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Composites: Part A 34 (2003) 695708

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Inverse algorithm for optimal processing of composite materials


J.-L. Bailleul*, V. Sobotka, D. Delaunay, Y. Jarny
UMR CNRS 6607, Laboratoire de Thermocinetique, La Chantrerie-Rue Christian Pauc, 44306 Nantes Cedex 03, France
Received 3 July 2002; revised 23 January 2003; accepted 2 April 2003

Abstract
During thermoset composite materials processing, the chemical reaction is highly exothermic and because of the low thermal conductivity
of the material, significant temperature and state of cure gradients can be generated in thick parts. This creates non-uniform stresses that
provoke defects. We propose to control the transformation by monitoring the temperature of the mold walls. A general inverse analysis based
on the conjugate gradient method of minimization associated to the adjoint equations is used. After having detailed the method, we propose
two examples. The first one presents an optimal cycle to obtain uniform conversion at the end of the curing of an epoxy/glass-fiber composite.
The second example is concerned with the control of the temperature variations during the curing of a polyester/glass-fiber composite. The
method is experimentally validated and proves to be very powerful and flexible.
q 2003 Elsevier Ltd. All rights reserved.
Keywords: A. Thermosetting resin; E. Cure; E. Heat treatment

1. Introduction
Composites are more and more used in structural
applications and often reach thickness of the order of one
centimeter and this even for large series applications where
for productivity reasons the duration of the cycles becomes
relatively short. The composite materials are insulating,
and since the heat released during the chemical reaction of
curing is in the heart of the piece, the evacuation of the
heat generated is difficult. This provokes large temperature
and degree of conversion gradients. The quality of the part
is altered by the internal stresses that can provoke warpage
and in some cases cracks. The shrinkage of organic resins
reaches 7% during curing, even if thermoplastic additives
compensate partially at the end of curing [1,2]. If the
surfaces of the piece come unstuck from the mold wall
during gelation, the aspect of the surface is damaged. If
one has imperatives of surface aspect, it is therefore
necessary to control the development of shrinkage during
curing. In any case, one may try to master either the space
and time distribution of the temperature, either of the
conversion distribution, or the distribution of the shrinkage
* Corresponding author. Tel.: 33-2-4068-3137; fax: 33-2-4068-3141.
E-mail address: jean-luc.bailleul@polytech.univ-nantes.fr (J.-L.
Bailleul).
1359-835X/03/$ - see front matter q 2003 Elsevier Ltd. All rights reserved.
doi:10.1016/S1359-835X(03)00141-6

or the stresses, or even several of these parameters at a


time. These distributions are not independent, they are
coupled, and the control of one can prove to be sufficient or
on the contrary it is impossible to control them simultaneously. The parameters on which one can act are the
cycles of pressure or the applied temperature profiles on
the walls of the mold.
In a recent article, Antonucci et al. [3] proposed a
methodology to act on the temperature profile of the mold
walls, in order to reduce the temperature gradients
connected with the exothermal reaction. The authors
show that the cycle limits also the gradients of conversion. Ruiz and Trochu [4] established a cycle of curing
permitting to reduce the residual stresses in the piece. In
these two examples, the authors follow an empirical
approach, based on intuitive physical considerations.
Although this approach gave excellent results, it cannot
take into account multiple constraints and couplings, for
example the impossibility to get very fast time variations
of the mold wall temperature or the complexity of the
thermo-mechanical coupling. An alternative consists then
of using a method of optimization in which one is
searching for an optimal cycle allowing to minimize a
criterion chosen according to a specific objective. It is
what we chose to illustrate in this article. The choice of
the criterion is delicate, but in this exploratory study, we

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J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

Nomenclature

a
ad
b
dH
DH
f
g
l
m
r
Cp
d
F
G
J
K
L

state of cure
desired state of cure
conjugate factor
residual energy
total enthalpy of the transformation (J/g)
value of the criterion
penalization factor
thermal conductivity (W/(m2 K))
distance of descent
density (kg/m3)
specific heat (J/(g K))
descent direction
function product of KG
kinetic function of a
deviation criterion
kinetic function of T
thickness of the piece (m)

chose to determine a curing cycle so that the degree of


conversion remains uniform in all points of the part
during a time between a time t1 and the time final tf : Two
examples will be presented to test the capability of the
algorithm. The first one consists of obtaining a uniform
partial conversion at the end of cure. This choice is linked
to a strategy of determining the thermal conductivity
according to the degree of conversion, that requires
obtaining a uniformly transformed sample. The second
consists of taking one of the cases treated in Ref. [3] and
applying the optimization method. We will search therefore a cycle that allows a conversion distribution in which
the state of cure gradients are limited during part of the
curing cycle. We will consequently limit the temperature
gradients and then the stresses.

2. Cure modeling
We consider a mold filled of raw composite, after the
filling phase. The piece is of uniform thickness and its size is
such that it can be considered as a plate. The walls of the
mold are heated and cooled, but the performance of the
temperature control system is such that the heating and
cooling rates are lower than a given limit. This will be
integrated like a constraint in the optimization process. The
temperature of the mold walls will be supposed uniform on
all their surface. We will consider that the variations of
temperature along the length and the width are negligible in
comparison to the thickness. As a consequence, the problem
will be considered as unidirectional across the thickness x:
The temperature and conversion field obey the energy and
kinetic equations coupled through the heat source due to the
curing reaction, and the thermal properties that depend on
the temperature and the state of cure.

L
Q
R
t
T
U
U
x
X

Lagrangian of the direct system


Lagrange multiplier
contact resistance (m2 K/W)
time (s)
mold temperature (8C or K)
mold process control temperature (K)
mean initial control (K)
space coordinate
mass ratio of resin in the composite

Subscript

normal
0
space coordinate equal to zero
f
fiber or final state
i
lower
n
iteration index
r
resin
s
upper

Considering the configuration of the system represented


in Fig. 1, the conversion and temperature fields verify the
system of Eq.(1):


8
T
T
a
>
>
rCp a;T
l a;T
rXr DH
>
>

t
x

x
t
>
>
>
>
>
a
>
>
FT;a
>
>
t
>
>
<
initialcondition:
>
>
>
Tx;0T0 tandax;0a0 t
>
>
>
>
>
boundaryconditions:
>
>
>


>
>
T  T0;t2Ut
T  TL;t2Ut
>
>
x02
xL2
l
:

Rs t
Ri t
x  0
x L
1
The signification of the parameters is given in the
nomenclature. On the boundaries x0 and xL; we
suppose the existence of thermal contact resistances Rs t
and Ri t: The boundary conditions at x0 and xL are
completed by the mold temperature Ut which is imposed
in time. The goal of our optimization method is the
determination of the mold wall temperature during the
whole process.

Fig. 1. Configuration of the system.

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

The thermal properties are calculated according to the


degree of conversion by the rule of mixture, the validity
being demonstrated in Ref. [5]. The FT; a function
appearing in the kinetic equation describes the chemical
reaction with a phenomenological relation of Kamal and
Sourour [6] or a Bailleul type [7], for example. The
generality of the algorithm allows the integration of all these
types of expressions.
The control algorithm of such a strongly coupled nonlinear system of equations, under the constraint of
maximum rate of evolution for the boundaries requires
relatively complex methods of optimization. The objective
of this article is to test the feasibility of their usage on real
cases, in order to solve practical problems of composite
processing: with a press of a given performance, how can
we achieve a thick piece with a uniform conversion degree?
How can we minimize the temperature gradients
during curing? Two examples are proposed to reach this
objective.

3. Optimization method
The inverse Lagrangian method [8] is based on the
elaboration of a criterion. We try to determine a state of cure
as uniform as possible at the end of the cycle for which the
temperature does not exceed the boundary limit beyond
which degradation starts. We use an optimization method
which is detailed in Appendixes A and B. We thus define the
following criterion to be minimized:
 22
JU kaU 2 ad k21 gkU 2 Uk

with
tf L
kf k21
f 2 dxdt

kf k22

tf

f dt

where tf is the final processing time.


In the above expression, aU verifies the set of Eq.
(1) where U is imposed, ad is the required state of
cure and U is a curing cycle introduced a priori to
avoid unrealistic controls. In actual practice, the value
of U is selected in the practical range of curing
temperatures.
The optimum solution Up(t), which minimizes JU; is
determined by a conjugate gradient iterative method. The
principles of this method may be found in Ref. [8]. The
iterated values U n are determined by the following
algorithm (Eq. (4)):
Repeat:
U n1 U n mdn
with :

dn t 27J n t bn dn21 t

697

and:
8
tf L
>
>
7J n 7J n dxdt
>
>
>
0
0
n
< b t L
f
7J n21 7J n21 dxdt
>
>
0
0
>
>
>
: 1
b 0

Until JU n , 1In algorithm (4), d n t is the direction of


descent, m is the length of descent and bn designates the
conjugate state (See Appendix A for more details. Eq. (4) is
identical to Eq. (A37) in this appendix).
Both the descent direction d n and the descent depth m are
determined by introducing the Lagrangian of the problem as:
La; T; Q1 ; Q2 JU:

L tf  a
2 KTGa Q2 dtdx

t
0 0


L tf 
T
a

T
2 rXm DH
2

rC p
l
Q1 dtdx
x
t
t
x
0 0
5
where Q1 and Q2 are Lagrange multipliers associated to T
and a; respectively. The increment of the Lagrangian is
defined by:
dLa; T; U; Q1 ; Q2

L
L
L
dT
dU
da
a
T
U

The Lagrange multipliers Q1 and Q2 are chosen such as


(see Appendix A):
8
L
>
>
< T dT 0 ;dT
7
>
>
: L da 0 ;da
a
We then obtain two equations defining the adjoint system
(Eq. (8)). The details on how to derive these equations and
how to compute Q1 and Q2 may be found in Appendix A.
8


C p Q 1

Q 1
F
>
>

Q
r
l
W
>

>

t
x

x
T 2
>
>
>
>
>
>
>
Cp T
l T
>
>
Q1
8
r
>
<
T t
T x
>
>
Cp T
>
Q 1 Q 2
F
Q
>
>
W
Q1 rXDH 1
Q2 r
>
>

t
t
>
>
>
>
>
>
l T Q 1
>
:
2a 2 ad

a x x
with the boundaries conditions:



Q 
Q 0; t
Q 
Q L; t
2 l 1 xL 1
2l : 1 x0 1
Rs t
Ri t
x
x
Moreover, when T and a satisfy the direct system, i.e. the
integral terms equal to zero in the Lagrangian expression

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J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

(5), we have:
dLa; T; U; Q1 ; Q2

L
dU 7JUdU
U

so

L
7JU
U
The derivative of the Lagrangian versus U provides the
gradient of the criterion, which is used to calculate dn t
from Eq. (4).
We are now concerned with the determination of the
descent depth m (Appendix B). For U and d fixed, the
scalar m is determined by the solution of the optimization
problem:
minimize JU mdn fm

with m . 0

10

We have:
 22
fm kax; t; U m dn 2 ad k21 gkU m dn 2 Uk

11

Having established both the descent direction d n t and


depth m; we can now modified the boundary conditions and
reiterate the process according to Eq. (4).
The calculation of the mold wall temperature U p t
should be achieved by making sure that the value found is
not physically impossible to obtain. Rates of heating and
cooling depend on the equipment available. They must be
attainable with the device used to produce the composite
piece. A set of constraints on the mold wall temperature
values is then defined as:
8
>
< Umin # Ut # Umax
dUt
>
: Vmin #
# Vmax
dt

15

For practical consideration, the mold wall temperature


U p t on the interval 0; tf  has been calculated on a limited
number of points. The algorithm computes U p tj with j
1; ; n; n being defined by the user (of the order of 10 in
the realistic examples presented here).

Then we obtain, after linearization of Eq. (11):


 22 m2 :kdak21 kdnk22
fm ka 2 ad k21 gkU 2 Uk

tf L

tf
 dndt
2m
a 2 ad da dxdt g U 2 U
0

12
which can be written as:

fm A 2Bm Cm2

13

This equation is quadratic with respect to m: The


minimum of fm is defined as: m 2B=C: The increment
da is determined by the resolution of the sensitivity
equations which are obtained by writing first the direct
system (1) with T m dT and a m da: Then the same
equations for T and a are subtracted from the preceding
ones to yield the following system



Cp
Cp
dT
T
r
dT
rCp
da
t
a
T
t




dT

l
l
T
l
da dT

x
x
x
a
T
x

da
rDHX
14
t

da
F
F

dT
da
t
a
T
with the boundary conditions:
8


dT 2dn
dT
l
l
T
>
>
>
< Rs l x a da T dT x ;t;x 0


> dT 2dn
dT
l
l
T
>
>

;t;x L
l
da dT
:2
Ri
x
a
T
x

4. Demonstration examples
In order to check more surely the validity of the
calculations we have used an experimental method.
4.1. Example 1. Partial uniform curing at the end
of the processing cycle
The objective is to obtain a uniform predefined
distribution of curing at the end of the process. This is
necessary to measure the thermal conductivity la; T of a
sample as a function of the state of cure a: In order to use
classical methods to measure thermal conductivity such as a
guarded heat plate or a function estimation it is easier with a
uniform cure. For the guarded heat plate method, if a is not
uniform we can not know for what value of a the results
correspond. For function estimation, it is very difficult to
identify simultaneously the temperature and state of cure
dependence of the thermal conductivity. It would be an
estimation method for two functions what is very difficult.
The progression of the reaction must reach the required
value at the end of the partial curing process with a curing
rate equal to zero to prevent the continuation of the reaction
after the end of the cycles as illustrated by Fig. 2. The
measure of the thermal conductivity will correspond to a
fixed and not time dependant state of cure. The evolution
curves 1 and 2 illustrating the state of cure evolution at are
considered correct because they provide a degree of curing
with a plateau between t1 and tf ; unlike evolution curve 3
which keeps on rising beyond tf :
To reach a curing rate equal to zero at the end of the
cycle, the ultimate progression stage must remain constant
at the ad value on the interval t1 ; tf : In this example, we use

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

699

Table 1
Parameters of the kinetic function K for the epoxy resin

a composite made of an epoxy resin associated with a U.D.


fiber glass reinforcement (Brochier M10).
As presented in Eq. (1), the thermal parameters depend
on temperature T and the state of cure a: So we have to
measure these parameters as a function of T and a: The
methods are described in Ref. [7] for the specific heat and
in Ref. [5] for the thermal conductivity. For the specific
heat we consider a simple model based on the rule of
mixtures:
16

where Cp0 is the specific heat of the raw resin and Cp1 is
the specific heat of the cured resin. By measurement, we
obtain the specific heat in J/g K, with T in Celsius:
Cp0 T 1:584 3:259 1023 T

^0:06 J=g K

17

before Tg 135 8C :
Cp1 T 1:213 4:338 1023 T

^0:1 J=g K

after Tg :
Cp1 T 1:944 1:378 1023 T

^0:05 J=g K

For the through-thickness thermal conductivity, we use a


model for transverse conductivity found in Refs. [10,11] in
which the following equation was established:

l lr a; T

1 vf lf T 1 2 vf lr a; T
1 2 vf lf T 1 vf lr a; T

Value

Tref (K)
kref (s-1)
A

423
6.988 1023
17.631

Eq. (20)) by a polynomial function (function Ga), Eq.


(21)). The parameter values are shown in Tables 1 and 2.



T
20
KT kref exp 2A ref 2 1
T

Fig. 2. Examples of possible cure evolution.

Cp a; T Cp0 Ta Cp1 T1 2 a

Parameter

18

where lf is the conductivity of the fibers (0.9 W/(m2 K)),


and lr is the resin conductivity. By measurement, we obtain
the orthogonal composite thermal conductivity in W/(m2 K)
with T in (8C):

G n a

kp
X

a k ak

21

k0

For our resin, the exothermal reaction enthalpy is equal


to 412.3 J/g.
The validation of the inverse algorithm was carried out as
follows: for a given thickness L 10 mm; a curing cycle
giving a spatially uniform ad 0:5 has been determined.
We started from an homogeneous temperature (40 8C)
and a state of cure equal to zero ax; 0 0: We will only
discuss the case with ad 0:5; but other cases can be found
in Ref. [12]. The results obtained with ad 0:5 are shown
in Figs. 3 5.
Fig. 3 shows the optimum mold wall temperature U p t
computed for 12 points. The cycle has been applied on a
press since it satisfies the constraints of Eq. (15). Fig. 4
shows the evolution of the deviation criterion JU to tend
towards a minimum.
We can note that 15 iterations are required to reach the
minimum value of JU: The convergence, here, was
achieved in two stages: a first stage up to iteration 7 and a
second stage between iterations 11 and 15. Fig. 5 shows the
evolution of the temperature and the state of cure in
the> heart of the sample versus time. We show also the
temperature evolution at the boundary x 0: The temperature gradient in the sample remains small.
The exothermic process in the heart of the sample is well
controlled. The cycle obtained U p t allows the reaction to
start doing a first heating plateau. It anticipates the start of
Table 2
Parameters of the kinetic function G of the epoxy resin
Parameter

Value

a0
a1
a2
a3
a4
a5
a6
a7

0.042
5.078
28.502
2265.238
727.932
2961.274
627.499
2162.547

raw composite :

l T 0:1 1:756 1023 T

19

cured composite :

l T 0:554 3:1 1024 T


For the kinetic reaction, we use a model which gives
a=t as the product of an Arrhenius law (function KT;

700

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

Fig. 3. Curing cycle to reach 50% curing for a 10 mm part.

the reaction in the center of the piece, which is controlled by


a first cooling stage.
A low temperature post-cure plateau allows to keep the
reaction velocity steady before stopping it definitively with
the final cooling stage. Fig. 6 shows the evolution of the
state of cure through the thickness of the part for several
times.
Two heating Plate (diameter 162 mm) placed inside a
press apply pressure on the sample ensuring 1D heat
transfer. Details on the press may be found in Ref. [9].
We checked the spatial distribution of residual heat in the
piece and compared it with the desired spatial distribution of
state of cure at the end of the curing ad 0:5:
The validation consists of measuring the spatial distribution of residual heat dH 1 2 aDHX: We cut out a
piece of material in the axial area of the partly cross-linked
sample (Fig. 7). We successively removed some thin layers
at position xi to prepare the samples on which the residual
energy measurement dHi will be carried out.
The measurement of the residual energy is carried out
with a DSC. Given that we are performing this analysis on
very small composite material samples, the resin Xi mass
ratio is unknown and must be determined by thermal
gravimetric analysis by decomposing the sample and
keeping the fibers only. We can then deduce the state of
cure at position xi by:

Fig. 4. Evolution of the deviation criterion.

Fig. 5. Evolution of temperature in the heart of the sample at 50% curing for
a 10 mm part.

axi ; tf 1 2

dHi
Xi DH

22

The curing profile in the part can be obtained by


repeating this procedure at several locations across the
thickness of the part. The experimental results shown in
Fig. 8 are very satisfying.
4.2. Example 2. Optimal curing of a polyester-glass fiber
composite
The second test is related to the curing of a highly
reactive polyester resin and random glass mat (fiber volume
fraction: 0.32) of 10 mm thickness treated in [3]. The
objective is to minimize temperature gradients in the
thickness of the part during curing.
The physical properties of the materials used are listed in
Table 3. The kinetic model of the resin given in Ref. [3]
verifies Eqs. (23) (27).

a_ Kp 1 2 aR
dR
2fKd I
dt
dI
2Kd I
dt
where,

Fig. 6. Evolution of state of cure at 50% curing (10 mm part).

23
24
25

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

701

Table 3
Physical properties of polyester-glass fiber composite
Properties

Resin

Fiber

Composite

Density (kg/m3)
Specific heat (J/kg K)
Thermal conductivity (W/m K)

1100
1680
0.168

2560
670
1

1567
1152
0.13

Table 4
Kinetic parameters of the polyester resin
Fig. 7. Descriptive diagram of the operating mode.



E
Kd Ad exp 2 d
RT

26




Ep
a m
Kp Ap0 exp 2 0 1 2
af
RT

27

Table 4 reports the values of the kinetic parameters


of Eqs. (23) (27). Fig. 9 represents the reaction
velocity calculated with Eqs. (23) (27) for various
curing cycles.
The formulation of our optimization method uses a
specific description of the kinetics based on an assumption
of separation of variables, so that the thermal release rate
can be written as:
da
KTGa
dt

28

In this formula, da=dt is the product of a function of


temperature in Arrhenius form by a function of the
conversion degree.
We are then obliged to adopt a strategy consisting of
rebuilding the resin kinetics in the form of Eq. (28) starting
from the mechanistic model (Eqs. ((23) (27))). Optimization is then performed from the phenomenological model
(Eq. (28)) and its validity will be checked for the
mechanistic model.
Function K is determined by simulating constant heating
rates from 15 to 40 K/min. For each heating rate the cycle is

Fig. 8. Comparison between calculated, desired and measured states of


cure.

Parameter

Value

f
af
Ad
Ap0
Ed J=mol
Ep0 J=mol
It0
Rt0
Hr J=g
m

0.1
1.0
5.55 1016
0.38 1010
1.41 105
4.27 104
5.208 1023
0
244
4

composed of a first isotherm at 25 8C/min, then a


temperature ramp between 25 and 220 8C and it is
completed by a last isotherm at 220 8C for 3 min. Then
for each scanning run, at a given time t; the temperature, the
conversion degree of the reaction, a; as well as the reaction
velocity da=dt are known. Fig. 10 represents the evolution of
the reaction rate, da=dt; according to the state of cure, a; for
several temperatures.
For each temperature, the curves pass by an extreme
which is approximately located at the same value a ap :
A reduced value of G is considered so that Gap 1: For
each level of temperature, one can determine the value of
the reaction velocity for a ap :

da 
KT
29
dt aap

Fig. 9. Curing rate for various cycles of cure.

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J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708


Table 5
Parameters of the kinetic function K for the polyester resin
Parameter

Value

Tref (K)
kref (s21)
A

361.5
6.192 1023
29.887

Fig. 10. Curing rate in function of conversion degree, for various


temperatures.

Each extreme then gives a point for the determination of


the function KT: This function is in the form of Eq. (20),
where Tref is a temperature chosen arbitrarily in the domain
of work at which a parameter Kref is associated. Thus, if we
draw the logarithm of KT for a ap as a function of
Tref =T 2 1 we obtain a straight line (Fig. 11). The slope is
2A and the line crosses the Y-axis at lnkref : This is
applied by taking a reference temperature of 361.5 K. The
parameters of function KT are given in Table 5.
The relationship between the reaction velocity and the
value of the function KT gives the value of function Ga
for a given conversion degree a: All the values obtained for
function G at several temperatures are presented in Fig. 12.
One thus can, with a good approximation, represent the
function Ga by a single curve, interpolated by
polynomials.
The interval [0,1] is divided into n subintervals
ai ; ai1 0#i,n in which
G is interpolated by a
P the function
k
polynomial Gn a kp
a
a
:
Table
6 gives the park
k0
ameter values of function G:
Fig. 13 shows that the phenomenological model is very
close to the mechanistic model for isotherms from 85 to
125 8C. We will thus use this model for optimization.
In order to approach realistic range of experimental
conditions, the maximum rate of the mold wall temperature
Ut is limited to 10 8C/min. It is a plausible maximum
heating rate for the Plate of a press.

Fig. 11. Straight vertical line allowing to determine function KT:

Fig. 12. Determination of the function G:

The initial conditions are as follow: uniform temperature


equal to 20 8C and state of cure equal to zero ax; 0 0:
The initial cycle is a temperature ramp from 20 to 70 8C at
10 8C/min, then an isotherm at 70 8C for 30 min. Fig. 14 also
shows the cycle resulting from optimization, where four
points were examined in the cycle. One is composed of a
ramp from 20 to 68.5 8C, then a cooling to 24 8C and finally
of a second ramp to 75 8C. The rates of heating and cooling
Table 6
Parameters of the kinetic function G for polyester resin
State of cure interval

Parameter

Value

0 # a&lt; 0:1

a0
a1
a2
a3
a4
a5
a6

0.0546
31.627
2431.148
3015.48
211,399.6
21,690.4
216,248.8

0:1 # a&lt; 0:6

a0
a1
a2
a3
a4
a5

0.646
6.862
243.252
96.90
2104.198
45.373

0:6 # a&lt; 0:8

a0
a1
a2
a3

2.116
26.107
5.777
21.782

0:8 # a

a0
a1
a2
a3

4.632
214.787
15.729
25.575

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

703

Fig. 13. Comparison of the curing rate given by the mechanistic model
(Eqs. (23)(27)) and by the phenomenological model (Eq. (28)) for a series
of constant temperatures presented in Ref. [3].

are identical and close to 4 8C/min, which is perfectly


realistic in experiments.
We use the cycle of Fig. 14, determined by the inverse
algorithm and we add to this cycle a post-curing to 160 8C
for 30 min. The plateau at 160 8C is reached by a ramp at
10 8C/min. Then, one again calculates the changes of
temperature and conversion degree through the thickness of
the part (Fig. 15a and b). This direct calculation was carried
out by using the mechanistic formulation of the resin
kinetics.
We observe in Fig. 15a the very good homogeneity of
temperature during all the cycles. The most significant
variation, about 20 K, is for t 930 s at the beginning of the
cooling, the material not yet solid a , 0:6: The cooling
phase makes it possible to limit the heat released and as a
consequence, the temperature gradients.
Fig. 15b represents the state of cure in the part. The
reaction begins after 500 s. Then the conversion degree
increases quickly between 500 and 1000 s which corresponds to the heating ramp. During cooling, polymerization
is more rapid in the heart of the part, but the difference
decreases to lead to a quasi-uniform conversion degree a
0:64 at the end of the optimization, which was taken to
initiate the post-curing analysis.
If we focus more precisely on the beginning of the
reaction 500 s , t , 1000 s; we can see that it begins

Fig. 15. Evolutions of temperature (15a) and conversion degree (15b)


through the thickness of the part.

from the edges of the part and that for a conversion


degree equal to 0.24 an inversion occurs. The reaction
becomes faster in the middle of the piece. The cycle is
well optimized because it anticipates this inversion and
begins cooling before a 0:24: The edges being colder,
the heat released in the center of the piece can thus be
evacuated. This protocol prevents the trapping of residual
stresses in the part.
During the phase of post-curing t . 2300 s the edges
polymerize again more quickly than the heart. However, the
variations in the thickness are negligible because the largest
part of the heat released by the resin polymerization has
already been dissipated.
Optimization made it possible to obtain a realistic cycle.
It must be noted that this cycle would be very difficult to find
by an intuitive method and that it limits the temperature and
state of cure gradients in a part, avoiding the trapping of
residual stresses.

5. Conclusion

Fig. 14. Initial and optimized representation of the mold wall temperature.

We have presented a methodology to control the curing


of composite material based on an inverse method. It
consists of minimizing a criterion under constraints. In this
paper, this criterion is based on the state of cure, but the
generalization of the method allows to define any specific
criterion depending on the desired objective. The minimization method based on the adjoint state method is described.

704

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

Two examples demonstrate the feasibility of the inverse


method to handle realistic situations. The first case
corresponds to a partial uniform state of cure through the
thickness of the part. It was experimentally validated. The
second example is concerned with the control of curing for a
highly reactive polyester resin. A cycle achieving a quasiuniform temperature through the thickness of the part during
curing was found. This cycle is realistic because it is
possible to apply it on an industrial press for which heating
and cooling rates are limited.
Future perspectives of this work concern the use of such
an algorithm with a criterion based on the pressure evolution
in the mold cavity and secondly on the stress distribution
through the thickness of the part. This supposes complicating the model and as a consequence the adjoint equations,
but it seems accessible.

Appendix A. Determination of the descent direction dn


We detail in this appendix the method used to resolve the
inverse problem based on the 1D direct problem described
by the set of Eq. (A1):


T

T
a

A1
rCp a; T
la; T
rDH r
x
t
x
t
a
WhTFa; T
t
with
hT

tind
0

 

T
exp 2B ref 2 1 dt 2 tref
Tt

Wx 0

if x , 0

Wx 1

if x # 0

T0; x T0 x

dUt
# Vmax
dt

A3

Tx; t # Tmax

ax; tf ad
The Lagrangian L associated to the minimization
problem is introduced by:
La;T;U;Q1 ;Q2

L tf  a
2WhTFa;T Q2 dtdx
JU
0 0 t



L t f 
T
T
a

2 rDH r
Q1 dtdx
rCp a;T 2
la;T
t x
x
t
0 0
A4

Q1 and Q2 are the adjoint variables respectively


associated to T and a: This Lagrangian may be expressed
by a sum of five integrals: L J A B C D E: In
this expression the function Ut; that we want to determine,
does not appear explicitly because it is a boundary
condition. It appears implicitly in the integral D :

L tf 
T
la; T
Q1 dtdx
x
0 x
0

A5

By space integration by parts, D may be written as:

D2

0 , t , tf
0 , t , tf

f 2 x; tdtdx

where aU is the solution of the system of Eq. (A1).

T
Q
la; T
x 1

dt

L tf

la; T

T Q 1
dtdx
x x
A6

And, with the specified boundary conditions, we obtain:

with

tf

 2
JU kaU 2 ad k2 gkU 2 Uk

Vmin #

D2


ad x; t and Ut
are given on the intervals 0; tf  and
0; L; and g . 0: ad x; t is the state of cure that we want to
reach. We are searching a curing cycle Ut which
minimizes the criterion:

kf k2

Umin # Ut # Umax

0,x,L

a0; x a0 x 0 , x , L

T 
Tt; 0 2 Ut
la; T

Rs
x x0

T 
Tt; L 2 Ut
la; T


Ri
x xL

L tf

To find a realistic Ut; that is to say a realistic mold wall


temperature, we impose the constraints given by Eq. (A3).
These constraints are due to the press capacities.

L tf

T Q1
dtdx
la; T
x x
tf  T0; t 2 Ut
Q1 0; t

Rs
0

TL; t 2 Ut

Q1 L; t dt
Ri
0

A7

A2
Then, the Lagrangian expression in which Ut appears
explicitly becomes:

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

La; T; U; Q1 ; Q2
JU

L tf  a
0

I1
da
a


2 WhTFa; T Q2 dtdx

L tf
0

la; T

T Q1
dtdx
x x

tf  T0; t 2 Ut
Rs

Q1 0; t


TL; t 2 Ut
Q1 L; t dt
Ri
A8

In first order, we can write:


Fa 1 da; T Fa; T 1

which can be written in a condensed way by:


La; T; U; Q1 ; Q2 J I1 I2 I3 I4


1 L tf a 1 da
a
2
2 WFa 1 da; T
1!0 1 0
t
t
0

L tf  da
WFa; T Q2 dtdx lim1!0
t
0
0

Fa 1 da; T 2 Fa; T
2W
Q2 dtdx
1
A15

lim


L tf 
T
r a
2 rDH

rCp a; T
Q1 dtdx
t
t
0 0

A9

which is the detailed expression of Eq. (5). From Eq. (6), we


see that we have to calculate: L=ada; L=TdT and
L=UdU:
For the determination of the above terms, we have to
derive the Lagrangian (Eq. (A4)) versus a; T and U:

L
L
L
dT
dU
da
a
T
U

A10

Let us consider first the lagrangian derivation versus a :

L
da
a

J
I
I
I
I
1 2 3 4 da
a
a
a
a
a

By time integration by parts, we obtain:


I

daQ2 t0f dx 2

L t f Q
2
da dtdx
0
0 t

Q2 x; tf 0

; [ 0; L;

J
1
 2
da lim ka 1da 2 ad k2 gkUa 2 Uk
1!0 1
a


L tf  Q
I 1
F
da
2 2 2W
Q2 da dtdx
a
t
a
0
0

By developing this expression, we obtain:

A13

2rCp


T
a
rDH r X
Q1 dtdx:
t
t


L tf  C 2C T
pa
p
r da
lim
2 rDH X
r
Q1 dtdx
1!0 0 0
1
t
t
A20

Introducing (A13) in (A12) gives:


L tf
J
da 2
a 2 ad da dtdx
a
td
0

A19

The third term of Eq. (A11) is the derivative of I2 versus


a: By definition:

I 2
1 L tf
T
a 1 da
da lim
rCpa 2 rDH r X
1!0 1 0 0
a
t
t

ka 1da 2 ad k2
ka 2 ad k2 21a 2 ad da 12 :kdak2

A18

Considering that for t 0; we have da 0 and that Q2 is


chosen so that

it comes finally:

A12

A17

L t f da
Q2 dtdx:
0
0 t

The first term is the derivation of J versus a: It is defined


by:

 2
2 ka 2 ad k2 2 gkU 2 Uk

A16

Considering the first part of the integral in Eq. (A17) we


pose:

A11

F
da Qda2
a

By introducing (A15) it comes:



L tf  da
I 1
F
2W
da
da Q2 dtdx
a
t
a
0
0

I
dL

705

A14

The second term of (A11) is the derivative of I1 versus a:


By definition:

By writing:
Cpa Cp 1

Cp
da Qda2
a

A21

706

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

We choose Q1 so that
Q1 x; tf 0

; [ 0; L

and we use a procedure similar to the one used for the case
of I1 :

L tf  C T
I 2
Q
p
Q1 rDH r X 1 da dtdx
da
r
a
a t
t
0
0
A22
The fourth term of (A11) is the derivative of I3 versus a:
It is obtained by a procedure analogous to the one used for J:
We obtain:
L tf l T Q
I 3
1
da dtdx
da
A23
a
0 a x x
0

L tf 
C p T
L
F
dT
Q2 r
Q
2W
T
T
T t 1
0
0
C p Q 1
l T Q 1

2r
t
T x x



Q1
l
2
dT dtdx
x
x

A28

The derivation of I4 versus T puts into evidence the


boundary conditions on Q1 :
8

Q1 
Q1
>
>
:
;t [ 0; tf 
l
>
x0

<
x
Rs
A29

>
Q1 
Q1
>
>
:
l

2
;t
[
0;
t

:
f
x xL
Ri

The last term of Eq. (A11) is the derivative of I4 versus a:


It is not a function of a; so:

But, due to the definition of the adjoint variables, we


have:

I 4
da 0
a

L
dT 0
T

A24

Finally the Lagrangian derivative expression versus a is


obtained by summing the terms of Eq. (A11):
tf
IL
da 2
a 2 ad dadt
a
td
L tf  Q
C p T
F

Q
2 2 2W
Q r
t
a 2
a t 1
0
0
rDH r X

Q 1
l T Q 1

da dtdx
t
a x x

L
da 0
a

;da

A26

And we can deduce the first adjoint equation:

C p T
Q 2
F
Q
W
Q1 rDH r X 1
Q2 r
t
a
a t
t
l T Q 1
2a 2 ad

a x x
on td ; tf 

Cp T
l T Q1
Q
T t 1 T x x

A31

with

2:l



Q1 
Q1 0;t
Q1 
Q1 L;t

;t[0;t

l
;t[0;tf 
x0
f
xL


x
x
Rs
Ri

Let us consider finally the Lagrangian derivative versus


U appearing in Eq. (A10). Only two integrals J and I4
depend of U: By a procedure identical with the one used for
a; we obtain:
tf
J

dU 2g U 2 UdUdt
A32
U
0
and:

A27

tf
I4
dU 2
U
0


Q1 0; t
Q L; t
1
dUdt
Rs
Ri

A33

So, we deduce the Lagrangian derivative versus U :

with
(

So, the adjoint equation relative to the temperature is:




Cp Q1
F

Q
W
Q2
r
l 1
x
t
T
x

A25

By definition of the adjoint variables, we have:

A30

;dT

Q1 x; tf 0

;x [ 0; L

Q2 x; tf 0

;x [ 0; L

Let us consider now the lagrangian derivative versus T


appearing in Eq. (A10). By a procedure identical to the one
used for a; we derive all the terms which constitute
the Lagrangian. We obtain the Lagrangian expression
versus T :



tf 
L
Q1 0; t
Q1 L; t

dU
2gU 2 U 2

dUdt
Rs
Ri
U
0
A34
We can now express dL from Eq. (A10). Due to the
choice of the adjoint variables Q1 and Q2 which verify Eq.
(7), we have:

L
da 0
a

;da and

L
dT 0
T

;dT;

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

so:
dL



L
 2 Q1 0; t Q1 L; t
dU 2gU 2 U
Rs
Ri
U
A35

Since temperature and cure degree are solutions of the


direct problem, Eq. (9) gives:


 2 Q1 0; t Q1 L; t
7JU 2gU 2 U
A36
Rs
Ri

707

a
WFa; T
t
By substituting Eq. (A41) into (A40), we obtain:

Tm
T
2 Cp
r Cpm
t
t





Tm

T
lm
l

2
x
x
x
x


a m
a
2
rDH r
A42
t
t

We see from the above equation that by solving the


adjoint system, we can compute the gradient of the criterion.
By using the conjugate gradient method, we have the
descent direction [8].

a m
a
2
Wm Fm 2 WF
t
t

dn t 27J n t bn d n21 t

da lim

A37

By considering that m ! 0; we define da and dT as:


m!0

and
8 1
>
b 0
>
>
>
>
L tf
<

7J n 7J n dtdx
0
0
n
>
>
b L tf
>
>
>
:
7J n21 7J n21 dtdx
0

a 2 am
lim dam
m!0
m
A43

dT lim

m!0

T 2 Tm
lim dTm
m!0
m

In first order we have:

;n . 1

Cpm Cp

For the calculation of the new value of Ut; we have to


determine the descent depth. The method is presented in
Appendix B.

lm l

Cp
Cp
dTm Q2 da2m ; dTm2
dam
a
T

A44

l
l
dT Q2 da2m ; dTm2
da
a m T m

Let us write:
Appendix B. Determination of the descent depth m

From Eq. (4) we have:


U n1 t U n t mn dn t

A40

a m
a
2
t
t

am
a
2
t
t

E Wm Fm 2 WF

And, T and a are solutions of:




T

T
a

l
rDH r
x
t
x
t

C rDH r

am
Wm Fm
t

rCp





Tm

T
lm
l
B
2
x
x
x
x

A39

To U correspond the solutions T and a of the direct


problem, and to U m dU correspond the solutions Tm and
am So, Tm and am are solutions of:


Tm
Tm
am

rCpm
lm
rDH r
x
t
x
t

A45

A38

where mn is the depth descent for the iteration number n: It is


defined such as J is a minimum at the iteration n 1: For a
given iteration, J is a function of m :
 2
Jm kaU m dU 2 ad k2 gkU m dU 2 Uk


Tm
T
2 Cp
A r Cpm
t
t

A41

We have:


Cp
Cp
A
dT
T
r
dT
lim
rCp
da
m!0 m
t
a
T
t

A46






dT

l
l
T
:
l
da dT

m!0 m
x
x a
x
T
x

A47

lim

708

J.-L. Bailleul et al. / Composites: Part A 34 (2003) 695708

lim

m!0 m

rDH r

da
t

A48

D da

m!0 m
t

A49

lim

E WF
WF
lim
dT
da
A50
m!0 m
T
a
To completely determine the sensitivity of the system,
we consider the initial and boundaries conditions.
for t 0 we have:
dax; 0 dTx; 0 0

;x [ 0; L

at x 0 we have:


dT
l
l
T
dT 2 dU

dT

l
da
Rs
x
a
T
x
at x L we have:


dT
l
l
T
dT 2 dU

dT
2
l
da
Ri
x
a
T
x

da
t

tf


U 2 Uddt

tf
0

dddt

tf L
td
tf

0
L

td

a 2 ad dam dxdt
A61
da da dxdt

References
A53

A54

A55

A56

From Eqs. (A55) and (A56) it comes:


 2
JU md ka m da 2 ad k2 gkU md 2 Uk
 2ma 2 ad da
ka 2 ad k2 gkU 2 Uk
A57

or, in another form:


JU md f m a 2b:m c:m2

A60

But, J is a minimum only if c . 0: da2 ; d2 and g are


positive, so c is also positive. Finally, the depth of descent is
given by:

m2

and:

 md m2 kdak2 gm2 :kdk2


2gmU 2 U:

b
c

A52

By taking dU d n ; we obtain dT and da by resolution of


the system (A54). We have then:

am ax; t; U md ax; t; U m da

m2

da
WF
WF

dT
da
t
a
T

 2
JU md kam 2 am k2 gkU md 2 Uk

A59

Then we have:

A51

Finally, we can sum up the sensitivity system:




C p
Cp
dT
T
r
dT
rC p
da
t
a
T
t





dT

l
l
T
dT

l
da

x
x a
x
T
x
rDH r X

df m
2b 2cm 0
dm

A58

The minimization of J is equivalent to the minimization


of f(m) versus m:

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