Separation and Purification Technology 70 (2009) 96–102

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Separation and Purification Technology

journal homepage: www.elsevier.com/locate/seppur

Prediction of microfiltration membrane fouling using artificial neural

network models
Qi-Feng Liu a , Seung-Hyun Kim a,∗ , Sangho Lee b
a
Department of Civil Engineering, Kyungnam University, 449 Wolyoung-dong, Masan 631-701, Republic of Korea
b
Korea Institute of Construction Technology, Gyeonggi-Do, 411-712, Republic of Korea

a r t i c l e i n f o a b s t r a c t

Article history: In this study, artificial neural network (ANN) models were applied to predict the performance of micro-
Received 23 April 2009 filtration (MF) system for water treatment. A series of bench scale experiments were conducted at critical
Received in revised form 17 August 2009 flux and supra-critical flux conditions with various permeate fluxes and feed water qualities. The effects
Accepted 25 August 2009
of operating parameters on membrane performance were evaluated based on the comparison of trans-
membrane pressure (TMP) as a function of operating time. The ANN models used five input variables
Keywords:
including permeate flux (Jw ), feed water turbidity (Turf ), UV254 , time (h), and backwash frequency for
Microfiltration
predicting corresponding TMP. The modeling results indicated that there was an excellent agreement
Artificial neural networks
TMP
between the experimental data and predicted values. Nevertheless, selection of database for training is
Fouling important for the accuracy of ANN prediction. Relative weights of each input variable were calculated to
find out key operational factors affecting the performance of MF system.
© 2009 Elsevier B.V. All rights reserved.

1. Introduction
Although there are handfuls of models available for the anal-
ysis of membrane fouling, it is still difficult to get a quantitative
prediction of filtration performance based on them with various
design and operational conditions. This is because membrane foul-
ing results from complicated physical and chemical interactions
between membrane and feed waters. Resistance-in-series model
provides a legibly physical description of fouling mechanism but
fail to apply in real practice. The mass transfer or film theory
model is also limited for practical use because they only analyze
the fouling behavior in steady state. The classical blocking laws
[1] are useful to understand fouling mechanisms such as complete
pore blockage, intermediate pore blockage, pore constriction and
cake filtration. But the blocking laws require a number of idealized
assumption and they are applicable in a relatively short operating
period.
During last two decades, artificial neural network (ANN) models
have drawn attention as a new approach for determining com-
plex relationships between many input variables and outputs. ANN
models have potential to describe highly non-linear behaviors such
as flux decline or resistance increasing under different conditions.
Therefore, they are suitable for use in pilot or full scale membrane
plants where mathematic models cannot be applicable.
∗ Corresponding author. Tel.: +82 55 249 2671; fax: +82 55 249 2664.
E-mail address: shkim@kyungnam.ac.kr (S.-H. Kim).
Therefore, a few works have been done for the application of
ANN models in membrane filtration. Delgrange et al. [2] developed
an ANN models to predict the evolution of the total hydraulic resis-
tance of a pilot plant producing drinking water by ultrafiltration
(UF) of natural water. Five inlets including temperature, turbid-
ity, permeate flow rate, resistance at the filtration start and before
previous backwash, have shown to be sufficient to correctly pre-
dict the total resistance at the end of current filtration period and
after next backwash. Cabassud et al. [3] developed a model consist-
ing of two interconnected recurrent neural networks coupled with
the Darcy’s law. The model inputs are water quality parameters
(turbidity, pH, dissolved oxygen, UV absorbance, TOC, tempera-
ture, oxido-reduction potential) and operating conditions during
filtration time (permeate flow rate, circulation flow rate) and dur-
ing backwash (filtration time, chlorine concentration in backwash
water, backwash pressure, backwash duration). The results showed
that the optimized conditions using ANN models provided higher
performance of membrane system compared to typical operating
conditions in industry.
Piron et al. [4] developed a hybrid model, which combined neu-
ral network with semi-physical approach for the crossflow MF
process to filter suspensions of baker’s yeast. The hybrid approach
appears to be more accurate and is a means for complementing the
description of a physical model. Hamachi et al. [5] proposed a recur-
rent neural network to describe the evolution of permeate flux and
deposit thickness based on the inlets parameters: transmembrane
pressure, crossflow velocity, concentration of the suspension and
the starting point values for permeate flux and deposit thickness.

1383-5866/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.seppur.2009.08.017
 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102
According to the results obtained, this ANN model is able to repre-
sent the evolution of deposit thickness and permeate flux, and may
sometimes even bring a sufficient correction for deposit thickness
evolution.
Other applications of neural networks in different membrane
filtration were found in following literatures. For crossflow mode,
Chen and Kim [6] used radial basis function neural network
(RBFNN) to predict the long-term permeate flux with feed water
parameters such as particle radius, solution pH, and ionic strength
as inputs. Curcio et al. [7] presented a neural network, which has
been built on the basis of the experimental results collected during
UF of bovine serum alumin (BSA) solutions under pulsating con-
ditions. Sahoo and Ray [8] tried to use genetic algorithm (GA) to
search the optimal geometry and values of internal parameter of a
multiplayer feedforward back-propagation neural network (BPNN)
and a RBFNN. For dead-end filtration, Mhurchú and Foley [9] stud-
ied the correlation of specific cake resistance and flux data using
ANN models. The network weights were interpreted to evaluate
the relative effect of the input parameters on the specific cake
resistance and the steady-state flux.
However, the application of ANN models in membrane fouling is
still limited. Most studies focused on constant pressured operation
using flat membrane in a short term operating period. On the other
hand, most membrane filtration plants adopt constant flux mode
with hollow fiber membrane to satisfy the requirement of constant
productivity and compactness.
Therefore, this study focuses on the test of ANN models under
operating conditions similar to those in membrane filtration plants.
The experiments were conducted using a hollow fiber membrane
module under constant flux mode with periodic backwashing. A
synthetic water, simulating the characteristics of surface water,
was used as feed water to minimize the impact of water quality
variations. The obtained operating parameters and experimental
results are used as training database for an ANN model.
The first objective of this study is to evaluate the effects of
permeate flux, feed water quality, and backwash strategies on
membrane performance. The second objective is to predict and/or
simulate membrane fouling behavior using well trained ANN mod-
els at conditions, which are relatively similar to real practices.
2. Theory of artificial neural network
In general terms, an NN can be understood as a nonlinear func-
tion that transfers certain inputs into outputs via a training process.
This process can be described by the following equation.

p
yj = ωji xi + bj
i=1
where xi represents the input to a neuron, p is the number of input
nodes, ωji is the corresponding weight from ith to jth neurons, and
bj is bias of the jth neuron. The expected output yj is obtained via
adjusting weights ωji in the networks.
After a neuron performs its function, it passes its output to all
of the neurons in the layer below it, providing a feed-forward path
to the output through a non-linear transfer function. The transfer
function is one of fundamental elements, which correlate inputs
with outputs in various ways based on different transfer func-
tions. Three of the most commonly used functions are the hard
limit transfer function, the linear transfer function, and the sig-
moid transfer function. Selecting the appropriate transfer function
and algorithm can avoid the NN stuck in local minima and improve
the generalization performance in a certain extent.
Another important issue for building statistical models is the
choice of the appropriate inputs. The inputs must be indepen-
dent, representative and easily measurable. For membrane process,
97
Fig. 1. ANN models architecture employed in this study with an input layer, two
hidden layers, and one output layer. Inputs parameters are permeate flux (Jw ), raw
water turbidity (Turf ), UV254 (cm−1 ), operating time (h), backwash types and the
output is TMP data. The binput , b1 , b2 represent the biases for the input and hidden
layers, respectively.
usually, the inputs consist of some operational and feed water qual-
ity parameters that most possibly affect membrane fouling. Once
inputs are selected and data are divided into training, validation
and test sets. The next step is to design the network architecture.
Designing a certain type of architecture involves choosing the num-
ber of layers and the number of neurons per layer. When choosing
the number of hidden neurons, too few are insufficient to solve the
problem and too many may easily cause overfitting. The maximum
number of hidden neurons also depends on the number of train-
ing cases available. Overfitting takes place when the fitting process
progresses beyond a certain point and the ANN models, instead of
learning the basic features of the variables being modeled, starts to
learn various idiosyncrasies associated to the random noise varia-
tion of the particular data. In these cases, the ANN models obtained
generalize poorly and will not yield accurate predictions for new
observations.
The problem of overfitting can be avoided using a third indepen-
dent validation data set to assess the performance of the model at
various stages of learning. Training will stop when the error in this
validation set reaches a minimum. This approach is known as early
stopping. Training a network usually starts from random values of
the parameters to estimate. After building any model, an impor-
tant aspect is the evaluation of its performance when faced with
the testing subset. The most widely used measures of agreement
for a model are the Pearson correlation coefficient R and its square
(1) R2 .
3. Materials and methods
3.1. Neural network architecture in this study
The neural network toolbox in Matlab 7.0 was used to model the
experimental data. The optimal network structure was determined
to include two hidden layers, one input layer, and one output layer
(see Fig. 1) where 5 neurons in the input layer and 1 neuron in
the output layer. The neurons in the two hidden layers were deter-
mined using the trial try-and-error method (Fig. 2). Since 5 neurons
in the first hidden layer combined with 8 neurons in the second hid-
den layer represent the best performance, they are selected as the
hidden neuron numbers in this model. The ANN input layer con-
sists of permeate flux, feed water turbidity, UV254 , backwash types
(enhanced and normal backwash) and operating time. The output
is the TMP. Network input and output are normalized between 0
and 1 to avoid numerical overflows due to very large or very small
98 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102
Fig. 2. Effect of number of hidden neurons on accuracy of fouling predictions.
weights. The normalization equation used is of the following form:
xi − xmin

xi =
xmax − xmin

where xi is the normalized value of xi . The xmax and the xmin are
the maximum and minimum value of xi , respectively. The sigmoid
function
1 Fig. 3. The whole dataset included the minimum and maximum val-
f (yi ) =
1 + exp(−yi )
was used as a transfer function. The Levenburg-Marquardt tech-
nique was used as the back propagation algorithm to improve the
learning rate and stability of the BP algorithm for searching the min-
imum mean square errors between data and fit values (MSE). An
intermediate learning rate of 0.2 was chosen because a lower value
increases the convergence time, whereas, a higher value results in
an unstable network. The weights for each input were randomly
initialized between −0.5 and 0.5. Network learning was performed
in batch mode to ensure convergence to a global minimum of MSE.
The weights were updated only after all the inputs were presented.
The network was trained separately until the MSE decreases below
10−4 for each pressure. If this desired tolerance was not attained
even after performing 10,000 iterations (training cycles or epochs),
the initial weights are reassigned and the training was resumed
until the MSE decreases below 10−4 .
1
ntrain
MSE = (yi,exp t − yi,pred )2
2
i=1
Fig. 3. Three-dimensional plots of NNs training and validating data distribution. (A) Parameters of time, turbidity and flux. (B) Parameters of time, UV254 , and backwash
types.
Table 1
Summary of data sets used for ANN models.
Data/sets parameters Set I (training and validation) Set II (test)
Flux (LMH) 75–150 100
Turbidity (NTU) 1.6–8 5.5
UV254 (cm−1 ) 0.101–1.350 0.28
Backwash frequency 10 s/5 min and 30 s/30 min 30 s/30 min
where yi,exp t is the ith experimental value, yi,pred is the corre-
sponding ANN prediction, and ntrain the number of points used for
network training (learning). This approach was classified as super-
vised learning because the desired output is provided during the
training phase.
3.2. Database
Databases were built based on a series of experiments under
different feed water compositions and operating conditions. The
experimental method was described in detail in Section 3.3. Total
(2) 938 data were obtained for ANN models. Among these results, 625
data were used for training and 313 were used for validation. The
generalization of the well trained ANN models was verified by other
52 data, which has not been used in training process (Table 1). The
distributions of training, validation and test data sets are shown in
(3) ues of permeate flux, feed water turbidity, UV254 , and two types of
backwash strategies. The test data were obtained from the experi-
ment in the range of these extreme conditions.
3.3. Experimental set-up
An outside-in polyvinylidene fluoride (PVDF) hollow fiber mem-
brane (Kolon, Korea), having an average pore size of 0.1 ␮m and
17.3 cm2 of effective filtrated area, was used in this study. A single
hollow fiber housed in a plastic tube of 6 mm inner diameter with
the upper part sealed by epoxy resin forms a dead-end module
(DEMF).
A DEMF system is shown in Fig. 4. Constant flow was pumped
into membrane module via a variable speed peristaltic pump
(MasterFlex® L/S, Model 7014-20). The TMP was recorded every
10 s by pressure gauge ISE 40-01-22 which was subsequently trans-
ferred to the computer by data acquisition Agilent 34970A. A
magnetic stirrer was used to ensure supply of homogeneous feed
(4) solution during membrane filtration. The system was automatically
controlled via the programmable logic controller (PLC).
 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102 99

Fig. 5. TMP as a function of time for both synthetic water and distilled water exper-
iments with step increasing fluxes.

protocols used by Chan et al. [10], Huisman et al. [11], and Choi
and Dempsey [12]. The critical point was found at the flux of
75 L m−2 h−1 in this study due to the phenomena of TMP “jump”
occurred when flux was higher than this point (see Fig. 5). Based
on these results, a set of filtration experiments were conducted
under critical flux (75 LMH) and supra-critical flux (120 or 150
LMH), respectively.

4.2. Effects of feed water quality

Fig. 4. Diagram of the bench-scale DEMF system used in this study.
To investigate the effects of raw water quality on membrane
Table 2 fouling potential, three types of feed water were used as shown
The characteristics of the synthetic feed water. in Table 2. Fig. 6 shows TMP as a function of time fed with three
Parameters/ Turbidity UV254 (cm−1 ) pH Temperature types of feed water. The results indicate that TMP increasing rate is
water types (NTU) (◦ C) directly proportional to the concentration of turbidity and UV254
I 1.5–1.7 0.100–0.102 8.14–8.21 25
causing material. Feed water with higher turbidity and UV254
II 6.1–6.3 0.116–0.118 8.48–8.55 25 accelerated fouling rate both in critical flux (75 LMH) and supra-
III 7.9–8.1 0.345–0.358 8.34–8.47 25 critical flux (150 LMH) conditions. This is because more particles
and organic compounds tend to deposit on membrane surface or
penetrate in membrane pores at higher contaminant concentra-
3.4. Feed solution and analytical methods tion.
In addition, there was an inflection point when the operation
All chemicals used in this study are reagent grade or better. reaches certain time in each experiment. Initially, the rate of TMP
There are three different type of synthetic water (types I, II, III). The increase was high and became low after the inflection point. First, it
synthetic water type I contains 2.5 mg/L of kaolinite, 2.5 mg/L of alu- was suspected that reduced permeate flow might be responsible for
mina, 5.0 mg/L of Aldrich humic acid (AHA), 0.5 mM of NaHCO3 , and this phenomenon since flow rates may decrease with applied pres-
0.2 mM of CaCl2 . The synthetic water represents the typical river sure. Thus, flow rates are checked over an entire filtration period.
in Korea, which is the major drinking water source. The amount The result showed that the flow rates were constant over an entire
of Georgia kaolinite is increased to 7.5 mg/L for type II water. The filtration period, indicating that the inflection of TMP is not caused
amount of Georgia kaolinite and AHA increased to 7.5 mg/L and by flow reduction.
15 mg/L for type III water, respectively. Kaolinite and alumina par- Instead, the inflection point can be attributed to the changes
ticles are dispersed in distilled water and the suspension is placed in fouling rate during filtration. There are several possibilities
in an ultrasound bath for 20 min, then NOM, NaHCO3 and CaCl2 for these phenomena. First, the physico-chemical interactions
were added and the suspension is mixed for an hour. The synthetic between membrane and foulants can be changed during filtration
water is prepared and characterized (turbidity, pH, UV254 , temper- because the membrane surface is being covered by foulants, leading
ature) everyday. The characteristics of the synthetic raw water are to a change in surface properties. This may shift the fouling mech-
summarized in Table 2. anisms from pore blocking to cake formation. Second, the foulant
The characteristics of the synthetic raw water and the filtrate layer formed outside of the membrane surface may have critical
(UV254 , turbidity, and pH) are analyzed using the following instru- thickness above which the foulant layer erosion is becoming more
ments: Shimadzu UV-2101 UV/vis spectrophotometer, Dr. Mini important. Finally, backwash of membrane can limit the growth of
DMT 110 for turbidity, and pH meter 410A. foulant layer above a certain point.

4. Results and discussion 4.3. Effects of permeate flux

4.1. Determination of critical flux Experiments using three types of feed water were conducted
at critical flux (75 LMH) and supra-critical flux (150 LMH). Fig. 7
Prior to the filtration experiments, the critical flux was deter- compares the TMP profiles under different operating conditions.
mined using the “flux-steps” method that is consistent with the As expected, TMP slowly increased for the experiments at crit-
100 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102

Fig. 6. Three type of feed water at flux of 75 LMH and 150 LMH.

Fig. 7. Three types of feed water with flux of critical flux (75 LMH) and supra-critical flux (150 LMH), respectively.

ical flux while it rapidly increased at supra-critical flux. These
results are consistent with our previous research [13] indicating
the importance of critical flux on optimizing membrane perfor-
mance.
4.4. Effects of backwash frequency
Fig. 8 presents TMP as a function of time with different
feed water and backwash frequencies. The results indicate that
enhanced backwash effectively retarded membrane fouling in both
types of feed water. The effect of backwashing became more impor-
tant for the filtration of feed water with higher concentration of
contaminants. Removal of cake layer formed on membrane sur-
face by backwashing seems to be the reason for this permeability
improvement.
4.5. ANN training and simulation
The neural network was trained using more than 120 epochs
before SSE reaches the aim of 10−4 . The training and validation
squared error versus epochs is plotted in Fig. 9.
The performance of a trained network can be measured by per-
forming a regression analysis between the network response and
the corresponding targets. Fig. 10 illustrates the network outputs
versus the experimental data of TMP. A dashed line indicates the
best linear fit. The solid line indicates the perfect fit (output equal
to target). A perfect fitting curve would make the slope as 1, and the
y-intercept as 0. The R-value is the correlation coefficient between
the outputs and targets. It is a measure of how well the variation
in the output is explained by the targets. The R-value is 0.85 in this
study, implying that there is high correlation between targets and
outputs.
After training, the ANN was used to predict TMP profile under
conditions that are not included in the training database. The ANN
prediction was compared to experimental data in Fig. 11A. The ANN
models matched with the experimental data within first 10 h, but
it failed to predict TMP changes after 10 h. The differences between
experimental data and ANN models prediction was attributed to
the deficient training database.
Accordingly, new data set was added to the training database to
improve the accuracy of ANN models prediction. Additional exper-

Fig. 8. Two types of feed water (types I and III) with different backwash frequency.
 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102 101

Fig. 9. The illustration of the ANN training squared error versus time.

iments were conducted at flux of 120 LMH with type III feed water
and the results were used for further training. Fig. 11B shows that
the ANN models prediction improved with training database being
added. The new ANN models matched experimental data very well
and the correlation coefficient R-value reaches to 0.98. These results
suggest that the database for ANN training is critical for prediction
accuracy.

4.6. Evaluation of relative importance of input parameters

ANN is trained to perform a complex function by adjusting the

values of the connections (weights) between elements. Each input
parameter is endowed with an initial weight. The initial values of
the weights have strong effect on the finial weights obtained for
the trained network [9]. Thus, the relative effect of input parame-
ters can be analyzed from the variety of their weights. The simple
arithmetic mean is used. The weight of each parameter is divided
by the summation of the total absolute weights of all parame-
ters.
Fig. 11. (A) The TMP as a function of time of both network out and experimental
data. (B) The TMP as a function of time of both network out and experimental data.
Fig. 12 shows the mean results of five times training. Among
many variables, time (t) seems to be the most important (0.30)
in predicting experimental results. Except for time, the other four
input variables seem to have similar impact (0.17). It is likely that
this approach of calculating the relative effects of each input param-
eters is useful for better understanding how each variable affects
the membrane performance.

Fig. 10. Regression analysis between the network response and the corresponding
targets. Fig. 12. The mean relative effects of input parameters on the TMP.
102 Q.-F. Liu et al. / Separation and Purification Technology 70 (2009) 96–102

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