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chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

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Chemical Engineering Research and Design


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

Experimental investigation, modeling and optimization of


membrane separation using articial neural network and
multi-objective optimization using genetic algorithm
Reza Soleimani a , Navid Alavi Shoushtari b , Behrooz Mirza c , Abdolhamid Salahi d,
a

Department of Gas & Chemical Engineering, Petroleum University of Technology (PUT), Ahwaz, Iran
Department of Chemical & Petroleum Engineering, Sharif University of Technology, Tehran, Iran
c Department of Chemistry, Faculty of Science, South Tehran Branch, Islamic Azad University, Tehran, Iran
d Department of Applied Chemistry, Faculty of Science, East Tehran Branch, Islamic Azad University, Tehran, Iran
b

a b s t r a c t
In this work, treatment of oily wastewaters with commercial polyacrylonitrile (PAN) ultraltration (UF) membranes
was investigated. In order to do these experiments, the outlet wastewater of the API (American Petroleum Institute) unit of Tehran renery, is used as the feed. The purpose of this paper was to predict the permeation ux and
fouling resistance, by applying articial neural networks (ANNs), and then to optimize the operating conditions in
separation of oil from industrial oily wastewaters, including trans-membrane pressure (TMP), cross-ow velocity
(CFV), feed temperature and pH, so that a maximum permeation ux accompanied by a minimum fouling resistance, was acquired by applying genetic algorithm as a powerful soft computing technique. The experimental input
data, including TMP, CFV, feed temperature and pH, permeation ux and fouling resistance as outputs, were used to
create ANN models. This fact that there is an excellent agreement between the experimental data and the predicted
values was shown by the modeling results. Eventually, by multi-objective optimization, using genetic algorithm (GA),
an optimization tool was created to predict the optimum operating parameters for desired permeation ux (i.e. maximum ux) and fouling resistance (i.e. minimum fouling) behavior. The accuracy of the model is conrmed by the
comparison between the predicted and experimental data.
2012 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Keywords: Industrial oily wastewater; Ultraltration; Permeation ux; Fouling resistance; Multi-objective optimization; Articial neural network

1.

Introduction

Oil polluted wastewater has been recognized as one of the


most concerned pollution causes. This kind of wastewater
comes from variety of sources such as oil renery, petrochemical industry and metal processing. The oily wastewater
is considered as hazardous industrial wastewater, because it
contains toxic substances which inhibitory to plant and animal growth and also mutagenic and carcinogenic to human
being. Issues of water pollution needed to be resolved urgently.
These wastes are usually treated by a number of physical, chemical and biological techniques in water treatment
units, before being disposed in the environment or reused as

agricultural water. One of the treatment techniques used for


oil separation from wastewater is membrane ltration (Salahi
et al., 2010a).
As membrane technology has been applied for wastewater treatment, it has been growing rapidly due to the need
for high quality water requirements. Membrane technology
in wastewater treatment has signicant progresses in recent
years. Despite their expensive investment and construction
costs, membrane processes are widely employed due to their
success in reducing efuent concentrations to as low as 5 mg/L
(Mulder, 2002). Fouling is generally a problem in membrane
ltration, especially in the ltration of wastewater. This phenomenon was a damaging appearance in the membrane

Corresponding author. Tel.: +98 21 33580330; fax: +98 21 33580330.


E-mail address: hamidsalahieng@gmail.com (A. Salahi).
Received 14 June 2012; Received in revised form 19 July 2012; Accepted 3 August 2012
0263-8762/$ see front matter 2012 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.cherd.2012.08.004

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chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

process. Wastewater oil content can exist in several forms


of free, dispersed, emulsied and dissolved oils. The differences are based primarily on size. In an oil/water mixture free
oil is characterized with droplet sizes greater than 150 m in
size, dispersed oil has a size range of 20150 m, emulsied
oil is dened as having particle sizes ranging from 1 to 20 m
and dissolved oil has droplets typically less than 1 m. Mean
particle size of oil droplets in this study was set at 0.75 m.
Free oils can be readily removed by gravity separation. However microltration (MF) can be applied to remove dispersed
and emulsied oils, but it is inefcient in separation of dissolved oils. UF membranes are composed of some type of
polymer material with pores ranging from a little less than
0.01 m to 0.1 m, so these membranes are attractive choice
for removing of tiny particles (dissolved oils) in oily wastewater. In oily wastewater research area, the UF membrane
process presents indisputable advantages such as no need
to chemical reagent, the ultraltrated water shows approximately no oil content and the UF plants are quite compact
and are fully automated (Loeb and Sourirajan, 1964). So the
research and development on the UF behavior of oil/water
emulsion have been investigated global. The application of
UF to the treatment of oil/water separation has been reported
(Anderson and Saw, 1987; Dal-Cin et al., 1998; Lin and Lan,
1998; Viadero et al., 2000).
Nowadays polymeric membranes including UF process
are used for numerous applications in industries (Barzin
et al., 2004). Membrane UF is a pressure driven process used
for separation, purifying and concentrating macromolecular
(11000 kDa) solutions (Cheryan, 1986; Sirkar, 1996).
Quantication of the effects of basic parameters such as
CFV, TMP, feed temperature, pH and molecular size of solutes
on membrane fouling in UF is not completely understood.
In this way, there is not a completed theoretical model,
accomplishes to quantitatively describe UF process so accurately (Susanto et al., 2009; Vela et al., 2008; Kim et al., 1997;
Koltuniewicz et al., 1995; Marchese et al., 2000). Accordingly,
there is an increasing interest to select optimum operating
parameters that take apart in process such as TMP, CFV, feed
temperature and pH in order to reduce the fouling resistance
and simultaneously increase permeation ux. Optimization
of membrane processing by simulation or modeling is a challenging task. Because there are a large number of parameters
as mentioned above to be consider. In this context, utilization
of soft computing was appeared to be an interesting practice,
which was the aim of this paper.
Recently, machine learning (ML) techniques, such as
articial neural network (ANN), genetic algorithm (GA) optimization, genetic programming (GP) and fuzzy logic modeling,
because of their ability to model and analyze complex problems that were previously difcult or impossible to solve, have
been increasingly used in membrane separation. In the recent
years, modeling of membrane processes via neural network
has been received immense attention, the ANN application of
these articles was summarized in Table 1. According to this
table, it can be concluded that ANN modeling of UF was most
frequently observed in the literature. For example ANNs have
been successfully applied to predict membrane fouling during
UF of drinking water process (Delgrange et al., 1998a), colloids
(Bowen et al., 1998a), proteins (Bowen et al., 1998b). In another
study Teodosiu et al. (2000) utilized ANN to show the ability of
neural network for prediction of the ux during UF of wastewater. Razavi et al. (2003a) have been successfully employed
ANN to estimate the milk UF performance.

Genetic algorithm (GA) has been used to solve multi objective optimization problems such as membrane separation
modules (Yuen et al., 2000), membrane gas separation systems (Chang and Hou, 2006) and reverse osmosis desalination
units (Guria et al., 2005). Genetic programming (GP) has been
used to simulate membrane processes, such as prediction of
membrane fouling in a microltration (MF) system (Hwang
et al., 2009), and prediction of ux decline during MF of
oily wastewater (Shokrkar et al., 2012). Finally, Madaeni and
Kurdian (2011) used fuzzy logic modeling and hybrid GA
optimization of virus removal from water using MF. It was
observed that fuzzy inference system (FIS) predicted rejection and ux during MF for different operating conditions,
with an acceptable error. It is fairly observed that ANN models are used to study as simple single-objective optimization
problems, using genetic algorithm (i.e. coupling of ANN and
GA). For instance, the effects of polymer and additive concentrations on membrane performance were investigated by
validated ANN, and the optimum concentrations to achieve
maximum ux (single-objective) for quaternary systems
(PES/PVP/DMAc/IPA + water), and (PS/PVP/DMAc/IPA + water)
were estimated by genetic algorithm and assembled ANN
(Madaeni et al., 2010). But in most cases, conicting requirements and constraints govern the optimal choice of decision
variables. In fact, these optimization problems may involve
several objectives, some of which must be maximized, while
the others minimized simultaneously. There have also been
some attempts to model UF/MF of the oily wastewater via
soft computing; however, the effect of operating conditions
on permeation ux and fouling resistance has not been precisely modeled by such intelligent approaches (i.e. coupling of
ANN and GA), on the other hand in our knowledge, no record
for coupling ANN modeling accompanied by multi-objective
optimization using genetic algorithm of UF of oily wastewater
was found in the literature.
In this paper we pursued two goals, development of two
distinctive neural network models for prediction of permeate ux, and fouling resistance during UF of industrial oily
wastewater was the primary goal of the current research. The
developed models were useful tools to analyze the effects of
feed temperature, TMP, CFV and pH on permeation ux of
cross-ow UF of industrial oily wastewater and the fouling
mechanisms involved in cross-ow UF of the industrial oily
wastewater. And nally the optimum operating conditions to
achieve maximum ux and minimum fouling resistance (twoobjective optimization) for cross-ow UF of oily wastewater
were estimated by genetic algorithm and assembled ANNs.

2.

Materials and methods

A schematic diagram of the batch pilot-scale membrane unit


operated in this study is shown in Fig. 1. This is a crossow membrane system. Experiments were carried out using
a at sheet polyacrylonitrile (PAN, 20 kDa) membrane, from
Sepro membrane (USA). From hydrophilic property towards
hydrophobic characteristic the membranes can be arranged as
follows PAN > PES (polyethersulfone) > PVDF (polyvinylidene
uoride). PAN membrane with hydrophilic group (CN) has
high permeate ux, this membrane combines high selectivity with high permeation rate in other words. High rejection,
low fouling resistance and also high mechanical strength
are another features of PAN membranes. As we know spiral
wound membrane module uses at sheet membrane element,

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

885

Table 1 Summary ANN application of researchers studies in modeling of membrane processes.


References
Niemi et al. (1995)
Dornier et al. (1995)
Al-Shayji and Liu (1997)
Piron et al. (1997)
Delgrange et al. (1998a)
Bowen et al. (1998a)
Bowen et al. (1998b)
Delgrange et al. (1998b)
Hamachi et al. (1999)
Bowen et al. (2000)
Teodosiu et al. (2000)
Delgrange-Vincent et al. (2000)
Jafar and Zilouchian (2001)
Al-Shayji and Liu (2002)
Bhattacharjee and Singh (2002)
Cabassud et al. (2002)
Shetty and Chellam (2003)
Shetty et al. (2003)
Razavi et al. (2003a)
Razavi et al. (2003b)
Lee et al. (2004)
Razavi et al. (2004)
Fu et al. (2005)
Chellam (2005)
Geissler et al. (2005)
Ou and Achenie (2005)
Zhao et al. (2005)
Abbas and Al-Bastaki (2005)
Curcio et al. (2005)
Aydiner et al. (2005)
Rai et al. (2005)
Cinar et al. (2006)
Wang et al. (2006)
Curcio et al. (2006)
Sahoo and Ray (2006)
Ni Mhurchu and Foley (2006)
Chen and Kim (2006)
Shahsavand and Pourafshari Chenar (2007)
Al-Zoubi et al. (2007)
Darwish et al. (2007)
Liu and Kim (2008)
Cheng et al. (2008)
Al-Abri and Hilal (2008)
Hilal et al. (2008)
Sadrzadeh et al. (2008)
Liu et al. (2009)
Sadrzadeh et al. (2009)
Libotean et al. (2009)
Purkait et al. (2009)
Sarkar et al. (2009)
Shokrian et al. (2010)
Guadix et al. (2010)
Madaeni et al. (2010)
Nandi et al. (2010)
Baroutian et al. (2010)

ANN application
Simulation of RO membrane separation
Modeling of cross-ow MF
Modeling and optimization of large-scale commercial water desalination plants
Modeling of cross-ow MF
Prediction of UF transmembrane pressure
Prediction of the rate of cross-ow membrane UF of colloids
Dynamic modeling UF of proteins
Modeling of UF fouling
Dynamic modeling of cross-ow MF of bentonite suspension
Predicting salt rejection at NF membranes
Predicting the time dependence of ux evolution in UF
Prediction of fouling and backwash efciency in UF for drinking water
production
Modeling of an RO water desalination
Modeling of large-scale commercial water desalination plants
Modeling of a continuous stirred UF process
Predictive control algorithm to improve the productivity of an UF plant
Predicting membrane fouling during municipal drinking water NF
Predicting contaminant removal during municipal drinking water NF
Dynamic modeling of milk UF
Dynamic prediction of milk UF performance
Modeling of polymer electrolyte membrane FC performance
Predicting the permeate ux and total hydraulic resistance during cross-ow
milk UF
Modeling of the adsorption of bovine serum albumin on porous polyethylene
membrane
Modeling of transient cross-ow MF of polydispersed suspensions
Modeling of capillary modules in MBR
Modeling of proton exchange membranes
Predicting RO/NF water quality
Modeling of an RO water desalination
Analyze of UF membrane systems behavior
Modeling of ux decline in cross-ow MF
Modeling batch UF of synthetic fruit juice and mosambi juice
Modeling of submerged MBR treating cheese whey wastewater
Modeling of hydrogen recovery from renery gases
Modeling the reduction and control of ux decline in cross-ow UF
Prediction of ux decline in cross-ow membranes
Correlating specic resistance and ux of Dead-end ltration of yeast
suspensions
Prediction of permeate ux decline in cross-ow membrane FT
Modeling the separation of CO2 from CH4 using hollow ber module
Modeling the rejection of sulphate and potassium salts by NF
Simulation of the ltration of sodium chloride and magnesium chloride
solutions using NF membranes
Evaluation of membrane fouling
Predicting effect of interparticle interactions on permeate ux decline in
crossow membrane ltration (CMF) of colloidal suspensions
Simulation of combined humic substance coagulation and membrane ltration
Prediction of permeate ux and rejection for separation of bentonite in tubular
ceramic MF membranes
Prediction separation percent of lead ions from wastewater using ED
Prediction of MF membrane fouling
Modeling of Pb2+ removal from wastewater using ED
Forecasting RO plant performance and for potential use for operational
diagnostics
Prediction of permeate ux in treatment of leather plant efuent using NF
followed by RO
Prediction of permeate ux during electric eld enhanced cross-ow UF
Predicting separation factor during C3 H8 separation from CH4 and H2 using a
synthesized PDMS membrane
Predicting the ux decline in milk cross-ow ceramic UF
Modeling and optimization of membrane fabrication
Predicting ux in oily wastewater using low cost ceramic membrane
Simulation the rate of methanol recovery

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chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Fig. 1 Schematic diagram of the laboratory scale cross


ow ltration system.
therefore the data were collected in this study and consequently modelling results that were achieved can be used in
ltration of industry oily wastewater.
The unit included a UF membrane placed in a stainless
steel module, feed and permeate tanks, feed sanitary centrifugal pump, recycle and permeate ow meters, and heat
exchanger. The feed pump had a closed impeller with six
reversed blades especially t to transfer liquid at media-high
pressure in order to optimize the hydraulic efciency. The
cross-ow ltration was also run for 2.5 h.The feed pumps
had a maximum discharge pressure of 15 bar and a maximum
capacity of 5 m3 /h for UF membrane system. The feed was
pumped from the feed tank toward the cell. Concentrate was
returned to the tank. Therefore, the feed concentration in the
circulation loop remained virtually constant. To analyze permeate after each run it could be collected in the permeate
sample. The feed tank was Plexiglas, with a capacity of 50 L
and two walls which allowed the feed temperature to be kept
constant using the circulation of cooled water or heater. The
membrane permeation ux was measured by collecting the
permeate in an Erlenmeyer ask and using a digital balance.
The inlet pressure and CFV were controlled by the by-pass and
outlet valves, respectively. The cross sectional area of the cell
was 0.75 cm2 and membrane surface area in contact with uid
was 66 cm2 . A shell and tube type heat exchanger is included in
the feed stream to control temperature. TMP and feed temperature measurements were obtained from thermocouples and
pressure transducers located at the membrane inlet and outlet. The recycle retentate and permeate ows were measured
with variable section ow meters.
Wastewater disposal of API separator of Tehran renery
wastewater treatment unit was employed as the feed. The
results of treatment of oily wastewater by PAN membranes
listed in Table 2. From the results presented in Table 2, it can
be observed that the treatment efciency is relatively high.
This shows that the membrane was able to effectively treat
the wastewaters.
Table 2 Characteristics of the wastewater and the
treated wastewater.
Parameter

Unit

Feed

Ultraltration

Turbidity
Total suspended solids (TSS)
Oil and grease content
Total organic carbon (TOC)

NTU
mg/L
mg/L
mg/L

53
60
78
81

0.4
Trace
0.2
19

Samples for measurements of the feed and the permeate


total organic carbon (TOC), turbidity, total suspended solids
(TSS), and oil content were taken as necessary and analyzed
by the procedure outlined in the standard methods (APHA,
2001).
After each set of experiments with oily wastewater feed,
the system was rinsed with water, and then pure water ux
was measured again under the conditions of initial testing
until the steady state was attained. During the experiments,
CFV, TMP, feed temperature, ltration time, oil concentration and pH, were carefully controlled. All of the adjustments
and measurements for the combined membrane experiments
were the same.
For each experiment a raw PAN membrane was used, so
we have no fouling in starting of any experiment. In other
words the conditions of applying membranes are identical in
all experiments.
Many parameters affect performance of the UF process. It is
believed that feed temperature, TMP, CFV and feed pH have the
greatest effect on permeate ux and fouling resistance. Four
factors were adjusted each with three levels (low, medium and
high) as follows:

Temperature (T): 25, 37.5 and 50 C


TMP: 1.5, 3 and 4.5 bar
CFV: 0.25, 0.75, 1.25 m/s
pH: 4, 7 and 10

and the numbers of whole observations equaled to 81.


Theoretically, steady-state is supposed to occur in crossow ltration (in this study after 2.5 h) but this steady-state
condition is not a rigorous steady-state condition but a
quasi-steady-state condition in actual cross-ow ltration
applications. This is due to the fact that although permeate
ux is nearly constant for long time scales, it decreases very
slowly until a permeate ux of zero is obtained for very long
time scales.
The permeate was collected for 2.5 h and the pure water
permeate ux (L/m2 h) was calculated using the following
equation:
J=

V
At

(1)

where A is the membrane area, V is the collected permeate volume and t is 2.5 h. All of the adjustments and measurements
for the UF experiments were the same.
Flux shows the amount of permeate rate. Fouling resistance
shows the signicance of cake/gel layer on the membrane surface. The ux was measured gravimetrically with an electronic
balance with weighting the permeation.
Fouling resistance (Rf ) was calculated as follows:
Rf =

 P   P 
Jww

Jwi

(2)

where P is the TMP,  is the solution viscosity, Jwi is the initial


water ux and Jww is the water ux after fouling.

3.

Theory

3.1.

Articial neural network

In accordance with the human brain, an ANN model, usually called neural network (NN) model, is composed of an

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

interconnected assembly of neurons and dendrites. Neurologists have found that the human brain learns by changing the
strength of the synaptic connection between neurons upon
repeated stimulation by the same impulse. Inspired by the biological neural system, the ANN model learns the training set
by adjusting the values of inter-neuron connection strengths
(weights) between processing elements (neurons), until the
network output approximates the target (training examples),
based on a comparison between the output and the target.
According to Fig. 2 there are 3 basic elements of an articial
neuron:
i. A set of synapses connections (connecting links), whose
strengths are represented by a set of weights and a bias:
X = X1 , X2 , . . ., Xn (a vector of model input signals) with corresponding weights: W = Wk1 , Wk2 , . . ., Wkn and b = (bk ). The
synapses store parameters called weights that manipulate the data in the calculations. Their values will directly
effect on the output of the neural network.
ii. The total synaptic input, Sk , to the neuron k is given
by the inner product of the input and weight vectors:
Sk = (Wkj Xj + bk ) (it is assumed Wk0 = bk and X0 = 1), where
k = [1, r], (r = number of neurons in one layer) and j = [1, n]
(n = number of input). In other words, the input signal X
is multiplied by the weight W and summed in the adder
with all the other items. The result of this summation S
will go to the input of the activation function.
iii. The activation function that converts a neurons weighted
input to its output activation. [Total synaptic input is
transformed to the output via the activation function]:
Yk = (Sk ). The activation function has a key role in the
scheme of a neuron. It generated the output according
to the summed input signals calculated in the adder.
Abridged, the output signal of neuron can be dened as
follows: Yk = ((Wkj Xj + bk )).
The neurons formed a layer and the layers interconnected
to another forms of NN. A NN is thus typically dened by
its model inputs and its architecture: the number of layers,
the number of neurons in each layer, the activation function
in each layer that converts a neurons weighted input to its
output activation and the way in which the layers are interconnected (the learning process for updating the weights and
biases of the interconnections).
The multi-layer perceptron (MLP) architecture, a feed
forward-type NN, usually has good model performance, and
also it is the most common neural network model used in
membrane processes (Dornier et al., 1995; Bowen et al., 1998b;
Jafar and Zilouchian, 2001; Lee et al., 2004; Al-Zoubi et al.,
2007; Shokrian et al., 2010). A MLP maps sets of input data
onto a set of appropriate output. In this type of feed forward
neural network model, each layer consists of a group of neurons that share the same input and output connections, but
that does not interconnect with the other neurons forming
the same layer. Also, connections are strictly oriented in a
directed graph: from the input toward the output. Mathematically, MLPs with one input layer, one hidden layer and one
output layer by applying sigmoid transfer function for the hidden layer and linear transfer function for the output layer
(purelin) are known to be universal approximators (Hornik
et al., 1989).
NN training is the process by which the weights and biases
are adjusted systematically so that the network exhibits some
desired or interesting behavior. Mathematically training a

887

network is meant to minimizing the error of a cost function,


such as the mean squared error function. A commonly used
performance function is the mean-squared error (MSE), which
tries to minimize the average squared error between the networks output, pi , and the target value (true value) ti over all
the example pairs, dened as

N
MSE =

i=1

(ti pi )

In general, training can be supervised, unsupervised.


Supervised: In this type of learning the ANN is trained
through a given input/target data training pattern includes
input pattern associated with the corresponding target or
desired pattern. As the inputs are applied to the network, the
network outputs are compared to the targets. The learning
rule is then used to adjust the weights and biases of the network in order to move the network outputs closer to the targets
in such a way to minimize an error function between the two
values.
Unsupervised: There is no target in unsupervised training
and the system must be learnt by discovering and adapting
to structured features in the input pattern. This is done by
adapting itself to regularities in the system, according to the
rules implicit in its design. The nature of regularities found
by the system depended on details of its design. Simply, in
unsupervised learning, the weights and biases are modied
in response to network inputs only.
In our knowledge Back-propagation which is a supervised training algorithm is by far the most commonly used
method for training MLPs especially in membrane separation processes (Bowen et al., 1998b; Teodosiu et al., 2000;
Bhattacharjee and Singh, 2002; Lee et al., 2004; Chen and Kim,
2006; Sadrzadeh et al., 2008; Shokrian et al., 2010). Minimizing
MSE by back-propagation involved the computation of and
of its derivative, for that this method requires that activation
functions are differentiable as the weight update rule is based
on the gradient of the error function which is dened in terms
of the weights and activation functions.
Although back-propagation has been used successfully on
a wide range of problems, one of the common disadvantages is
that it is slow, therefore the LevenbergMarquardt algorithm
(trainlm) that provides faster training can be chosen as the
optimization tool, because of its proven computing efciency
and high performance (Tan and Van Cauwenberghe, 1999). The
weight and bias update procedure of the LevenbergMarquardt
back-propagation training algorithm uses an approximate
Hessian matrix for the second derivatives of the cost function
(Coulibaly et al., 2000).
When training multilayer networks, the general practice is
to rst divide the data into three subsets. The rst subset is
the training set used for updating the network weights and
biases. The second subset is the validation set. The validation
error normally decreases in initial steps of training, as does
the training set error. Nevertheless, when the network begins
to overt the data, the error of the validation data increase.
When the validation error increases for a specied number
of iterations, the training is stopped and the network weights
and biases are saved at the minimum of the validation set
error. In the domain of training data sets, the test set was used
to evaluate the predictive ability of the network. The test set
error is not used during training, but it is used to compare
different models.
The three transfer functions demonstrated in Fig. 3
were the most commonly used transfer functions for back

888

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Fig. 2 Schematic representation of single neuron with n inputs.


propagation, but other differentiable transfer functions can be
created and used with back propagation if desired.

3.2.
Multi-objective optimization using genetic
algorithm

Linear transfer function (purelin)

Optimization is a procedure of nding and comparing feasible solutions until no better solution could be found. When
an optimization problem involves more than one objective
function, the task of nding one (using higher-level qualitative
considerations) or more optimum solutions is known as multiobjective optimization (Srinivas and Deb, 2002). Optimization
problems that have more than one objective functions are
rather common in every eld or area of knowledge.
Many, or even most, real engineering problems actually
done, have multiple-objectives, i.e., minimize cost, maximize
performance, maximize reliability, etc.; in such problems, the
objectives to be optimized are normally in conict with respect
to each other, which means that there is no single solution
for these problems, and optimizing a particular solution with
respect to a single objective that can result in unacceptable
results with respect to the other objectives. Therefore, a practical (reasonable) solution to a multi-objective problem is to
investigate a set of solutions, each of which satised the objectives at an acceptable level without being dominated by any
other solution. So, none of the solutions can be considered
to be better than any other with respect to the all objective
functions.
General multi-objective optimization problem (MOP) solution methods range from classical approaches to population
based techniques. Unlike classical search and optimization
methods that usually work with a point-by-point principle
and, thus, are required to be applied many times, each time
nding one pareto-optimal solution. Evolutionary Algorithms
(EAs), are suited well to multi-objective optimization problem
as they are able to capture multiple pareto-optimal solutions in a single simulation run. EAs are computer-based
problem solving systems which are computational models of

(s) = s

(4)

which is regularly used in the output layer. The main interest


of MLPs resides in their nonlinear sigmoid function (such as
logsig and tansig) principally used in their hidden layer.
Log-Sigmoid transfer function (logsig)
(s) =

1
1 + es

(5)

which is easily differentiable, is frequently nonlinear transfer


function used for engineering application. However, because
it is limited between 0 and 1, its linearly transformed type is
used instead. It is known as the bipolar transfer function
(s) =

2
1
1 + es

(6)

which is bounded between 1 and +1.


Hayperbolic Tangent Sigmoid (tansig)
(s) =

es es
es + es

(7)

which is very alike in form and shares many mathematical


properties with the bipolar transfer function and it is bounded
between 1 and +1. It is also frequently used in engineering
application.

Fig. 3 Typical transfer functions: (a) logsig, (b) tansig and (c) purelin.

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

evolutionary processes as key elements in their design and


implementation. These algorithms are proved to be a, exible,
robust and powerful search mechanism also simple implementation and broad applicability of these algorithms proved.
GAs have been the most well-known EA approach to multiobjective design and optimization problems (Deb, 1999; Konak
et al., 2006). GA relies on the evolution of solution populations. In a GA, the genome tness is the driving mechanism
of the genetic evolution, and hence, a crucial parameter in
determining the effectiveness and efciency of a GA-based
multi-criteria algorithm (Barakat et al., 2008). The multiobjective genetic algorithm can solve smooth or non-smooth
optimization problems with or without bound and linear
constraints; also it does not require the functions to be differentiable or continuous.
The multi-objective problem in its general form (mathematical representation) is presented as:
m = 1, 2, . . . , M

Minimize/Maximize fm (x),

(8)

subject to
hj (x) 0(is the inequality constraints),
gk (x) = 0 (is the equality constraints),

(lb)

xi

(ub)

xi xi

j = 1, 2, . . . , J

(9)

k = 1, 2, . . . , K

(10)

(is the bound constraints),

i = 1, 2, . . . , n
(11)

where f1 (x), f2 (x), . . ., fM (x) are the objective functions.


Multi-objective optimization is concerned with the minimization/maximization of multiple objective functions that
are subjected to a set of constraints. In multi-objective optimization, the effort must be made in nding the set of
trade-off optimal solution by considering all objectives to be
important.
(1)
(2)
A solution xi is said to dominate the other solution xi , if
both the following conditions are true (Deb, 2001):
(1)

(2)

(1)

(2)

1 xi dominates xi if xi is not worse than xi in all objectives.


(1)
(2)
2 xi is strictly better than xi in at least one objective.
A solution is said to be Pareto optimal if it is not dominated
by any other solutions in the solution space. A pareto optimal solution cannot be improved with respect to any objective
without worsening at least one other objective. The set of
all feasible non-dominated solution in x, is referred to as the
pareto optimal set, and for a given pareto optimal set, the corresponding objective function values in the objective space is
called the pareto front.
Multi objective optimization uses a concept of domination
by comparing between two solutions. If a feasible solution is
not dominated by any other feasible solutions of the multiobjective optimization problem, a solution is said to be a
non-dominated solution. For a given set of solutions or corresponding points on the objective space, for example, those
shown in Fig. 4, the non-dominated solutions are the black
circle. One property of any two such points is that a gain in
an objective from one point to the other happens only due to
a sacrice in at least one other objective and the dominated
solutions are clear circle. Pareto optimal points are also known

889

Fig. 4 A set of solutions (corresponding points) of


objective functions.
as efcient, non-dominated or non-inferior points that are in
the relationship of trade-off solutions.
Summary, if the given set of points for the multi-objective
optimization task contain all points in the search space
(assuming a countable number), the points lying on the nondomination front, by denition, do not get dominated by any
other point in the objective space, hence are pareto-optimal
points (together they constitute the pareto-optimal front) and
the corresponding decision variable vectors are called paretooptimal solutions.
There are many formulations or methods of multi objective GA such as Multi-objective Genetic Algorithm (MOGA)
(Fonseca and Fleming, 1993), Niched Pareto Genetic Algorithms (Horn et al., 1994), Non-dominated Sorting Genetic
Algorithm (NSGA) (Srinivas and Deb, 1994), Strength Pareto
Evolutionary Algorithm (SPEA) (Zitzler and Thiele, 1999),
Random Weighted Genetic Algorithm (RWGA) (Murata and
Ishibuchi, 1995), Rank-Density Based Genetic Algorithm
(RDGA) (Lu and Yen, 2003) and fast Non-dominated Sorting
Genetic Algorithm (NSGA-II) (Deb et al., 2002). Elitist Nondominated Sorting GA (NSGA-II) is one of the popularly used
evolutionary multi-objective optimization (EMO) procedures,
which attempt to nd multiple pareto-optimal solutions in a
multi-objective optimization problem. Because of (1) robustness and easily congurable to a variety of engineering
problems and (2) the algorithm was shown to generally outperform other algorithms the NSGA-II was used which is the
advanced version of NSGA. Generally, multi-objective GA differs based on their tness assignment procedure, elitism, or
diversication approaches. Detail differences of these algorithms are comprehensively described in the literature (Konak
et al., 2006).

4.

Methodology

We had two purposes in this paper: First, constructing two


models, capable of predicting the permeate ux and fouling
resistance according to the variation in operating conditions.
ANN was selected as the primary modeling tool to carry out
the task. Temperature, TMP, CFV and pH were input arguments (independent variables) to the networks and for one
network permeation ux and another one fouling resistance
were target arguments (dependent variables). For these two
targets, two distinctive networks were made. Feed-forward
architecture with a LevenbergMarquardt back-propagation
training algorithm was utilized to develop the models, which
is a proper algorithm in agreement with the literature (Shetty

890

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Fig. 5 Structure of the constructed two-layer feed-forward articial neural network to predict (a) permeation ux and (b)
fouling resistance.
Table 3 Settings used in the development of the permeate ux and fouling resistance neural networks.
Network type

FFBP
Performance function
MSE

Training function

TRAINLM
Time
Goal
Inf.
0

Epochs
1 103

Layer no.

2
max fail
6

et al., 2003; Abbas and Al-Bastaki, 2005; Chen and Kim, 2006;
Liu and Kim, 2008; Sadrzadeh et al., 2008, 2009; Shokrian
et al., 2010). For the rst and second targets, permeation ux
and fouling resistance, the optimal number of neurons of
hidden layer of networks was accomplished using trial and
error method. Results demonstrated that each network with
8 neurons in their hidden layers gave the smallest error. The
numbers of neurons were tested for the hidden layer of each
network ranged from 5 to 20. Shamseldin et al. (1997) claimed
that the best way to determinate this number (number of neurons in hidden layer), is trial and error (Shamseldin et al.,
1997). The structure of the networks and various settings in
adjustment of neural networks are given in Fig. 5 and Table 3,

Neuron no.

min grad
1 1010

Transfer function

Layer #1

Layer #2

Layer #1

Layer #2

8
mu
1 103

1
mu inc
10

TANSIG
mu dec
1 101

PURELIN
mu max
1 1010

respectively. To evaluate the performance of the ANN model,


the total 81 experimental data were randomly divided into
three subsets of training, validation and testing, as you can
see in Table 4. The entire experimental data obtained were
Table 4 Select percentages in modeling of permeate
ux and fouling resistance.
Function

Algorithm

Dividerand
Training ratio
Validation ratio
Test ratio

Divide the data randomly


0.70
0.15
0.15

57 samples
12 samples
12 samples

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

891

Fig. 6 Distribution of (a) training, (b) validation and (c) testing data sets for permeation ux and fouling resistance versus
operating parameters.
trans-TMP, CFV, temperature, pH, permeate ux and fouling
resistance. The ranges of the used database for the models
are shown in Table 5. For better visualization, Fig. 6 shows
the three-dimensional plots of distribution of training, validation and testing data sets for both outputs (i.e. permeation
ux and fouling resistance) versus operating parameters. After
the network has been created and all weights and biases
were initialized by the use of the NguyenWidrow method,

Table 5 Range of variables.


Measures
T
TMP
CFV
pH
PF
FR

Parameters

Temperature ( C)
Trans-membrane pressure (bar)
Cross-ow velocity (m/s)
pH ()
Permeation ux (L/m2 h)
Fouling resistance (1/m)

Min
25
1.5
0.25
4
65.22
43.67

Max
50
4.5
1.25
10
212.93
220.19

the network becomes ready to be trained. During the training,


the weights and biases of the network were systematically
updated to minimize a performance function (MSE in this
study) between the desired (target) output(s) and the network
output(s).
As previously mentioned another goal of the paper was to
assemble a system that can efciently estimate the optimal
operating parameters of a desirable permeation ux (maximum) and fouling resistance (minimum) simultaneously. To
achieve this goal, genetic algorithm seemed to be most useful. A program was developed to facilitate the procedure. It
took two neural models developed for predicting permeation
ux and fouling resistance. It then searched the space of
possible solutions created by the neural models to nd the
optimal operating parameters. Genetic optimization found the
optimal operating parameters by minimizing the error (tness) function. The error function is dened as mean square
error (MSE) among all the predicted two-objective functions

892

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Fig. 7 Hybrid systems owchart in optimization of operating parameters.

(permeation ux and fouling resistance) values and the


desired values:
1
2
(pi di )
N
N

ErrorFunction =

(12)

i=1

where pi and di are the predicted and desired objective functions, respectively. Fig. 7 provides a schematic diagram of
the neural-genetic hybridization. Each iteration dened new
input parameters to the already trained neural network. The
genetic optimizer then evaluated networks outputs and compared them with the desirable permeation ux and fouling
resistance. The genetic evolution converged stochastically to
design parameters that caused the greatest decline in the error
function. The algorithm proceeded with its iterations until a
specied performance criterion was satised.

5.

Result and discussion

After preparing the neural model, it is necessary to measure its performance. Performance efciency of the networks
was evaluated using the measured and ANNs estimated
value. Some important statistical parameters for training,
validation and testing data divisions of permeate ux and fouling resistance were calculated and these are summarized in
Tables 5 and 6, respectively. Tables 6 and 7, reports the ANNs
performances in terms of mean percentage error (MPE), mean
absolute percentage error (MAPE), mean squared error (MSE),

root mean square error (RMSE), normalized mean squared


error (NMSE), mean absolute error (MAE), the coefcient of
determination (R2 ) between the real targets and neural network outputs and correlation coefcient (R). Briey, the ANN
predictions are optimum if MPE, MAPE, R, R2 , MAE, NMSE, MSE
and RMSE are found to be close to 0, 0, 1, 1, 0, 0, 0 and 0,
respectively.
Coefcient of determination (R2 ) showing the amount of
variation the model is able to describe. R2 is a statistic that will
give some information about the goodness of t of a model.
In regression, the R2 is a statistical measure of how well, the
regression line approximates the real data points. An R2 of 1.0
indicates that the regression line perfectly ts the data.
The experimental results versus neural networks predictions for three subsets of data are plotted in Figs. 8 and 9
for permeate ux and fouling resistance, respectively. Performance of the selected networks (4:8:1) is portrayed in
Figs. 8 and 9. The coefcient of determination is found to be
more than 0.99 for both network predictions. This indicates
that the neural networks have been well trained.
Correlation coefcient (R) measures the correlation
between outputs and targets. An R value of 1 means a close
relationship, 0 a random relationship. The R value is calculated
by taking the square root of the coefcient of determination
(R2 ) value.
Mean square error (MSE) measures the average of the
squares of the errors that is the amount by which the value
implied by the model differs from the quantity to be observed,

250
Training data

Predicted permeaon ux (L/m2.h)

Validaon data
Tesng data

200

150

100

50

0
0

50

100

150

Experimental permeaon ux (L/m2.h)

200

250

R = 1

Fig. 8 Plot between experimental and neural network predicted permeate ux.

893

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Table 6 Different quality measures evaluated for the trained permeate ux neural model.

MPE
MAPE
Standard Deviation of Observations
Standard Deviation of Predictions
MSE
RMSE
NMSE
MAE
R2
R

Training

Validation

Testing

2.671E06
1.137E04
37.4224928
37.4224935
3.545E08
1.883E04
2.532E11
1.512E04
9.999E01
9.999E01

1.742E04
3.516E04
28.2035008
28.2035040
5.227E07
7.230E04
6.571E10
5.270E04
9.999E01
9.999E01

2.371E04
5.540E04
26.7025211
26.7033796
2.020E06
1.421E03
2.833E09
8.811E04
9.999E01
9.999E01

Table 7 Different quality measures evaluated for the trained fouling resistance neural model.

MPE
MAPE
Standard Deviation of Observations
Standard Deviation of Predictions
MSE
RMSE
NMSE
MAE
R2
R

Training

Validation

Testing

1.386E07
3.234E05
41.500306076
41.500306081
1.761E09
4.197E05
1.023E12
3.260E05
9.999E01
9.999E01

1.277E05
8.004E05
40.841818913
40.841775696
2.246E08
1.499E04
1.347E11
9.654E05
9.999E01
9.999E01

9.106E04
9.798E04
48.413385086
48.413067523
1.234E05
3.514E03
5.267E09
1.095E03
9.999E01
9.999E01

when MSE approaches to 0 it represents that the error of our


model decreases. MSE has the same units of measurement as
the square of the quantity being predicted.
Root mean square error (RMSE) or root mean square deviation (RMSD) is a frequently used measure of the differences
between values predicted by a model and the experimental
values. RMSE is dened as the square root of the MSE. It is
a good measure of accuracy. Smaller value of RMSE means a
better performance of the model. The RMSE, also, describes
the average magnitude of the errors. The RMSE scores range
from 0 to (lower values are better), show the errors in the
unit and scale as the parameter itself.
Normalized mean squared error (NMSE) is the MSE
divided by  2 , the empirical variance of the observed values
calculated over all the N training patterns (Aussem and Hill,
2000). Smaller value of NMSE means a better performance of
the model.
Mean absolute error (MAE) is a quantity used to measure
how close predictions are to the eventual outcomes. As the
name implies, the mean absolute error is an average of the
250

Predicted fouling resistance (1/m)

Training data
Validaon data
Tesng data

200

150

100

50

0
0

50

100

150

Experimental fouling resistance (1/m)

200

R = 1

Fig. 9 Plot between experimental and neural network


predicted fouling resistance.

250

absolute errors, i.e. ti pi  where pi is the prediction and ti


the true value. As this error approaches to 0, the network is
our satisfaction. The mean absolute error is one of the ways
of comparing forecasts with their eventual outcomes. The
mean absolute error (MAE) describes the average magnitude
of the errors, without considering their sign (it is a linear score
because all errors are equally weighted). The MAE scores range
from 0 to (lower values are better), show the errors in the
unit and scale as the parameter itself.
Mean absolute percentage error (MAPE), also known as
mean absolute percentage deviation (MAPD) is a measure
of accuracy of a model that is applied for prediction. Very
small values of MAPE for the training, validation and testing
data sets prove that the network outcomes only show a small
amount of error. When having a perfect t, MAPE is 0. But in
regard to its upper level the MAPE has no restriction in other
words MAPE scores range from 0 to (lower values are better).
Mean percentage error (MPE) in statics is the computed
average of percentage errors by which estimated predictions
differ from actual values of the quantity being predicted. Very
small values of MPE for the training, validation and testing
data sets prove that the network outcomes only show a small
amount of error.
Eventually, equal quantities of standard deviation for
experimental and predicted data indicate that the true distribution of data around the mean is very well simulated by
the model (Reihanian et al., 2011).
The equations for statistical parameters are listed in
Appendix A. These gures and facts clearly demonstrate that
the neural network has been well trained, validated and
tested.
In Figs. 10 and 11, permeation ux (PF) and fouling resistance (FR) are plotted versus operating parameters in 3D
plots, respectively. The corresponding generalization performances of the selected structures (4:8:1 networks), as shown
in Figs. 10 and 11, show no oscillations, and it conrms an
excellent prediction performance of ANNs (Sadrzadeh et al.,

894

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Fig. 10 Generalization performances of 4:8:1 network, effects of (a) temperature and trans-membrane pressure at
CFV = 0.25 m/s and pH = 4, (b) temperature and cross-ow velocity at TMP = 4.5 bar and pH = 4, (c) temperature and pH at
TMP = 4.5 bar and CFV = 0.25 m/s, (d) trans-membrane pressure and cross-ow velocity at T = 37.5 C and pH = 4, (e)
trans-membrane pressure and pH at T = 37.5 C and CFV = 0.25 m/s and (f) cross-ow velocity and pH at T = 37.5 C and
TMP = 4.5 bar on permeation ux.
2009). In these gures, the 4:8:1 networks predictions are
indicated by the surfaces. As can be seen increasing temperature (Fig. 10ac) at the range of 25 C T 50 C increases
permeation ux, because viscosity decreases and diffusivity
increases at elevated feed temperature (Abbasi et al., 2010a).
Increasing TMP (Fig. 10a, d, e) at 1.5 bar TMP 4.5 bar
increases PF, according to Darcys law, increasing TMP
increases PF; however, fouling restricts this fundamental law.
Increasing TMP makes the oil droplets more compact on the
membrane surface and blocks the membrane pores (Abbasi
et al., 2010a; Ghidossi et al., 2009). It can be observed that, with
increasing TMP up to 3 bar, permeation ux increases linearly;
however, at higher TMP it increases with less steep. This may
be due to compression of the cake/gel layer formed on the
membrane surface at higher TMP. Increasing CFV (Fig. 10b, d,

f) at 0.25 m/s CFV 1.25 m/s increases PF through the membrane. Enhanced turbulence both reduces boundary layers and
improves UF membrane process performance (Hesampour
et al., 2008). The main reason is reduction of concentration
polarization effect. Turbulence and shear stress on the membrane surface are enhanced by increasing CFV (Madaeni and
Yeganeh, 2003). Therefore, the accumulated compounds on
the membrane surface are returned into the bulk of uid and
concentration polarization effect diminishes. In other words,
increasing permeation ux with CFV is due to the reduction of
concentration boundary layer and cake/gel layer thicknesses
(Salahi and Mohammadi, 2011a; Mohammadi and Esmaeelifar,
2005). The results show that, as CFV increases to about 0.751,
PF increases very considerably but at higher CFV this positive effect is not signicant. In other words, it increases with

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

895

Fig. 11 Generalization performances of 4:8:1 network, effects of (a) temperature and trans-membrane pressure at
CFV = 0.75 m/s and pH = 7, (b) temperature and cross-ow velocity at TMP = 1.5 bar and pH = 7, (c) temperature and pH at
TMP = 1.5 bar and CFV = 0.75 m/s, (d) trans-membrane pressure and cross-ow velocity at T = 25 C and pH = 7, (e)
trans-membrane pressure and pH at T = 25 C and CFV = 0.75 m/s and (f) cross-ow velocity and pH at T = 25 C and
TMP = 1.5 bar on fouling resistance.
less steep. It agrees with the results obtained by Madaeni and
Yeganeh (2003) and Salahi and Mohammadi (2011a). While
increasing pH has a dual effect on PF. As indicated in (Fig. 10c, e,
f) at 4 pH 10 increasing pH decreases permeation ux up to
a minimum value then increase. As observed, with acidic and
basic solutions, PF increases but PF increase in basic solutions
is more signicant with comparison to this increase value in
acidic solutions. The results show that the minimum values
of PF are at a pH value of about 7. It can be said that the net
electrostatic forces between solutes and membrane surface
are attractive (Salahi et al., 2010b).
ANN permeation ux predictions concerning to the effect
of operating parameters on PF is shown in Fig. 10. Two other
parameters, in all gures, are set at CFV = 0.25 m/s and pH = 4,
TMP = 4.5 bar and pH = 4, TMP = 4.5 bar and CFV = 0.25 m/s,
T = 37.5 C and pH = 4, T = 37.5 C and CFV = 0.25 m/s and
T = 37.5 C and TMP = 4.5 bar for Fig. 10af, respectively.
Fig. 11af demonstrate variation of FR under steady state
condition versus T-TMP at CFV = 0.75 m/s and pH = 7, TCFV at TMP = 1.5 bar and pH = 7, T-pH at TMP = 1.5 bar and

CFV = 0.75 m/s, TMP-CFV at T = 25 C and pH = 7, TMP-pH at


T = 25 C and CFV = 0.75 m/s and CFV-pH at T = 25 C and
TMP = 1.5 bar, respectively.
Regarding Fig. 11ac, it is obviously shown, increasing temperature at the range of 25 C T 50 C decreases FR and this
is due to increasing the oil solubility (Salahi et al., 2011b).
According to Fig. 11c, b and f, FR decreases as the CFV increases
at the range of 0.25 m/s CFV 1.25 m/s because at low CFV
values there was a little turbulency so the cake/gel layer could
be formed easily (Salahi et al., 2011b). As observed in Fig. 10c,
e and f, increasing pH at the range of 4 pH 10 decreases
fouling resistance. The oil droplets such as emulsions had the
higher negative charge at higher pH so the cake layer became
more open at high pH due to the inter-droplet repulsion
(Hua et al., 2007), and this phenomenon, i.e. the inter-droplet
repulsion, prohibited the particle from depositing, and led to
the decrease of the thickness of cake layer (Elzo et al., 1998).
Finally as observed in Fig. 11a, d and e, at lower pressure values of about 3 bar, FR increases slightly with pressure. This
can also be due to low tendency to cake/gel layer formation at

896

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Table 8 Non-dominated solutions (the Pareto optimal set), and the corresponding objective function values generated
by GA.
Decision variables
T ( C)
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56
57
58
59
60
61
62
63
64
65

49.97
49.93
49.92
49.87
49.93
49.94
49.94
49.98
49.94
49.95
49.96
49.98
49.98
49.93
49.95
49.94
49.95
49.95
49.95
49.94
49.98
49.94
49.95
49.97
49.93
49.93
49.93
49.94
49.91
49.95
49.93
49.92
49.94
49.96
49.95
49.93
49.93
49.93
49.93
49.95
49.95
49.93
49.93
49.92
49.93
49.94
49.96
49.95
49.97
49.95
49.95
49.95
49.94
49.94
49.94
49.94
49.94
49.95
49.93
49.94
49.96
49.94
49.92
49.93
49.95

TMP (bar)
3.55
4.22
2.51
4.24
3.26
4.15
4.19
3.33
4.18
4.17
3.45
3.46
3.47
4.15
4.18
4.15
4.12
3.62
3.61
3.43
3.41
4.16
3.50
3.55
2.36
3.25
3.54
4.16
4.24
4.18
4.15
4.19
3.22
3.34
3.58
3.31
3.17
3.44
4.23
3.57
4.18
4.21
2.96
4.22
3.30
4.16
3.63
4.18
3.60
3.49
3.19
3.53
3.61
2.79
3.23
3.28
3.36
4.12
3.13
3.59
3.56
4.13
2.06
3.62
4.12

Objective functions

CFV (m/s)

pH

1.24
1.23
1.25
1.23
1.23
1.22
1.23
1.25
1.21
1.21
1.24
1.25
1.24
1.19
1.18
1.20
1.17
1.23
1.24
1.24
1.24
1.23
1.24
1.24
1.23
1.24
1.25
1.23
1.23
1.18
1.19
1.23
1.24
1.24
1.24
1.23
1.25
1.25
1.23
1.25
1.20
1.22
1.23
1.21
1.24
1.21
1.24
1.19
1.24
1.24
1.24
1.24
1.24
1.21
1.24
1.24
1.24
1.18
1.23
1.24
1.25
1.19
1.25
1.25
1.17

9.99
10.00
9.99
10.00
10.00
10.00
10.00
9.99
10.00
10.00
9.99
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
9.99
10.00
10.00
9.99
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
9.99
10.00
10.00
10.00
10.00
9.99
10.00
10.00
10.00
10.00
10.00
10.00
9.99
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
10.00
9.99
10.00
10.00
10.00
9.99
10.00
10.00
10.00
10.00

PF (L/m2 h)
215.46
215.81
208.59
215.71
214.36
216.04
215.88
214.69
216.01
216.04
215.15
215.18
215.21
216.15
216.17
216.11
216.21
215.62
215.59
215.05
214.99
215.94
215.30
215.44
206.78
214.32
215.40
215.96
215.77
216.17
216.16
215.89
214.19
214.73
215.52
214.58
213.94
215.09
215.78
215.50
216.11
215.92
212.65
215.98
214.54
216.08
215.65
216.13
215.58
215.28
214.04
215.38
215.60
211.30
214.24
214.48
214.81
216.20
213.69
215.55
215.48
216.18
202.84
215.62
216.20

FR (1/m)
68.22
76.40
43.98
74.84
51.44
82.12
77.78
53.97
81.24
82.17
61.09
61.40
62.20
86.56
87.44
84.51
90.29
73.48
72.04
59.70
58.15
79.44
64.51
67.67
43.92
50.90
66.84
80.12
75.56
87.36
86.57
78.19
50.07
54.53
70.11
53.33
48.60
60.18
75.66
69.40
84.26
78.72
45.52
80.36
52.69
83.43
74.21
85.34
71.68
63.99
49.09
66.28
72.66
44.67
50.42
52.21
55.83
89.47
47.85
70.93
68.67
88.16
43.76
72.98
90.17

897

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

Table 8 (Continued)
Decision variables
T
66
67
68
69
70

( C)

TMP (bar)

49.94
49.94
49.96
49.91
49.94

4.17
2.18
2.72
4.20
2.92

Objective functions

CFV (m/s)

pH

1.21
1.25
1.25
1.23
1.24

10.00
10.00
10.00
10.00
9.99

lower pressure up to 3 bar, and as a result, the FR growth rate is


low, however, after that at higher pressure, FR increases more
signicantly with pressure because the cake/gel layer on the
membrane surface becomes denser (Abbasi et al., 2010b).
The validity of the models has also been checked by
Figs. 12 and 13, where a comparison is conducted between the
predicted and measured PF and FR. A satisfactory agreement
can be noted between the experimental and the networks
responses. These results indicate the high capability of the
ANN in predicting the PF and FR of a given operating parameters.
Fig. 12ad provide a visual representation of the actual PF
and network prediction data points versus temperature, TMP,
CFV and pH, respectively, as the gures are indicated, the predicted and actual PF cover each other very well and have the
same behavior by increasing of temperature, TMP, CFV and
pH. Fig. 12ad shows the actual PF that were measured in the
experimental investigation and networks prediction in y-axis
and temperature, TMP, CFV and pH in x-axis, respectively.
Fig. 13ad shows the actual FR and its networks prediction
versus temperature, TMP, CFV and pH, respectively. Clearly,
experimental and predicted FR values have same behavior

PF

(L/m2

h)

FR (1/m)

216.07
204.51
210.66
215.84
212.34

83.16
43.79
44.28
77.44
45.13

with operating parameters (i.e. temperature, TMP, CFV and pH)


increasment. By comparing the ANN values and actual values
in Fig. 13, it can be seen that ANN model gives very reliable
estimates of FR of the UF process.
If all independent variables that obtained from the
NN model are xed, except temperature, it can be seen
from Fig. 12a that increasing temperature increases PF at
25 C T 50 C. For depiction of this gure TMP, CFV and
pH are xed at 3 bar, 0.75 m/s and 7, respectively. In other
words, Fig. 12a illustrates variation of PF under steady state
condition versus temperature (@ TMP = 3 bar, CFV = 0.75 m/s
and pH = 7). According to Fig. 12b and c, the experimental
results, as well as the model predictions, both indicate increasing TMP and CFV increase PF values at 1.5 bar TMP 4.5 bar
and 0.25 m/s CFV 1.25 m/s, respectively. But increasing pH
has a dual effect on permeation ux at 4 pH 10. According to Fig. 12d, increasing pH decrease permeation ux up
to a minimum value then increase it. Briey, Fig. 12bd
demonstrate variation of PF under steady state condition
versus TMP, CFV and pH, respectively, at medium levels of
other factors, i.e. T = 37.5 C, TMP = 3 bar, CFV = 0.75 m/s and
pH = 7.
160

180

Exp

Exp
ANN

ANN

PF(L/m2.h)

PF(L/m2.h)

160
140
120
100
0

20

T(C)

40

60

150

140

130
0

TMP(bar)

(a)

(b )
200

180

Exp
ANN

Exp
ANN

180

PF(L/m2.h)

PF(L/m2.h)

160
140

160

120
140

100
0

0.5

CFV(m/s)

(c )

1.5

10

15

pH

(d )

Fig. 12 Comparing ANN and experimental data, effect of (a) temperature, (b) trans-membrane pressure, (c) cross ow
velocity and (d) pH on permeation ux at medium levels of other factors, i.e. T = 37.5 C, TMP = 3 bar, CFV = 0.75 m/s and
pH = 7.

898

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

140

100

Exp

Exp

ANN

ANN

120
FR(1/m)

FR(1/m)

90

80

70

100

80

60

60
0

20

40

60

T(C)

(a)

10

15

(b )
Exp

Exp

ANN

ANN

120

100
FR(1/m)

FR(1/m)

120

140

100
80
60

4
TMP(bar)

80

60

40
0

0.5
CFV(m/s)

1.5

5
pH

(c )

(d )

Fig. 13 Comparing ANN and experimental data, effect of (a) temperature, (b) trans-membrane pressure, (c) cross-ow
velocity and (d) pH on fouling resistance at medium levels of other factors, i.e. T = 37.5 C, TMP = 3 bar, CFV = 0.75 m/s and
pH = 7.
According to Fig. 13, the experimental results, as well
as the model predictions, both indicate increasing temperature, CFV and pH decrease FR values at the ranges
of: 25 C T 50 C, 0.25 m/s CFV 1.25 m/s and 4 pH 10,
respectively. But increasing TMP increase FR at the range of:
1.5 bar TMP 4.5 bar. In summary Fig. 13ad demonstrate
variation of FR under steady state condition versus T, TMP,
CFV and pH, respectively at medium levels of other factors,
i.e. T = 37.5 C, TMP = 3 bar, CFV = 0.75 m/s and pH = 7.
Succeeding to developing of the models, an effort was made
to optimize operating parameters (i.e. temperature, TMP, CFV
and pH) for a desired permeation ux (i.e. maximum) and fouling resistance (i.e. minimum) as a two-objective problem. To
achieve this, genetic algorithm was used together with the validated neural models as the principal tools. It took two neural
models developed for predicting PF and FR. The optimization
problem studied is represented mathematically by:

The multi-objective solution yielded a set of optimal solutions in which an improvement in one objective requires a
degradation of another. The plot of this two objective problem is shown in Fig. 14. This curve is known as the Pareto
front and shows a clear trade-off between the FR and PF; an
improvement (a decrease) in the FR results in a degradation (a
decrease) in the PF or an improvement (an increase) in the PF
results in a degradation (an increase) in the FR.
Table 8 present the set of non-dominated solutions (the
Pareto optimal set), and the corresponding objective function
values in the objective space (called the Pareto front).
As can be seen in Table 7, the optimum decision values, so that a maximum permeation ux accompanied
by a minimum fouling resistance, were acquired and the
computed results for this purpose (i.e. maximize permeation ux and minimize fouling resistance simultaneously)
show higher temperature (all predicted T are greater than
100

(13)

min f2 (T, TMP, CFV, pH) = FR (which is obtained by neural network)

(14)


25 C T 50 C

bound constraints

1.5 bar TMP 4.5 bar

0.25 m/s CFV 1.25 m/s

4 pH 10

Fouling resistance (minimize)

max f1 (T, TMP, CFV, pH) = PF (which is obtained by neural network)

80

60

40

20
200

(15)

204

208

212

216

Permeaon ux (maximize)

Fig. 14 Pareto optimal front for permeation ux


maximization and fouling resistance minimization.

220

899

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

49.90 C, in comparison with experimental temperature range


25 C T 50 C) and it is consistent with neural network predictions, higher pH (all predicted pH are greater than 9.99,
in comparison with experimental pH range 4 pH 10). This
result agrees with the predictions obtained by networks,
approximate higher CFV (all predicted CFV are greater than
or equal 1.17 m/s, in comparison with experimental crossow velocity range 0.25 m/s CFV 1.25 m/s) it is worthy note
according to PF network and FR network, increasing CFV
increases PF and decreases FR considerably up to 0.751 m/s
but after that these behaviors continue with less steep and
the phenomena prove optimization values. Variable TMP values (2.06 predicted TMP (bar) 4.24, in comparison with
experimental TMP range 1.5 bar TMP 4.5 bar) cause highest steady PF and the lowest FR. A closer look at Figs. 12b and
13b reveals that in about medium levels of TMP values, both
high permeation ux and low minimum fouling resistance
is possible and this agrees with the results of optimization
section.
ANN is a strong tool in interpolation without adequate
accuracy for extrapolation. According to this, determination
of lower and upper limits of variables is required for optimization. The acceptable limit is established based on ANN training
and it can be seen that the estimated PF values, that were
achieved by GA, corresponding to optimum operating parameters are almost greater than those observed in experiments
and also it can be observed that some estimated FR values,
that were achieved by GA, corresponding to optimum operating parameters are almost near to the minimum quantities
those observed in experiments. We know that, this optimization problem involve two objectives. One of which must be
maximized (permeation ux).while the other minimized (fouling resistance), simultaneously. Often, a set of equally good
(non-dominated or Pareto optimal) solutions exist and our
results are completely consistent with this.

wastewater process by applying GA was obtained. In other


word, the optimum operating conditions to achieve simultaneously maximum permeation ux at steady state and
minimum fouling resistance, when the oily wastewater was
ultraltered, could be found by GA and constructed ANNs.
Results of the optimum section showed higher temperature
(all predicted T are greater than 49.90 C, in comparison with
experimental temperature range 25 T ( C) 50), higher pH
(all predicted pH are greater than 9.99, in comparison with
experimental pH range 4 pH 10), approximate higher CFV
(all predicted CFV are greater than or equal 1.17 m/s, in comparison with experimental CFV range 0.25 CFV (m/s) 1.25)
and variable TMP (2.06 predicted TMP (bar) 4.24, in comparison with experimental TMP range 1.5 TMP (bar) 4.5)
caused highest steady PF and the lowest FR. Finally it is
observed that the Pareto optimal front for this two-objective
(i.e. PF and FR) was convex.

Acknowledgments
This research was supported by East Tehran Branch, Islamic
Azad University, Tehran, Iran. Also, the authors would like to
appreciate Mr. S.R. Asadullahpour for his help and invaluable
guidance in optimization methodology.

Appendix A.




Standard Deviation of Predictions =


MPE =

1-ANNs were utilized to predict PF and FR corresponding to a given same operating conditions (i.e. temperature, TMP, CFV and pH). Feed-forward architecture with
LevenbergMarquardt back-propagation training algorithm
was employed to develop the models. It was found that both
networks with one hidden layer of 8 neurons in their hidden layers (4:8:1), are appropriate for prediction purposes.
The coefcient of determination of both networks (above 0.99
for whole data set) together with the important statistical
parameters indicated that the neural networks have been well
trained. ANNs successfully tracked the non-linear behavior of
PF and FR versus temperature, TMP, CFV and pH during UF
of oily wastewater. For all of the cases considered, the ANNs
proved to be an adequate interpolation tool, where an excellent prediction was obtained for all operation conditions not
represented in the training data set (i.e. testing data set).
ANN modeling method has many advantages such as
rapidity, robustness, fault tolerance, adaptability, generalization and simplicity which make it an interesting choice for
modeling of complex systems, such as wastewater treatment
processes.
2-Pareto optimal front for permeation ux (maximize) and
fouling resistance (minimize) as a two-objective optimization problem and corresponding decision variable vectors
(Pareto-optimal solutions), i.e. T, TMP, CFV and pH in UF oily

N1

N

i=1

(A.1)

(A.2)


(A.4)

i=1

(ti pi )

N

N
(t
i=1 i

RMSE =

(A.3)

100   ti pi 
 t 
N
i
N

MSE =

pm )

ti

i=1

Conclusion

tm )

N1

N
(p
i=1 i

t p 
i
i

100 
N
N

MAPE =

6.

N
(t
i=1 i

Standard Deviation of Observations =

pi )

(A.5)
2

(A.6)

N
1 1
2
(ti pi )
2 N
N

NMSE =

(A.7)

i=1


1  
ti pi 
N
N

MAE =

i=1

R2 (coefcient of determination) = 1

N
tm =

t
i=1 i

(A.8)

N
2
(ti pi )
Ni=1
2
i=1

(ti tm )

(A.9)

(A.10)

ti is the ith experimental value, tm is the average of experimental values,


pi is the ith predicted value, pm is the average of predicted values, N is
the number of data,  2 is the variance of experimental data.

Symbols
A
B
CFV
fm (x)
gk (x) = 0
h
hj (x) 0

membrane area (m2 )


bias
cross-ow velocity (m/s)
the mth objective function
the kth equality constraint s
hour
the jth inequality constraint

900

chemical engineering research and design 9 1 ( 2 0 1 3 ) 883903

J
Jwi
Jww
L
N
n
pi
pm
pH
Rf
r
S
Sk
T
TMP
TOC
TSS
ti
tm
V
W
X
(ub)
xi

ltration ux (L/m2 h)
initial water ux (L/m2 h)
water ux after fouling (L/m2 h)
liter
the number of data
number of input signals
the ith predicted value
the average of predicted values
()
Fouling resistance (1/m)
number of neurons
second
the net input to the neuron k
temperature ( C)
trans-membrane pressure (bar)
total organic carbon (mg/L)
total suspended solids (mg/L)
the ith experimental value
the average of experimental values
ltrate volume (L)
weight
input signal
upper bound of ith decision variable

xi
Y
P
m2
C

2

lower bound of ith decision variable


network response from output layer neuron
pressure gradient (Pa)
square meter
centigrade degree
dynamic viscosity (Pa s)
variance of experimental data
activation function

(lb)

Abbreviations
articial neural network
ANN
American Petroleum Institute
API
cross-ow membrane ltration
CMF
CFV
cross-ow velocity
N,N-dimethylacetamide
DMAc
EA
Evolutionary Algorithm
electrodialysis
ED
EMO
evolutionary multi-objective optimization
FC
fuel cells
Feed-Forward Backpropagation
FFBP
FR
fouling resistance
membrane ltration
FT
genetic algorithm
GA
GP
genetic programming
gas separation
GS
2-propanol
IPA
lb
lower bound
mean absolute error
MAE
mean absolute percentage error
MAPE
MAPD mean absolute percentage deviation
MBR
membrane bioreactors
MF
microltration
ML
machine learning
multi-layer perceptron
MLP
MOGA multi-objective genetic algorithm
MOP
multi-objective optimization problem
MPE
mean percentage error
MSE
mean squared error
nanoltration
NF
NMSE
normalized mean squared error

NN
neural network
non-dominated sorting genetic algorithm
NSGA
NSGA-II Elitist (fast) non-dominated sorting genetic algorithm
NTU
nephelometric turbidity units
PAN
polyacrylonitrile
polyethersulfone
PES
PF
permeation Flux
polysulfone
PS
PVDF
polyvinylidene uoride
polyvinylpyrrolidone
PVP
coefcient of determination
R2
R
correlation coefcient
rank-density based genetic algorithm
RDGA
root mean square deviation
RMSD
root mean square error
RMSE
reverse osmosis
RO
RWGA random weighted genetic algorithm
strength pareto evolutionary algorithm
SPEA
TMP
trans-membrane pressure
total organic carbon
TOC
TRAINLM LevenbergMarquardt training algorithm
total suspended solids
TSS
upper Bound
ub
UF
ultraltration

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