jourmlof

MEMBRANE
SCIENCE
ELSEVIER Journal of Membrane Science 98 (1995) 263-273

Dynamic modeling of crossflow microfiltration using neural

networks
M. Dornier a, M. Decloux a,*, G. Trystram a, A. Lebert b
a Ecole Nationale Sup~rieure des Industries Agricoles et Alimentaires, Food Engineering Department, 1, Av. des Olympiades,
91305 Massy, France
lnstitut National de Recherche Agronomique, S.R. V., St Genks Champanelle, 63122 Ceyrat, France
Received 27 May 1994; accepted in revised form 19 August 1994

Abstract

The neural network theory was used to dynamically model membrane fouling for a raw cane sugar syrup feed stream. The
use of neural networks enabled us to integrate the effects of hydrodynamic conditions on the time evolution of the total hydraulic
resistance of the membrane under constant temperature and feed stream concentration. The results obtained satisfactorily model
the effects of both constant and variable transmembrane pressure and crossflow velocity as the filtration was followed through
time. The effects of the hidden network structure as well as the scatter of data on the quality of modeling are discussed in this
paper.

Keywords: Crossflow microfiltration; Neural networks; Dynamic modeling; Membrane fouling; Raw cane sugar

1. Introduction tool. This model should particularly allow the best

Crossflow microfiltration can be the solution to many
problems in solid-liquid separation. However, the
development of this process in industry has been
delayed by the low permeation rates that reduce the
feasibility of the operation. Despite the tangential cir-
culation, membrane fouling slows the filtrate flux and
can be considerably important in many cases.
For a given product/membrane combination, it is
often difficult to predict the effects of operating con-
ditions and of the duration of filtration on the fouling
rate. A model that can predict the evolution of
membrane fouling during filtration as a function of the
operating conditions would therefore be a necessary
* Corresponding author.
optimization of the filtrate flux.
Membrane fouling is a consequence of a number of
dynamic and simultaneous phenomena: convective
mass transfer through the membrane, back-diffusion
caused by high local concentrations, shear-induced
hydrodynamic back-transport, electrochemical inter-
actions between the product and the membrane and
possible chemical or microbiological instabilities in the
feed stream. Considering the diversity of these phe-
nomena, the development of a dynamic model based
on the known principles of transfer, that globally rep-
resents fouling, is extremely difficult. Therefore, con-
trary to ultrafiltration, dynamic-knowledge-based
models specific to microfiltration are scarce in the lit-
erature. The few models proposed so far, only define
certain phenomena, do not take into account the effect
of operating conditions as a whole or make use of

0376-7388/95/$9.50 © 1995 Elsevier Science B.V. All rights reserved

SSD10376-7388(94)00195-2
264 M. Dornier et al. /Journal of Membrane Science 98 (1995) 263-273
parameters that are difficult to determine experimen-
tally [ 1-3].
Hence, modeling techniques based on the direct anal-
ysis of experimental data (descriptive models) appear
to be a good alternative to the models based on phe-
nomenological hypotheses (knowledge-based mod-
els). As a tool of dynamic simulation, these black box
models, although not explicative, can be used to rep-
resent the experimental results and are suitable to glob-
ally describe the considered phenomena.
The effects of operating conditions on fouling and
on its dynamic behavior are often not linear. Therefore,
the classical descriptive linear models cannot be used
in these cases [4]. Considering their features, connec-
tive models or neural networks should allow one to
account for the nonlinearity of many phenomena that
take place during membrane fouling.
This study aims to establish and validate the use of
neural networks for the dynamic modeling of
membrane fouling. The methodology of neural net-
works is applied to the particular case of raw cane sugar
syrup clarification by crossflow microfiltration, exper-
iments were conducted under different operating con-
ditions.
2. Neural networks
Following the first studies carried out in the forties
[5,6 ], neural networks cover a vast number of descrip-
tive models grouped under the name connective mod-
els. Among many types of neural networks developed
up to date [7-10], the multilayer perceptron was cho-
sen in this study. This type of network, originally devel-
oped by Rosenblatt [ 11 ], is actually used for a great
number of applications (approximation of function,
signal prediction, pattern recognition, classification,
data compression, etc.). In the case of process model-
ing, the multilayer perceptron has already been used
successfully for various applications such as fermen-
tation processes [12-14], drying [ 15,16] and other
chemical processes [ 17-19].
2.1. The neural cell and its organization in a network
The neural cell is a single calculation processor and
the neural network consists of an association of neural
cells. As schematically represented in Fig. 1, the prin-
ciple of calculation in a neural cell can be described in
two successive steps. The activations originating from
preceding cells (Aj) are individually multiplied by a
coefficient w 0. This coefficient is called the weight of
the connection; it determines the importance of the
connection between cell i and the preceding one,j. The
sum of all pondered activations is then calculated to
obtain the total stimulation of cell i, called S;. Following
the total stimulation of the neural cell i and with an
intermediate nonlinear activation function, f, the neural
cell then calculates its own activation Ai, such that
Ai = f(Si). In order for the network to represent phe-
nomena with thresholds, neural cells, whose activation
are constantly maintained maximum, are also defined.
These particular cells are called either neural cells of
polarization or bias.
Hence, the multilayer perceptron is a whole set of
neural cells organized in successive layers with non-
recurrent oriented connections among themselves.
Every neural cell of the same layer only receives acti-
vations from the cells of the immediate preceding layer
(Fig. 2). The first and the last layers are called the input
and output layer, respectively.
2.2. Principle of application
For a given network structure, it is necessary to deter-
mine the combination of coefficients w0, which will
best permit the model to represent the outputs versus
the inputs. The weights of all the connections of the
neural network are in fact the parameters of the model.
From randomized values, their identification is gener-
ally carried out using the back-propagation algorithm.
The principle of this algorithm is based on a classical
technique of gradient descent with a fixed step [ 20,21 ].
This stage is realized with a first series of data called
the learning base. Following this, a second series of
data constituting the so-called test base is treated, as
suggested by Bochereau [22], in order to verify
whether the model can be generalized for other cases.
Before using this type of model, it is necessary to make
a certain number of choices, particularly:
- Choice of the network structure: the output layer
contains the predicted responses and the input layer
contains the parameters that are likely to influence these
responses. A priori, there are no set rules for the choice
of the hidden structure. It is determined empirically:
the structure that gives the best results is chosen. How-
 M. Dornieret al. / Journal of Membrane Science 98 (1995) 263-273 265

which permits a real time fine regulation of operating

conditions and fast data acquisition. Details of this are
given by Punidadas et al. [ 23 ]. The filtration unit oper-
From .w i W
i~ t~ h~ i _ . . ' To ates with a partial recycling of the retentate. Different
neuralcellj A J ~ i j . A.I=~I,)-~ ttaO= ~ neuralcellh
membrane types of a surface area of ~ 0.2 m 2 can be
adapted in this pilot plant. The membrane used in this
study was a ceramic one with a multichanel profile,
Neuralcelli Membralox IP19-40 (Soci6t6 des C6ramiques Tech-
Fig. 1. Calculationin a neural cell. niques, Bazet, France). Its average pore diameter was
1.4 /xm. The filtration experiments presented in this
INPUT OUTPUT paper were carried out with total recycling (without
LAYER HIDDENLAYERS LAYER
concentration) and at a constant temperature of 80°C.
The procedure of cleaning between two filtrations was
described by Punidadas [ 2 ].
Described in detail in our previous work, two types
of experiments were carried out. The first series was
conducted at constant transmembrane pressures (Ptm)
between 1.50 to 3.00 bar and constant crossflow veloc-
ities (U) between 4.0 to 6.0 m / s [24]. The second
t", I"1 • s ~f•"" / S~JS
,-j/
Biases/~/•/ t/ • • • series of experimental data was obtained varying Ptm
from 0.20 to 2.25 bar and Ufrom 2.2 to 5.0 m / s during
Fig. 2. Schematicstructure of a multilayerperceptronwith n inputs the first minutes of filtration [ 25 ].
(1) and m outputs (O). The raw cane sugar originally came from La R6union
(France) and was commercialized by La G6n6rale Su-
ever, a constraint has to be considered: the total number cri~re (Marseille, France). The sugar syrups after dilut-
of the weights of the network should at most be equal ing in water at 50°C had a dry matter content of 60 g/
to one third of the data from the learning base. If this 100 g. This corresponds to the dry matter value during
condition is not satisfied, the number of parameters to the decolouring stage which takes place after the clar-
identify will be very high compared to the available ification process in industry [26]. At 80°C, the density
information. of this syrup was 1.251, with a dynamic viscosity of
- Choice of data base: the learning base should be as 5.2 mPa s and a pH of 6.3.
representative as possible. It is preferable that it does
not favor any particular operating parameter and that it 3.2. Use o f neural networks
does contain experimental data over the whole para-
metric region studied. The test base, however, should The transmembrane pressure and the crossflow
be significantly different from the learning base and velocity which are the principal hydrodynamic para-
should contain data sets sufficiently far from each other. meters define the first two inputs of the network. In
In order to ensure the validity of the study, at least one order to include the dynamic component in the model,
third of the set of data should be reserved for the test the simplest solution was chosen. This presented
base. explicitly the time at the input of the network. The total
hydraulic resistance defined by Darcy's law (Rt) was
modeled:
3. Experimental
Ptm
Rt = (1)
3.1. Filtration experiments ,0Jp
The software used was' ' B P " (Back-Propagation) ver-
The pilot plant used was connected to an automatic sion 1.0. Installed on work stations Hewlett-Packard
control system with a programmable microprocessor 9000-705 and 9000-730, this software imposes the
266 M. Dornier et al. / Journal of Membrane Science 98 (1995) 263-273
sigmoidal activation function given by Eq. (2), and a
constant learning rate in the back-propagation algo-
rithm. Details can be found in the work of McClelland
and Rumelhart [27].
1
f(x) = (2)
l + e -x
Three criteria were used to take into account the devi-
ation of the predicted values from the experimental
ones. The mean quadratic error,/~ [Eq. (3)], directly
estimates the standard deviation of the error of the
model. The variation coefficient, y [Eq. (4)],
expresses the quadratic error in terms of the percentage
of the experimental mean value. The determination
coefficient, R 2 [ Eq. (5) ], compares the quantity of the
information satisfactorily described by the model in
comparison to the total information.
/~= i=l (3)
n-1
J~
y = ~ . 100 (4)
n ^
R2=(1 i=~nZ
(X/ X_~)
2/.100 (5)
g(x,-x)2J
i=1
where, on the considered data base, n is the number of
experimental values, X; the ith experimental value, Xi
the ith calculated value, and X mean of experimental
values.
The experimental data were not prefiltered. The input
and output values were centred at 0.5 between 0.05 and
0.95 taking into account the activation function [Eq.
(2) ]. In order to limit the local minima problem, four
calculations were carried out after different randomized
initiations of weights between + 0.5 and - 0 . 5 . The
best results obtained are only presented below.
4. Results
Firstly, the dynamic modeling of fouling at constant
operating pressure and velocity will be discussed. Sec-
ondly, the application of neural networks to the filtra-
tion experiments conducted at variable operating
conditions will be presented.
4.1. Studies at constant operating conditions
In the first series of experiments, transmembrane
pressure and crossflow velocity were held constant dur-
ing the course of the filtration process. Different pres-
sure/velocity combinations were tested. Fig. 3 shows
these graphically in parametric space. Following each
experiment, the evolution ofR t = f(t) was recorded for
120 min. One registration (data file) contained ~ 400
data points.
4.1.1. Search o f a suitable hidden structure
Five experiments were carried out for the learning
stage to find a suitable network for our particular case
(Fig. 3a). This choice provided a good representation
of the parametric experimental region (with one exper-
iment in the centre and four others regularly distributed
in the periphery) as well as a perfect symmetry with
respect to the two experimental parameters Ptm
and U.
Four experiments were carried out as test in order to be
representative for the parametric space during gener-
alization. Various mono- and bi-layer hidden structures
were then tested:
- Monolayer hidden structures: progressively increas-
ing the number of neural cells from 0 to l 1 in a single
hidden layer, we found that the variation coefficients
from the learning base as well as from the test base first
decrease then pass through a minimum and tend to
increase slightly afterwards (Fig. 4). An optimum
number of hidden neural cells was thus found. The best
results were obtained with the structure NN8.
- Bilayer hidden structures: 16 bilayer structures were
tested changing the number of neural cells from 2 to 5
in the two hidden layers. The best results, from both
the learning and test base, were obtained with the struc-
ture NN5/3 (Table 1). This structure contains 8 hidden
neural cells which corresponds to the number of neural
cells that gave the best results in the monolayer struc-
ture. This bilayer structure seems to improve the quality
of modeling. In fact, the total coefficient of variation
decreased by ~ 8% with respect to the best results
obtained with monolayer structures.
Following these results, our study focused on the
 M. Dornier et al. / Journal of Membrane Science 98 (1995) 263-273 267

A
W
[] []

[] []
A
W

m
m

Experiments used in
learning base
[]
• [] Experiments used in
test base

[] •

d • !

I m
u

~ 6
U (m/s)

Fig. 3. Different distributions of learning and test bases in the transmembrane pressure (Ptm) and crossltow velocity (U) region explored.

hidden structure that gave the lowest variation coeffi-
cient, i.e., NN5/3 (Fig. 5). Comparing all the experi-
mental and calculated values from the learning stage,
we see that the model represented the data in a very
satisfactory way: the calculated values were very close
to the experimental points and the five curves were
almost superposed (Fig. 6). The four curves obtained
from the test base were also well represented by the
model although for the experiment carried out at 2.78
bar and 4.3 m/s, the model slightly underestimated the
values (Fig. 7). Nevertheless, according to the R 2
value, the neural network NN5 / 3 allowed to represent
268 M. Dornieret al. /Journal of MembraneScience98 (1995)263-273

18. more than 97% of the information contained in the

whole data base.
16;

14.
4.1.2. Importance of the quality of information gained
12. during the learning stage
In the following paragraphs, the study of the effect
10.
of decreasing and increasing the quantity of informa-
tion presented during the learning stage on the perform-
6.
ance of the model will be discussed. The optimum
hidden structure obtained before is used ( N N 5 / 3 ) .
4 • , • , • , • , • , • , • , • , • , • , • ,

0 1 2 3 4 5 6 7 8 9 10 11
Table 1 summarizes the principle results presented
Hidden neural cells below.
Decreasing the data in the learning base. In order to
Fig. 4. Variation coefficients (~/) versus number of hidden neural determine the quantity of minimum information
cells (monolayer hidden structures, filtrations at constant operating required, the number of data presented to the model
conditions, 5 experiments in the learning base). during the learning stage has been decreased:
- Four experiments in the learning base: it is necessary
to choose experiments in the centre and periphery of
the parametric region (in order to conserve a correct
representation of the parametric space). The distribu-
tion schematically represented in Fig. 3b was chosen.
It is noteworthy that this distribution does not cover the
whole parametric region studied and that it is more
Ill /~L'
representative in the region o f low pressures and low
× velocities. Three experiments were used for the test
base. The variation coefficients obtained in this case
X were comparable to those obtained with five experi-
× ments in the learning base. The decrease of information
~Ot did not have a significant effect on the prediction error.
W e found a good representation of various experiments
as before (Fig. 8).
- Three experiments in the learning base: the distribu-
tion in Fig. 3c was chosen. Two experiments were used
for the test base. For the network studied, the errors
Biases were significantly higher - twice as much - compared
to the results previously obtained with 5 or 4 experi-
Fig. 5. Schematic representation of the neural network NN5/3.
ments in the learning base. Therefore, it could not be
considered for the dynamic modeling of fouling during
Table 1
Effect of the quantity of information used during the learning stage on the modelingquality ( NN5/ 3, filtrationsat constant operating conditions)

Number ofexpedments used /~ (10 I° m -1) 3' (%) R2 (%)

in the learning base
Learning base Test base Total base Learning base Test base Total base Learning base Test base Total base

5 13.8 29.5 22.3 4.4 9.1 6.9 98.8 96.2 97.4

4 11.6 34.1 23.9 3.6 9.3 7.0 99.5 93.8 97.5
3 45.7 51.4 48.0 13.5 14.1 13.8 93.9 80.8 91.1
6 18.7 23.4 20.4 5.4 6.2 6.3 98.2 97.0 97.8
 M. Dornier et al. /Journal of Membrane Science 98 (1995) 263-273 269

700

600
Ptm = 3.00 b,,r
U - 5 . 0 m/s
500

4GO

=
200

100

£..
::1 Ptm = 2.25 bar
U = 4.0m/s
Ptm = 2.2S bar
U = S.Om/s
Ptm = 2.25 bar
U = 6~, m/s

vd~
J
_J~_.
=

o:
o 20 IOO 120 20 40 60 gO 100 120
600 P~m = I J O b a r (mlu)
U= S.Omh

=
[o. ]
100

ame (m~n)

Fig. 6. Total hydraulic resistance (Rt) versus filtration time obtained at different constant transmembrane pressures (Ptm) and crossflow velocities
(U). Experimental and calculated curves according to NN5/3 on the learning base.

7o0

6oo Ptm = 2.7B bar

U = 5 . 7 m/s
50o.

Ptm = 2.78 bar

U =4.3m/s

P l m = 1.72 bar Ptm = 1.72 bar

U =4.~m/s U :: 5.7 m/s

~J
IOO

o
r • . , . ,
r
. .
I

.
a

.
i IJ

I .° x'l
Fig. 7. Total hydraulic resistance ( Rt ) versus filtration time obtained at different constant transmembrane pressures (Ptm) and crossflow velocities
(U). Experimental and calculated curves according to NN5/3 on the test base.
270 M. Dornier et al. /Journal of Membrane Science 98 (1995) 263-273

700.

600. Learning base

O0
0 0

- 500.

400.

300
0 Oq
0

200

100

600 Test base

O

, 500.
O

O O

~ 200.

100,

• i i u i u u

0 100 200 300 400 500 600 700

Experimental Rt (101° m"1)

Fig. 8. Comparison between experimental and calculated total hydraulic resistance ( R t ) with 4 experiments in the learnning base (NN5/3,
filtrations at constant operating conditions).

the whole filtration time. After examining the different
curves, we found that the model did not represent sat-
isfactorily the beginning of filtration. However, the
model showed well the fouling evolution in the quasi-
stationary phase. Then the learning base with only three
experiments allowed to evaluate the total hydraulic
resistance evolution in time from 60 to 120 min of
filtration with a good precision.
Increasing the data in the learning base. The objec-
tive in this case was to quantify the effect of an aug-
mentation of the quantity of information presented in
the learning stage on the performance of the model.
This last distribution is represented in Fig. 3d. The
analysis of the variation coefficients showed a signifi-
cant improvement of the performance of the network
studied. Hence, the total quadratic mean error was
diminished by 9% compared to the best results obtained
previously. This model therefore appears to be better.
The curves obtained from simulations present a posi-
tive curvature in the quasi-stationary phase which does
not coincide with the experimental observations (Fig.
9). Although the mean error of the prediction has been
improved, these results do not appear to be satisfactory.
Following these studies, a distribution with 4 exper-
iments in the learning stage seems to be largely suffi-
cient to obtain a good representation of the whole set
 M. Dornier et al. / Journal of Membrane Science 98 (1995) 263-273 271

300.
filtration experiments conducted under operating con-
ditions varied in time. The data collected in this second
part of our study also represents the evolution of
200.
_ ,, o s. R t = f(t). The operating conditions were varied during
~ 1517.
the start-up procedure with more or less progressive
increase of P~m and U [ 25 ]. Different recordings (data
100 files) were less homogeneous since the sampling fre-
0 Experimental
quency and filtration time were variable. A recording
50
,.. C . a l e u l a t t ~ l contained 250 to 440 data points. The learning and test
, , , , • , , . , , , , ,
bases were made up respectively of 4 and 3 experi-
I0 20 30 40 50 60 70 80 90 100 110 120 130 ments.
time (min)
The weights obtained with a learning base under
Fig. 9. Comparison between experimental and calculated total constant operating conditions were used for the mod-
hydraulic resistance (R0 with 6 experiments in the learning base.
eling of the experiments carried out under variable con-
Example at Ptm= 1.5 bar and U= 5 m/s (NN5/3, filtrations at con-
stant operatingconditions). ditions. In this case, we found that the model elaborated
did not satisfactorily represent the experimental data
of data. Since 2 experiments were considered for gen- particularly during the initial stages of the experiment.
eralization, a total of 6 experimental values will be A new learning base with experiments obtained at var-
required. The introduction of the filtration time at the iable conditions would be required to improve this.
input of the network, has allowed to diminish strongly When a learning base was acquired for time variable
the number of different combinations of pressure and conditions, the results obtained were considerably bet-
velocity to be tested experimentally to elaborate this ter. As can be seen in Figs. 10 and 11, the simulated
type of model. curves followed the same trend as the experimental
ones for the initial stages as well as after the establish-
4.2• Studies at variable conditions
ment of the quasi-stationary regime. On the whole data
The objective was to investigate the capacity of the base,/~, T and R 2 were respectively 43.1 × 101° m - 1 ,
neural models to represent the evolution of fouling for 16.1% and 87.4%. Only in the first part of the curve G

3OO

it

~g
100 J
A '~ . . . . . . . . . . . . B
0 .

'l

0 20 40 60 80 I00 120 140 160 0 20 40 60 80 I00 120 140 160 IgO

UU~ (wan) ~ (m/u)

Fig. 10. Total hydraulic resistance (Rt) versus filtration time obtained with time variable operating conditions. Experimental and calculated
curves accordingto NN5/3 on the learning base (/~= 39.2 X 10~°m- ], y = 14.4%, R 2= 90.3%).
272 M. Dornier et al. /Journal of Membrane Science 98 (1995) 263-273

satisfactory representation of the evolution of the total

hydraulic resistance during filtration for both constant
,"" 300. - - ~ and variable operating conditions. These predictive
0
dynamic models can also find numerous applications
in the field of crossflow filtration.
For filtrations carried out under constant conditions,
6 experiments were sufficient to establish the models
in the tested parametric range. Hence, the quantity of
experimental tests that needed to be carried out on a
E pilot scale was quite low. The quality of the predictions
obtained showed that neural networks can be used to
predict the evolution of the hydraulic resistance during
the time course in the whole parametric region
explored. The model can directly be exploited to predict
the hydraulic resistance at time t, as well as the rate of
membrane fouling, over the whole range of transmem-
~ I00
brane pressures and crossflow velocities studied.
The results obtained at variable conditions showed
that neural networks can effectively be used to study
the complex effects of variations of operating condi-
tions on membrane fouling. The choice of the learning
300. and test data base is, however, delicate and requires a
more advanced prospective study. Once confirmed, this
tool will open numerous perspectives for the automa-
tization and optimization of the process.
In order to achieve this, it is envisaged to validate
100 this type of models with other experimental cases
(other product/membrane combinations, larger ranges
G of operating conditions) for both constant and time
0
0 " 2~0 " 4() " 60 " 80 " 100" t20" 1~10- 160 " 180 variable conditions and to extend our study to other
lime (rain)
types of networks, notably to recurrent networks.

o Experimental I
• Calculated
6. List of s y m b o l s
Fig. I 1.Totalhydraulicresistance(Rt) versusfiltrationtimeobtained
withtimevariableoperating conditions. Experimentaland calculated Ai activation of the neural cell i ( - )
curves accordingto NN5/3 on the test base (/]'=47.4× 10~°m-~, mean quadratic error on Rt ( m - 1)
T= 17.9%,R2= 83.4%). permeate flux (1 h - 1 m - z or m s - 1)
Ptm transmembrane pressure (bar or Pa)
(test base), the hydraulic resistance was overestimated R2 determination coefficient (%)
for the first 50 min of filtration. No satisfactory expla- NNx neural network with monolayer hidden
nation was found for this deviation. structure: x neural cells in the hidden layer
NNx/y neural network with bilayer hidden structure:
x and y neural cells in the first and second
5. Conclusions hidden layer, respectively
g t total hydraulic resistance defined by Darcy's
The application of neural networks to crossflow law (m -1)
microfiltration has shown that these models allow a s, stimulation of the neural cell i ( - )
 M. Dornier et al. /Journal of Membrane Science 98 (1995) 263-273
U crossflow velocity (m s- t )
weight of the connection between the neural
wi)
cell i (receptive) and the neural cellj
(emissive) (-)
7 variation coefficient (%)
~p dynamic viscosity of permeate
(mPa s or Pa s)
Acknowledgements
This study was carried out in collaboration with Elec-
tricit6 de France (E.D.F.), DEpartement Applications
de l'Electricit6 dans l'Industrie, Centre de Recherche
des Renardi~res, B.P. 1, 77250 Moret sur Loing,
France.
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