exponent is
not temperature-dependent 14. The
dependence of the thermophysical
properties on pressure is generally
described by a linear function15.
In most publications, modelling of
processes of polymer processing is
done on the assumption of the absence
of wall slip in the channels. However, in
a whole number of studies, the presence
of wall slip is shown both for rubbers
and for rubber mixes. In Malkin et al.11,
the exponential relationship between
wall slip velocity and wall tangential
stress was obtained experimentally,
and this was used subsequently
in mathematical modelling12. This
relationship is also used in the present
work in formulating the mathematical
model.
In formulating the problem, the
generally accepted assumptions are
made16. Most of these are based on
154
A.V. Baranov
the fact that rubber mixes have a high
viscosity and low thermal diffusivity.
The origin of the Cartesian system of
coordinates is positioned at the entry
section of the channel.
Thus, with account taken of the
above, the mathematical model of
non-isothermal flow of rubber mix in a
plane sprue channel of constant height
2h is presented by the following system
of equations:
Equation of motion:
(2.1)
Equation of energy:
(2.2)
Equation of discontinuity:
(2.3)
Dependence of viscosity and
thermophysical properties on
temperature and pressure:
(2.4)
In the equation of energy it is assumed
that:
System (2.1)–(2.4) must be
supplemented with the following
boundary conditions:
(2.5)
Polymers & Polymer Composites, Vol. 25, No. 2, 2017
(2.6)
(2.7)
Thus, as a result of the combined
solution of system (2.1)–(2.4) with
the prescribed boundary conditions
(2.5)–(2.7), it is possible to calculate
the temperature, pressure and velocity
fields and to find the complex non-
linear inverse relationship between
the thermal, rheological, and kinetic
factors.
The formulated problem was solved
by an iteration scheme, at each step
of which the Galerkin–Kantorovich
method was applied. According to
this method, the temperature profile
in dimensionless form for the half-
height of the channel h was set in the
following way:
(2.8)
where:
Fo is the Fourier number
The condition of symmetry of the
temperature profile (2.5) requires
fulfilment of the condition G0 = G1.
It must be noted that the sprue channel
and the moulding cavity are linked by
the feed gate, which is a convergent
channel. On passing through the feed
gate, additional pressure losses and
dissipative heating of the mix occur.
This gate may be a plane channel,
with one wall horizontal and the other
inclined at a certain angle. In this case,
to describe the flow through such a
channel, the model set out above can
be used, provided that the height of
the channel is a certain linear function
h(x). However, if the feed gate is a
convergent channel, with both walls
inclined, the problem is solved in a
cylindrical system of coordinates13.
 Non-isothermal Modelling and Optimisation Methodology of the Injection Moulding of Rubber Products
In practice, rubber mixes flow along
the sprue channels while being
heated from the mould walls, which,
combined with dissipative heating and
cooling on expansion, does not make
it possible to ensure temperature field
homogeneity. On account of this, the
chemical reaction of vulcanisation
will occur non-uniformly in the flow.
Furthermore, account must be taken
of the fact that particles with different
velocities in the flow have different
residence times in the channel. All this
affects the temperature and time regime
T(t) and the residence times of the
individual microvolumes of the medium
in the channel, and consequently their
possible scorching. It is assumed that
the kinetics of the chemical reaction of
vulcanisation can be described using
a single parameter – the degree of
transformation (vulcanisation). This
can be taken to mean, for example,
the relative concentration of binding
agent entering the reaction. It has
been established experimentally17 that
the reaction of vulcanisation can be
categorised as a reaction occurring in
one stage, the rate of which depends
only on the relative concentration of
binding agent and temperature:
(2.9)
It is known17, for example, that more
than 50% of rubber mixes have an
order r of 1.0 and 1.6. Integrating this
equation, it is possible to obtain the
following expression16,17, which can
serve as a criterion for assessing the
viscous flow state of the mix under the
given temperature and time regime:
(2.10)
Thus, Equation (2.10) can serve as a
criterion for assessing the boundaries of
the viscous flow state of any elementary
microvolume of the medium having
its own temperature and time regime
of residence in the channel. The
residence time in the sprue channel of
elementary volumes of the medium at
Polymers & Polymer Composites, Vol. 25, No. 2, 2017
different distances from the channel wall was determined numerically in the
following way:
where M is the number of sections of division of the sprue channel, within which
the temperature and velocity of an elementary microvolume of the medium
are considered to be constant and are calculated by means of the formulae:
By comparing the obtained value of criterion (2.10) with its maximum permissible
value J*, the possibility of a given microvolume of the medium being in the
viscous flow state is determined. In practice, however, it is sufficient to calculate
J for a particle whose residence time in the channel is equal to the injection time,
i.e. for a particle that is under the worst temperature and time conditions from
the viewpoint of scorching.
The choice of parameters when preparing the production of a new article begins
with determination of the rheological, thermophysical, and vulcanisation
characteristics of the rubber mix. The optimum values of the vulcanisation
temperature and time are then selected. It is assumed that the number of mould
cavities and the layout of the sprue system are in place by this time. Thus, during
modelling of the injection stage, the mould temperature and the channel length
are considered to be specified.
To determine the region of permissible values of the operating parameters of the
injection moulding machine, calculations were conducted for a rubber mix with
physical properties characteristic of moulding grades of rubber mixes:
With variation in the flow rate of rubber mix and its initial temperature at entry
into the channel (the mix temperature after plasticisation), it is possible to
assess the region of mix processability when the moulding process is completed
before the end of the induction period of the reaction in particles entering the
working cavity. As a result of a series of calculations, it is possible to find the
dependence of the minimum permissible injection velocity on the temperature
at entry into the sprue channel T0 (Figure 1). Injection velocity values below
Qmin cannot be realised on account of the risk of scorching. Here it was assumed
that injection occurred in a regime controlled by the moulding unit, i.e. with a
constant injection velocity.
The moulding pressure is generally limited at the top of its range to a certain
maximum value, determined either by the injection possibilities of the moulding
unit or by the condition of opening of the half-moulds and the formation of
flash. Therefore Figure 1 shows the dependence of the maximum permissible
(achievable) injection velocity on the initial temperature at entry into the sprue
155
 A.V. Baranov

Figure 1. The dependence of the minimum and maximum Figure 2. A diagram for determining the process
permissible injection velocity on the mix temperature after parameters of injection moulding. Counterpressure during
plasticisation: (a) l = 60 mm; (b) l = 80 mm plasticisation: 1 – 3.7 MPa; 2 – 18.5 MPa; 3 – 35 MPa

channel T0. Thus, to each temperature
T0 there corresponds a certain range
of possible shear velocities from Qmin
to Qmax, limited at the top of the range
by the injection possibilities of the
moulding unit (or the formation of
flash) and at the bottom of the range
by probable scorching. To each regime
of the injection stage there corresponds
a certain point on this diagram. Here,
from a comparison of Figures 1a
and b it can be seen that calculations
for different sprue channel lengths
reveal a considerable narrowing of
the working interval of the possible
injection velocities, which increases
the likelihood of the working point
falling outside the region of optimum
operating regimes of the unit.
In order to link the individual stages
of plasticisation, injection, and
vulcanisation, the diagram shown in
Figure 2 was plotted. The lower part
of this diagram corresponds to the
plasticisation process. In the present
work, no attempt was made to develop
a new mathematical model of the
plasticisation process. For this stage,
it is possible to use many models
now published in the literature. Here,
experimental data obtained for the
given rubber mix were also used. Thus,
the lower part of the diagram makes it
possible to find the mix temperature
after plasticisation as a function of
basic process parameters such as
counterpressure and screw speed. The
obtained mix temperature at the end
of the plasticisation stage is the initial
temperature at entry into the sprue
channel and makes it possible in the
middle part of the diagram to determine
the working range of feasible injection
velocities. Above this range, as noted,
flash may arise, and below this range,
scorching may occur. The upper part
of the diagram makes it possible to
assess the degree of heating-up of the
mix during injection, and to determine
the mass-average temperature at
entry into the moulding cavity Tm
as a function of the temperature at
entry into the sprue channel and the
injection velocity. It is important to
point out that the mass-average mix
temperature at exit from the sprue
channel (i.e., at entry into the moulding

156 Polymers & Polymer Composites, Vol. 25, No. 2, 2017

 Non-isothermal Modelling and Optimisation Methodology of the Injection Moulding of Rubber Products
cavity) is the output parameter of the
injection process and at the same time
the input parameter of the subsequent
stage of vulcanisation as the initial
mix temperature in the non-stationary
heat conduction problem. Therefore,
the temperature Tm will enable the
injection stage to be linked with the
following vulcanisation stage.
3. VULCANISATION STAGE
In this section, the final stage of
injection moulding – the vulcanisation
stage – is considered. We will
assume that injection into the mould
has proceeded with a combination
of parameters ensuring that the
mix enters the moulding cavity in
unscorched form. After plasticisation
and flow along the sprue channels,
the mix is heated up and enters the
cavity with a certain temperature Tm0
(it is assumed that filling of the cavity
occurs in a jet regime, which makes
it possible to average out the mix
temperature). The mould temperature
in this case is Tw.
In the present work, a mathematical
model is given, and a procedure is
developed for solving the problem of
non-stationary heat conduction during
the chemical reaction of vulcanisation,
making it possible to calculate the
temperature fields and the degrees of
vulcanisation in articles.
Owing to the low thermal conductivity
of the rubber mixes, the temperature
distribution and consequently the
degrees of vulcanisation of the material
have a pronounced inhomogeneity.
For example, the surface of the article
practically instantaneously acquires
the temperature of the mould Tw. The
centre of the article is heated through
most slowly, and vulcanisation is
delayed considerably in comparison
with the surface layers. This may
entail inhomogeneity of the degree of
vulcanisation through the mass of the
article and the consequent appearance
of a number of defects (residual
stresses, sinks, gate marks, etc.).
Polymers & Polymer Composites, Vol. 25, No. 2, 2017
The complexity of the problem
is that it is necessary to ensure
optimum vulcanisation at the centre
of the article but in so doing not
to allow overvulcanisation of its
surface. Determining the optimum
vulcanisation regime for solid moulded
articles is most complex. Here, it must
be borne in mind that there is no need
to bring the centre of the article to
optimum vulcanisation directly while
the article is in the mould. The low
thermal diffusivity, which led initially
to non-uniform heating of the article
in the mould, is then the cause of the
slowest drop in temperature at the
centre of the article after its removal
from the mould and its cooling in air.
Thus, the degree of vulcanisation is
evened out through the thickness of
the article.
After entering the cavity, the
temperature of the polymer can rise
by many tens of degrees. This can affect
the thermophysical properties of the
mix. Here, mix density, specific heat,
and thermal conductivity may either
increase or decrease with increase in
temperature. As a rule, the temperature
dependences of these parameters are
described well by linear functions. An
attempt to improve the accuracy of
the obtained solution by introducing
into the model only the temperature
dependence of one particular
thermophysical characteristic alone
may lead to the opposite result.
Therefore, it is only allowance for the
temperature dependences of all three
thermophysical constants that will lead
to correct results.
To d e s c r i b e t h e p r o g r e s s o f
vulcanisation, use is made of a
single-stage kinetic model of fractional
order17,18. An examination is made of the
injection moulding and vulcanisation
of bulky articles, the filling of the
cavities of which occurs in a jet regime.
In this case, the temperature of the mix
entering the moulding cavity is entirely
evened out. Therefore, under the initial
conditions of the heat conduction
problem, it is considered that the
mix temperature is homogeneous
throughout the article and equal to Tm0
(the mass-average mix temperature
at exit from the sprue channel). The
wall temperature T w (the mould
temperature) is assumed to be constant
in this case.
Thus, the mathematical model of the
process is presented by the following
system of differential equations:
(3.1)
(3.2)
(3.3)
(3.4)
(3.5)
The boundary and initial conditions
are as follows:
(3.6)
(3.7)
(3.8)
It must be pointed out that the heat
conduction equation (3.1) is written
simultaneously for a sheet (G = 0), a
cylinder (G = 1), and a sphere (G =
2). Here, R stands for either the half-
height of the sheet or the radius of the
cylinder or sphere.
The set problem is solved by an
iteration scheme, at each step of which
the Galerkin–Kantorovich method is
used. According to this method, the
temperature profile in dimensionless
form is given as follows:
(3.9)
where:
157

Fo is the Fourier number
The form of the set coordinate functions
yi(ξ) depends on the geometric shape
of the body and should satisfy the
boundary conditions. It is convenient
to select a system of orthogonal
coordinate functions obtained by
solving the corresponding problem with
constant thermophysical properties
(the known solution adopted as a first
approximation). We use, for example,
eigenfunctions of the problem for a
sheet. Then, Equation (3.9) can be
made more specific:
(3.10)
where:
Unknown functions Bn(Fo) are found
from the solution of a system of N
ordinary differential equations, which
is obtained after substituting Equation
(3.10) into the heat conduction Equation
(3.1) and compiling conditions of
orthogonality of misclosure to all
coordinate functions in the range 0 ≤ ξ ≤
1. The system obtained in this way was
solved by the combined application of
the Kutta–Merson and Gauss methods.
Low thermal diffusivity, which led
initially to non-uniform heating
through of the article in the mould, is
then the cause of the slowest drop in
temperature at the centre of the article
after its removal from the mould and
cooling in air. For theoretical calculation
of the temperature distribution and
degree of vulcanisation at the cooling
stage, the same model as during
heating is used, only thermal boundary
conditions of the first kind are replaced
with boundary conditions of the third
kind, i.e. instead of condition (3.7), the
following condition is used:
(3.11)
158
A.V. Baranov
The temperature profile at the cooling
stage is sought in the form:
(3.12)
The functions G n(Fo) are found
similarly to the algorithm set out above
when determining the functions Bn(Fo).
At this stage, the so-called scorch
criterion (2.10) is also used.
Figure 3 shows the time dependence
of the degree of vulcanisation of the
surface and centre of a cylinder at a
fixed mould temperature and different
initial temperatures Tm0. Here, the
relationship I(t) for the surface of the
article is linear in nature:
The point of intersection of this line
with the limiting line Imax determines
the permissible residence time tmax
Figure 3. The dependence of the degree of vulcanisation of the surface (1) and
centre (2, 3, 4) of a cylinder on the vulcanisation time: 1 – T0 = 180 °C; 2 – T0 =
100 °C; 3 – T0 = 85 °C; 4 – T0 = 70 °C
Polymers & Polymer Composites, Vol. 25, No. 2, 2017
of the article in the mould; I max
represents the maximum permissible
degree of vulcanisation, above which
overvulcanisation (degradation)
begins. From Figure 3 it can be seen
that, by the moment of removal of the
article from the mould, only curve 2
manages to reach the zone of optimum
vulcanisation. However, as already
pointed out, during cooling in air, the
vulcanisation process continues at the
centre of the article, while the degree
of vulcanisation of the surface no
longer changes. Thus, by the moment
of practically complete cooling
of the article, curves 3 and 4 also
manage to reach the zone of optimum
vulcanisation. The initial temperature
Tm0 = 70 °C under the given conditions
is the minimum permissible mix
temperature at which a high-quality
cylinder of 40 mm radius can still be
produced.
If we now plot similar graphs for
different values of the cylinder radius
and different mould temperatures,
and in each case select the minimum
permissible initial temperature of the
 Non-isothermal Modelling and Optimisation Methodology of the Injection Moulding of Rubber Products
mix , then it is possible to plot the
graphs shown in Figure 4. Using these,
we can, as a function of the article radius
and the mould temperature, immediately
determine the minimum permissible
temperature to which the rubber mix
must be heated at the previous stages
of injection moulding. In turn, the
combination of process parameters
ensuring the required temperature
can be determined from the diagram
presented in Figure 2. In this way, the
diagrams in Figures 2 and 4 link the
vulcanisation stage with the previous
stages of plasticisation in the injection
cylinder and injection into the mould.
4. CONCLUSIONS
In the present work, mathematical
models of non-isothermal processes
of rubber mix flow through the sprue
channels and vulcanisation during
injection moulding have been presented.
For the first time, the dependences of
all thermophysical properties and
viscosity, not only on temperature but
also on pressure, have been taken into
account simultaneously. It is important
to emphasise that the presented
mathematical model is not the end goal
of this work; at present there are a fair
Figure 4. The dependence of the minimum permissible initial mix temperature
on the radius of the article and the mould temperature: 1 – Tw = 200 °C; 2 – Tw =
180 °C; 3 – Tw = 160 °C; 4 – Tw = 140 °C
Polymers & Polymer Composites, Vol. 25, No. 2, 2017
number of very complex commercial
software packages describing the non-
isothermal flow of polymers in different
channels and moulds. However,
most of these publications contain
no methodology for engineering
calculation of the optimum process
parameters of the entire process,
from the very start to the end. At the
same time, the approach proposed
here dispenses with the need to use
such complex, expensive and time-
consuming programs. The presented
calculations form a basis for subsequent
use in engineering practice. On the
basis of the model presented here,
a new algorithm has been proposed
for optimising the parameters of the
entire process of injection moulding:
mould construction – plasticisation –
injection into the mould – vulcanisation
– cooling in air. All process variables
are included in the diagrams presented
in the work: screw speed, plasticisation
counterpressure, mix temperature
after plasticisation, sprue channel
length, mould temperature, injection
velocity and vulcanisation time. The
plotted diagrams illustrate the method
for finding the region of process
parameters, ensuring that the process
is conducted in the optimum regime.
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Polymers & Polymer Composites, Vol. 25, No. 2, 2017
Notation
a – thermal diffusivity;
x, y – longitudinal and transverse
coordinates respectively;
T – temperature;
p – pressure;
λ, ρ, c p – thermal conductivity,
density, and specific heat of the mix
respectively;
α – heat transfer coefficient in air;
Ta – air temperature;
vx, vy – longitudinal and transverse
velocity components respectively;
h – channel half-height;
K – consistency of the mix;
n – flow index;
U – activation energy;
R* – universal gas constant;
tw – channel wall stress;
ε – coefficient of volumetric expansion;
β – degree to which the chemical
reaction of vulcanisation proceeds;
b1, b2, A, g1, g2, g3, s, q – empirical
constants determined from experiments.