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2009 Modeling of A Permeate Flux of Cross-Flow Membrane Filtration of
2009 Modeling of A Permeate Flux of Cross-Flow Membrane Filtration of
ABSTRACT: Although traditional artificial neural networks have been an attractive topic in modeling membrane
filtration, lower efficiency by trial-and-error constructing and random initializing methods often accompanies neural
networks. To improve traditional neural networks, the present research used the wavelet network, a special feedforward
neural network with a single hidden layer supported by the wavelet theory. Prediction performance and efficiency of the
proposed network were examined with a published experimental dataset of cross-flow membrane filtration. The dataset
was divided into two parts: 62 samples for training data and 329 samples for testing data. Various combinations of
transmembrane pressure, filtration time, ionic strength and zeta potential were used as inputs of the wavelet network
so as to predict the permeate flux. Through the orthogonal least square alogorithm, an initial network with 12 hidden
neurons was obtained which offered a normalized square root of mean square of 0.103 for the training data. The initial
network led to a wavelet network model after training procedures with fast convergence within 30 epochs. Futher the
wavelet network model accurately depicted the positive effects of either transmembrane pressure or zeta potential on
permeate flux. The wavelet network also offered accurate predictions for the testing data, 96.4 % of which deviated the
measured data within the ± 10 % relative error range. Moreover, comparisons indicated the wavelet network model
produced better predictability than the back-forward backpropagation neural network and the multiple regression
models. Thus the wavelet network approach could be employed successfully in modeling dynamic permeate flux in
cross-flow membrane filtration.
Keywords: Artificial neural network; Colloidal fouling; Prediction; Ultrafiltration separation; Wavelet
INTRODUCTION
Applications of membrane technology in water and less competitive in many applications. Therefore,
wastewater treatment have been growing steadily in understanding membrane fouling and developing
recent years (Brindle and Stephenson, 1996; Liao et controlling methods are crucial for the future of
al., 2006; Visvanathan et al., 2000). Many full-scale membrane technologies.
facilities are running with immersed microfiltration or To optimize the operation of membrane filtration,
ultrafiltration membranes mainly because membranes many modeling methods have been used to predict the
can offer higher efficiency for liquid-solid separation permeate flux decline in recent years. Among these
(Visvanathan et al., 2000). However, the effectiveness methods, theoretical models have been established
of membrane separation is greatly affected by fouling- using numerous factors, which include feedwater
the decline in permeate flux due to accumulation of characteristics (such as types of foulants, pH and ionic
colloidal matter, organic molecules, sparingly soluble compositions), membrane properties (such as surface
inorganic compounds and microorganisms on roughness, charge properties and hydrophobicity) and
membrane surfaces or in membrane pores (Defrance et operational conditions (such as transmembrane
al., 2000; Song, 1998; Zhang and Song, 2000). Fouling pressure, cross-flow velocity and temperature) (Li and
is an unavoidable deleterious phenomenon in Elimelech, 2004; Song, 1998). Theoretical models can
membrane filtration and makes membrane technology produce highly detailed and complex descriptions of
*Corresponding Author Email: zgming@hnu.cn membrane fouling; however, they are computationally
Tel.: +86731 882 2754; Fax: +86731 882 3701 intensive and demand a high-level modeling expertise
A. L. Wei et al.
(Bowen et al., 1998). Moreover, the mechanisms of that RBFNs achieved better predictions than BPNNs.
membrane fouling and the effect of key factors on However, Sahoo and Ray (2006) pointed out that the
fouling are still not clear or quite controversial (Tarleton results of Chen and Kim (2006) were obtained through
and Wakeman, 1993; Zhang and Song, 2000), which the ANNs with unoptimized structures. With the same
makes theoretical models designed with some experimental data of Fabish et al. (1998), they showed
necessary assumptions. Such assumptions result in that there was no apparent difference in predictability
models which are only valid for certain types of between BPNNs and RBFNs when the structures of
feedwater under certain conditions. In order to control the both type of networks were optimized by genetic
membrane filtration effectively and easily, alternative algorithms (GAs). Although the GA optimized networks
methods are desired. Because avaiable information may improve the predictability of ANNs, Cheng et al.
often consists of measured data of several factors and (2008) stated that the GAs are inclined to encounter
permeate flux, the alternatives are expected to depend the pitfall of over fitting when the number of neurons
not on deep insight into complicated mechanisms, but is too large because of their intrinsic randomness.
on full utilization of available information. Furthermore, Cheng et al. (2008) presented a modified RBFN
such an alternative must have the ability to determine (MRBFN) which showed good convergence resulting
the connections between input and output only by from a well initialized structure. They constructed the
analyzing process data. Fortunately, data driven MRBFN by choosing neurons from a set candidate
models, such as artificial neural networks (ANNs), neurons which were prior determined according uniform
could act as these alternatives. ANNs are mathematical partitions of the domain of interest at different levels.
algorithms that simulate the capacityof the biological However, their method could encounter the problem of
brain to solve complex problems, and have the ability dimension curse when the input dimension increases,
to approximate almost any function in a stable and because the increasing dimension leads to an
efficient way (Chattopadhyay and Bandyopadhyay, exponential increase of the uniform partitions of the
2007). ANNs have already been extensively applied to domain. In particular, the dimension curse becomes
modeling membrane filtration (Chen and Kim, 2006; more severe when higher levels are carried out in the
Cheng et al., 2008). case of higher input dimension; and above all, this
In all types of ANNs, feedforward backpropagation dimension curse makes the choosing neurons of the
neural networks (BPNNs) and radial basis function MRBFN with higher cost of computation. Despite the
networks (RBFNs) have been proven to be the two vast efforts to improve the efficiency of ANNs in
most attractive methods for modeling membrane membrane processes as above, there are still some
filtration until now (Al-Abri and Hilal, 2008; Aydiner et problems, for instance, lack of specific methods or the
al., 2005; Chen and Kim, 2006; Sahoo and Ray, 2006). danger of encountering lower efficiency to determine
Dornier et al. (1995) first used BPNNs to predict the the initial network structures and the initial parameters.
dynamic process of membrane fouling during cross- Therefore, a more efficient type of ANNs will be
flow microfiltration of crane sugar. They studied the preferred to model the complex process of membrane
effect of the BPNN hidden structure and different filtration.
distributions of training data on the predictability, and Wavelet networks have shown to be a promising
they obtained satisfactory accuracy. In following alternative to traditional ANNs (Zhang and Benveniste,
studies, BPNNs have been shown to be sometimes 1992) and many studies describe wavelet networks as
better suited and more useful for high nonlinear a powerful tool for function approximation (Zhang and
processes of membrane filtration (Chellam, 2005; Cinar Benveniste, 1992; Zhang et al., 2001), system
et al., 2006; Curcio et al., 2006; Ni Mhurchu and Foley, identification (Billings and Wei, 2005; Sjoberg et al.,
2006). Unfortunately, there are lack of reliable rules for 1994), automatic control (Sanner and Slotine, 1998;
the choice of the hidden structure of BPNNs and the Oussar et al., 1998), etc. Such network is a special 3-
common way is by trial and error. Moreover, initial layer feedforward network as shown in Fig. 1 which is
parameters of BPNNs are often assigned random values calculated as follow:
which cause a slow convergence during training s
process. On the other hand, using the experimental
data of Fabish et al. (1998), Chen and Kim (2006) found
yˆ x ¦Z\
i 1
i i x (1)
396
Int. J. Environ. Sci. Tech.,
A. L. Wei 6et(3),
al. 395-406, Summer 2009
397
Modeling of a permeate flux
A. L. Wei et by
al. wavelet network
flow membrane ultrafiltration at five different is a popular method for choosing the smoothing
combinations of pH and ionic strength (I). For each parameter. An important early reference is Craven and
combination of pH and I, the permeate flux was Wahba (1979). The GCV criterion consists in estimating
measured under five different transmembrane pressures the expected performance of the model evaluated with
(ǻP) as shown in Fig. 4. In this paper, I, ȗ, ǻP and time fresh data based on the required data (Zhang, 1997).
(t) acted as the input of wavelet networks to predict Thus an initial form of the wavelet network model was
the dynamic permeate flux. Out of 391 data samples, 62 achieved. In the end, the initial wavelet network was
samples were chosen as training data such that more trained to get the final wavelet network model. The
samples were located in regions of greatest curvature, detailed steps are listed as follows:
as shown in Fig. 4. The other 329 samples were used as 1) Definition of wavelet support: For ȥm,n(x) in the family
testing data. (2), denote by Sm,n its support, i.e.,
Prior to be inputed the wavelet network, the values
of all experimental data were normalized between -1 and
1 as below: S m ,n ^x R d
:\ m ,n x ! 0 .662 max \
x
m ,n x ` (5)
X X cent
X norm (3) 2) Generating the family of candidate wavelets: With
X half
the definition of Sm,n, each training point xk among N
X max X min
training points is examined within five dilation levels
Where, X cent is the center of variable (n=0, 1, 2, 3, 4) to find the wavelets whose supports
2
contain xk. Then the index set of the found wavelet, Ik,
interval, X half X max X min is defined by:
is the half of interval length,
2
Xmax is the maximum value of a variable and Xmin is the Ik ^ m, n : xk S m , n ` (6)
minimum value of a variable. On the other hand, a
corresponding denormalization was done to achieve a The union of Ik for all xk in the family (2) gives the
reasonable permeate flux after an output of the network indices of candidate wavelets whose supports contain
was attained. The normalization method was derived at least one training data point. This results in the family
from Z-score normalization (Priddy and Keller, 2005). of candidate wavelets
Such normalization can minimize bias within the wavelet
network for one feature over another. It can also speed
up training time by starting the training process for W ^\ m,n : m , n I1 I 2 I N ` (7)
each feature within the same scale.
Let L be the number of wavelets in W. For
Constructing and training the wavelet network convenience of the following presentation, the double
According to Eq. 1, a so-called Mexican hat wavelet index (m, n) is replaced by a single index j=1, 2, …, L,
(Zhang, 1997) was chosen as a mother wavelet with the i.e.,
following form:
2
W ^\ 1 ,\ 2 , ,\ L ` (8)
x
2 (4)
\ x d x e 2 3) Determination of the initial wavelet network: The
initial wavelet network is achieved by a hybrid
Where, d is the dimension of x, ||x||2=xxT. Then a family algorithm (Zhang, 1992; Zhang, 1997) where, the OLS
of candidate wavelets was determined by the mother algorithm determines the relative optimal combination
wavelet and the training data. Then, further of certain number of candidate wavelets and then the
development was done by selecting different number GCV criterion points out the most reasonable
of wavelons from the candidate family according to the combination of certain number of candidate wavelets.
OLS algorithm and then, the number of wavelon was The hybrid algorithm can be done as follows:
determined by the generalized cross-validation (GCV) Algorithm: I={1, 2, …, L};
criterion. The GCV, a modified form of cross-validation, pj = ȥj for all jI;
398
Int. J. Environ. Sci. Tech., 6 (3),et 395-406,
A. L. Wei al. Summer 2009
399
A. L. Wei et al.
0.0002
0.00015
GCV
0.0001
0.00005
0
0 20 40 60 80 100 120 140 160
0.12
0.09
NSRMSE
0.06
0.03
0
0 30 60 90 120 150
Epochs
Fig. 3: NSRMSE with repect to epochs for training the wavelet network
successfully made a trade-off between the optimality strategy and the GCV criterion could lead to an
and the efficiency. The obtained initial network fitted efficient constructing procedure and a better
the training data with an NSRMSE of 0.103. Such initialization for the wavelet network.
smaller NSRMSE agrees with Zhang (1992) who With the initial wavelet network, the common back-
r epor t ed t h a t t h e OLS str a t egy coul d offer propagation was used as the traning method. During
satisfactory accuracy. Consequently, the OLS the traning procedure, NSRMSE drastically dropped
400
A. L.6 Wei
Int. J. Environ. Sci. Tech., (3), et al.
395-406, Summer 2009
0.07 0.1
(a) pH=4, I=0.072M, ȗ=-6.3 mV (b) pH=4, I =0.030M, ȗ=-17.9 mV
0.06
0.08
0.05
0.06
0.04
J/(cm/min)
J/(cm/min)
0.03
0.04
0.02
0.02
0.01
0 0
0 10 20 30 40 0 10 20 30 40
Time (min) Time (min)
0.14 0.1
(c) pH=4, I=0.0077M, ȗ=-24.0 mV (d) pH=7, I=0.031M, ȗ=-46.7 mV
0.12
0.08
0.1
J/(cm/min)
J/(cm/min)
0.06
0.08
0.06
0.04
0.04
0.02
0.02
0 0
0 10 20 30 40 0 10 20 30 40
Time (min) Time (min)
0.14
(e) pH=9, I=0.030M, ȗ=-80.5 mV
0.12
0.1
0.08
J/(cm/min)
0.06
0.04
0.02
0
0 10 20 30 40
Time (min)
300 kP a 300 kP a 200 kP a 200 kP a 100 kP a
100 kP a 60 kP a 60 kP a 40 kP a 40 kP a
Fig. 4: Effects of physic-chemical and hydrodynamic parameters on permeate flux, measured (open symbols) and predicted (solid
symbols) values
401
Modeling of a permeate
A. L. Weiflux by wavelet network
et al.
during the first 30 epochs (shown in Fig. 3). Clearly, decreasing I with the same pH and, in the latter, the
the training process converged so fast even in an enhancement in permeate flux was preceded by an
ordinary back-propagation training method. The fast increasing pH with the same I. In fact, both of the
convergence verified again the better initialization above operations led to an increasing ȗ (not
of the wavelet network approach. considering the sign) of colloids (Bowen et al., 1996).
The enhancements in permeate flux by ȗ in Fig. 4 a to
Effect of I, ȗ and ǻP on permeate flux c and Fig. 4 b, d and e, are in qualitative agreement
Fi g. 4 sh ows t h e mea sur em en t s a n d t h e with the published reports by Huisman et al. (1997)
predictions of the wavelet network model for and McDonogh et al. (1989). These authors
permeate flux during cross-flow ultrafiltration of silica explained the effect of ȗ qualitatively by reasoning
coloi ds a t five pressur es for ea ch of fi ve that high zeta potentials increase interparticle
combinations of pH and I. The wavelet network repulsion, thus causing less deposition (thinner cake
model excellently offered predictions (solid symbols) l a yer s) an d m or e per m ea ble ca ke l a yer s.
for both training (cross symbols) and testing (hollow Consequently, the thinner and more permeable cake
symbols) data. Moreover, the nonlinearity of the flux- layers lead to an enhancement of permeate flux. Such
time profiles was well reproduced by the wavelet an enhancement became more significant in this
network. As shown in Fig. 4, the predictions, as well paper because of the colloidal particles with a smaller
as the measurements accurately described permeate mean diameter 65 nm. Faibish et al. (1998) have
flux behavior greatly changing with the variations reported that for particles with diameters smaller than
of ǻP, pH, and I. For each combination of pH and I, about 100 nm, the effect of interaction repulsion on
the permeate flux was proportional to ǻP and the permeate flux becomes dominant. Among all the
ultimate flux at higher transmembrane pressure was predictions and experiments, the combination of
higher. These phenomena are due to the greater pH=9, I=0.030M and ȗ=-80.5mV in Fig. 4 e led to the
driving force for permeate flux by higher ǻP (Faibish highest permeate flux for each ǻP in earlier stage.
et al., 1998). Meanwhile, higher ǻP led to the steeper Besides, the effect of the highest ȗ, lower I also
flux decline at the earlier stage of the filtration. This enhanced the permeate flux for the case in Fig. 4 e,
trend is attributed to the higher convective mass of which is in accordance with the report by Elzo et al.
colloids toward the membrane surface and a more (1998) who stated that lower I corresponds to larger
densely packed cake layer at higher pressure (Faibish distances between particles and such distance
et al., 1998). On the other hand, for each combination results i n mor e per meable ca ke la yers. T he
of pH and I, the lowest ǻP was observed with the predictions in Fig. 4 e agree well with the theoretical
least flux decline for both experimental data and explanation.
predictions. This observation is an index of operation
approaching the critical flux below which colloids Performance comparison
do not deposit on the membrane surface (Faibish et This section describes the superiority of the
al., 1998). wavelet network over BPNN under the same
The predictions also accurately described the modeling conditions. The BPNN model used the tanh
positive effect of ȗ on permeate flux as shown in the function as hidden neurons. Moreover, a comparison
triple of Fig. 4 a to c and, the triple of Fig. 4 b, d and with the conventional MR method was used to show
e. In the former triple, an increasing flux followed a the better initialization of the wavelet network. Two
402
Int. J. Environ. Sci. Tech.,
A. L. 6Wei
(3),et395-406,
al. Summer 2009
0.14 0.14
0.12 0.12
0.1
0.08 0.08
0.06 0.06
0.04 0.04
Ntrain=62 Ntrain=62
Ntest=329 Ntest=329
0.02 R 2=0.774 0.02 R 2=0.975
NSRMSE=0.505 NSRMSE=0.161
0 0
-0.01 0.04 0.09 0.14 -0.01 0.04 0.09 0.14
0.14 0.14
0.12 0.12
0.1 0.1
Predicted flux (cm/min)
Predicted flux (cm/min)
0.08 0.08
0.06 0.06
0.04 0.04
Ntrain=62 Ntrain=62
Ntest=329 Ntest=329
0.02 R 2=0.940 0.02 R 2=0.780
NSRMSE=0.2445 NSRMSE=0.485
0 0
-0.01 0.04 0.09 0.14 -0.01 0.04 0.09 0.14
0.14
0.12
Predicted flux (cm/min)
0.1
0.08
0.06
Ntrain=62
0.04
Ntest=329
R 2=0.826
0.02
NSRMSE=0.474
0
-0.01 0.04 0.09 0.14
403
A. L. Wei et al.
MR models were built with the identical training data. the lines with ±10 % relative error. Only 12 out of
One is a linear regression equation with the following 329 predicted testing data lie outside the region
form: enclosed by the dotted lines, indicating that 96.4
% of the data are within the ± 10 % relative error
J = 2.488×10-2 – 2.401×10-1{I} – 2.230×10-4{ȗ} + range. In Fig. 5 c, 81 out of 329 predicted testing
1.376×10-4{ǻP} – 8.353×10-4{t}. data is not confined within the two dotted lines. In
Fig. 5 d, only 40 % of the data lie within the ±10 %
Another is a nonlinear multiple equation with the relative error range, which is mainly because the
following form: complex nonlinear membrane filtration process
could not be presented by a simple linear method.
J = 2.956×10-2 – 2.312×10-1{I} – 2.235×10-4{ȗ} + Moreover, the simple linear description led to 9
1.467×10-4{ǻP} – 2.747×10-4{ t} + 6.288×10-5{t2}. negative results. Although the nonlinear MR model
was slightly better than the linear MR model, it
Coefficients of both equations were proven provided 13 negative predictions, which suggest
significant by the t-statistic. Several other multiple that the MR method could not rationally depict the
polynomial regression models were also tested, but membrane filtration.
their coefficients showed worse significance by the
t-test. Table 1 shows the coefficients of multiple CONCLUSION
determination R2 and the NSRMSE for permeate flux The present study shows that a wavelet network
obtained with the initial wavelet network, the wavelet approach could be used to predict permeate flux
network model, the BPNN model, the linear MR model decline of cross-flow ultrafiltration of colloidal
and the nonlinear MR model. The wavelet network suspensions as a function of operating conditions.
model not only provided better results in fitting, but The wavelet network approach provided the benefit
also the best ones in prediction, with a R 2 of 0.997 of efficient constructi ng procedures by fully
for the training data and 0.965 for the testing data. ultilizing the sparseness of training data and the
The BPNN model provided results much better than compact support property of wavelets. In particular,
the MR models. The nonlinear MR model shows in case of multiple input dimensions (4 dimensions
slightly improved in the basis of the linear MR model, in this paper), this approach could avoid the curse
but its prediction ability is not comparable to the of dimensionality for the choice of hidden neurons.
BPNN and wavelet networks. This supposes that Moreover, a better initialization with an NSRMSE of
the existing high non-linearity of membrane filtration 0.103 by the OLS algorithm and GCV selection
is a challenge for the MR method. In particular, it criterion led to fast convergence within 30 epochs
can be stated that the NSRMSE obtained by the during training procedure. The wavelet network
wavelet network model is much smaller than that model excellently described the nonlinear variation
obtain ed with the oth er t hree methods. T he of permeate flux under different operating conditions.
superiority of the wavelet network model in fitting The predictions described the positive effect of ǻP
and prediction resulted from its better initialization, on permeate flux and moreover, an increasing ȗ was
because the initial wavelet network has already followed by an enhancement in permeate flux. Such
provided better results with a R 2 of 0.990 and an an accurate prediction ability of wavelet networks
NSRMSE of 0.103 for the training data. Moreover, could certainly be helpful to optimize practical
the number of wavelons of the initial wavelet operations of membrane filtration. Further, the wavelet
network, which was evaluated by GCV criterion, led network model offered such satisfactory accuracy that
to good generalization performance of the wavelet almost 96.4 % of predictions for the testing data
network model with an NSRMSE of 0.196 for the deviated measured data within the ± 10 % relative
testing data. error range. Meanwhile, the comparisons of the
Fig. 5 a-e shows the predicted versus measured performances of the initial wavelet network, the
flux for the initial wavelet network, the wavelet wavelet network model, the BPNN model, the linear
network model, the BPNN model and the MR MR model and the nonlinear MR model confirmed the
models. Most of data shown in Fig. 5 b fall within superiority of wavelet networks.
404
Int. J. Environ. Sci. Tech.,
A. L.6 Wei
(3), et
395-406,
al. Summer 2009
As it is shown, efficient contruction, better suspension: a radial basis function neural network approach.
Desalination, 192 (1-3), 415-428 (14 pages) .
initialization, faster convergence and higher
Cheng, L. H.; Cheng, Y. F.; Chen, J. H., (2008). Predicting
accuracy, all of these has proved that the wavelet effect of interparticle interactions on permeate flux decline
network is a promising alternative to traditional in CMF of colloidal suspensions: An overlapped type of
ANNs in modeling complex membrane filtration local neu ral network. J. Membr. Sci., 3 08 (1-2), 54-65
processes. As a modeling tool, wavelet networks (12 pages) .
Cinar, O.; Hasar, H.; Kinaci, C., (2006). Modeling of submerged
could be used both observation of membrane system membrane bioreactor treating cheese whey wastewater by
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ACKNOWLEDGEMENTS 125-132 (8 pages) .
This study was financially supported by the Da ubechies, I., (199 2). Ten lectures on wavelets. SIAM,
Natural Foundation for Distinguished Young Philadelphia, 11-17 (7 pages) .
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V., (2000). Contribution of various constituents of activated
National Basic Research Program (program 973, No. sludge to membrane bioreactor fouling. Biores. Tech., 73
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Technology Research Program of China (NO. Dornier, M.; Decloux, M.; Trystram, G.; Lebert, A., (1995).
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Zeng, G. M., Ph.D., Full professor and the head of College, College of Environmental Science and Engineering, Hunan University, Changsha,
P. R. China. Email: zgming@hnu.cn
Huang, G. H., Ph.D., Full professor, Environmental Systems Engineering Program, Faculty of Engineering, University of Regina, Regina,
Sask, Canada. Email: gordon.huang@uregina.ca
Liang, J., Ph.D. research candidate, College of Environmental Science and Engineering, Hunan University, Changsha, P. R. China.
Email: liangjie_ever@yahoo.com.cn
Li, X. D., Ph.D., Lecturer, College of Environmental Science and Engineering, Hunan University, Changsha, P. R. China.
E-mail: lxdfox@163.com
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