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Abstract
The capability of a radial basis function neural network (RBFNN) to predict long-term permeate flux decline in
crossflow membrane filtration was investigated. Operating conditions of transmembrane pressure and filtration
time along with feed water parameters such as particle radius, solution pH, and ionic strength were used as inputs
to predict the permeate flux. Simulation results indicated that a single RBFNN accurately predicted the permeate
flux decline under various experimental conditions of colloidal membrane filtrations and eventually produced
better predictability than those of the regular multi-layer feed-forward backpropagation neural network (BPNN)
and the multiple regression (MR) method. We believe further development of the artificial neural network approach
will enable us to design and analyze full-scale processes from results of laboratory and/or pilot-scale experiments.
Keywords: Artificial neural network; Radial basis function; Backpropagation; Multiple regression; Membrane
filtration; Colloidal fouling
Presented at the International Congress on Membranes and Membrane Processes (ICOM), Seoul, Korea,
21–26 August 2005.
can be generally classified into two categories: forms shortly after the CP layer is generated. Thus,
dead-end and crossflow filtrations. The former one of the main focuses of flux decline models is
(without periodic backwashing) is not of practical on the time-dependent variation of the cake layer
interest because of its rapid flux decline intrin- resistance during filtration while the CP layer’s
sically stemming from unceasing mass accumula- effect is considered to be negligible [8,10,14,15].
tion of suspended particles in the feed solution, Film theory, gel layer, osmotic pressure, and
while the tangential feed flow over the membrane boundary layer resistance models are several of
surfaces in the crossflow case carries suspended the theoretical approaches that have been de-
solids downstream due to fluid shear forces. In veloped [1,2,16]. However, the accuracy of theore-
MF/UF processes, the major aim for efficient fil- tical modeling has been hampered by insufficient
tration is to minimize permeate flux decline caused knowledge regarding the complexity of the micro-
by the accumulation of particles on the membrane scale phenomena occurring during the filtration
surface and/or within membrane pores. processes. In addition, model designs involve spe-
Fouling is an unavoidable deleterious pheno- cific assumptions that may lead to deviations be-
menon in the filtration process that causes serious tween theoretical predictions and experimental
permeate flux decline followed by deterioration observations. Such deviations imply that funda-
of product water quality. Particle accumulation, a mental theoretical models sometimes do not have
major fouling mechanism in MF and UF, can be sufficient capability to depict fouling phenomena
typically classified into two processes: concentra- occurring in real filtration systems, although the
tion polarization (CP) and cake layer formation models accurately depict basic underlying trans-
between the CP layer and the membrane surface port mechanisms. Purely empirical models, which
[1–8]. The solute (i.e., particles, in this study) CP can be built upon specific experimental obser-
layer reaches its steady state after a short time vations and then used to predict the membrane
period when the filtration process begins. There- system performance, appear to be new alter-
after, suspended particles continuously accumu- natives. One such method is the artificial neural
late and form a dense cake layer which becomes network (ANN) approach.
the major resistance to the permeate water flux. The primary advantage of ANN over theore-
Several studies on permeate flux decline indicate tical approaches is that, as a black box model, it
that particle accumulation during crossflow col- does not require any governing equation with
loidal membrane filtration is affected by physical forceful assumptions specifically describing the
and chemical characteristics of the feed water as underlying engineering phenomena. ANN can
well as hydrodynamic operating conditions [9–12]. learn the complex transport processes of a system
Design and application of membrane filtration from given inputs and observed outputs, serving
require development of predictive models that can as an instrument for universal data approximation.
inter-link solution properties and operating con- Accordingly, a considerable number of ANN
ditions to filtration performance. To predict perme- applications for prediction, classification, signal
ate flux decline, many theoretical models have processing, and optimization can be found in
been proposed using physical, chemical, and hyd- various fields of finance and economics, meteo-
rodynamic modeling parameters such as particle rology, chemistry and chemical engineering, com-
size, zeta potential, Hamaker constant, tempera- puter science, and so forth [17–20]. Those applica-
ture, solution pH, ionic strength, transmembrane tions exemplify the ANN’s great potential for
pressure, shear rate, and so forth [13]. In most predicting transport phenomena.
practical applications of MF/UF, effects of the CP Extensive research has been performed to
layer are barely measurable since the cake layer investigate the capability of an ANN as a tool for
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 417
RBFNN is another type of neural network. where ŷ is the RBFNN simulation result (output),
Such networks have 3 layers, i.e., the input layer, wi is the optimized connection weight determined
the nonlinear hidden layer, and the linear output through the training process [29], and b2 is the
layer. RBFNN can overcome some of the limita- bias in the output layer.
tions of BPNN by using a rapid training phase, Fig. 1 gives an insight into the structure and
having a simple architecture, and maintaining working procedure of the RBFNN. The open
complicated mapping abilities. circles are bias neurons that adjust the sensitivity
In most cases, the RBFNN simulates pheno- of the network. The biases are controlled by a
mena of interest by using Gaussian basis functions specific value, called “spread” number, and each
in the hidden layer and linear transfer functions bias is set to 0.8326/spread [31]. The selected
in the output layer. The major difference in “spread” value should be large enough for neurons
operation between RBFNN and BPNN speci- in the hidden layer to include the whole range of
fically exists in the hidden layer. Instead of the input data.
weighted sum of the input vector used in BPNN, In RBFNN simulations, the proper initial
the distance between the input and center, ex- choice of centers and weights should be regarded
plained below, is employed in the RBFNN learn- as key issues. Various methods are proposed to
ing process. initially locate the center, e.g., random selection,
The first layer of the RBFNN collects the input K-mean technique, max-min algorithms, etc.
data. Its training process determines the number Using the Neural Network Toolbox, we choose
of hidden neurons, m, which can be larger than the weight vectors as the center parameter. Instead
that of BPNN to achieve a certain accuracy of of being randomly generated, the initial value of
prediction [31]. For each neuron in the hidden the weights is set as the transpose of the input
layer, the distance between the input data and the vector. Once the centers are developed, the
center is activated by a nonlinear radial basis weights linking the hidden and output layers
function, as shown in the following equation: should be updated during the training procedure.
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 419
4
3 (a) pH = 6.1
2
1
Permeate flux (10 m/s)
0
-5
4
3 (b) pH = 8.3
2
1
0
4
3 (c) pH = 10.0
2
1
0
0 10 20 30 40 50 60 70 80 90 100 110 120
Time (min)
Fig. 2. Experimental data and ANN predictions on the effect of solution pH on permeate flux decline with ionic strength
of 10–1 M KCl. The filtration conditions employed are particle size 47 nm, transmembrane pressure 41.4 kPa (6 psi),
particle volume concentration 0.01%, crossflow velocity 0.246 m/s, and temperature 20°C. At each pH value, the solid
and the hollow symbols represent experimentally observed and ANN-simulated data while × indicates points selected
from the experimental data and used for the training process.
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 421
demonstrate that the feed water pH has only minor However, at the later stages of membrane filtration
effects on the permeate flux. Comparing Figs. 2 when cake resistance becomes dominant, the
and 3 indicates that the initial permeate flux slight- steady-state permeate fluxes become independent
ly decreases with pH, and this behavior is captured of the solution pH.
by the RBFNN. However, the trained RBFNN
does not accurately duplicate the almost identical
3.2. Effect of ionic strength
permeate fluxes at pHs of 8.3 and 10.0 (Fig. 3).
The neural network slightly over-predicts the The RBFNN’s predictability of the influence
initial permeate flux at a pH of 8.3 for the first of ionic strength on the permeate flux was inves-
10 min of filtration. We think this over-prediction tigated using three different particle sizes of
stems from the preparing the training data set only 47 nm, 110 nm, and 310 nm and four ionic strength
from pHs 6.1 and 10.0 cases, excluding pH 8.3 data. values of 10–4, 10–3, 10–2, and 10–1 M KCl [9]. The
Comparison of Figs. 2 and 3 also shows that experimental data and modeling results are shown
the initial permeate flux increases at higher ionic in Fig. 4, which clearly shows the excellent pre-
strength and lower pH(s) due to the narrow capil- dictability of the RBFNN for permeate flux over
lary effect on fluid viscosity. At the initial stage, a wide range of ionic strengths and particle sizes.
when particle deposition is negligible, the intrinsic The predictions and the experimental data do not
membrane resistance dominates. Under low pH show a noticeable difference with a correlation
and high ionic strength conditions, the decreasing coefficient of 0.9944 and RMSE of 0.076 at the
fluid viscosity near membrane pores allows water 99% confidence level throughout the entire range
to penetrate the membrane pores with relative of transient permeate flux.
ease, leading to the initial enhanced permeate flux. As expected, increasing ionic strength pro-
4
3 (a) pH = 6.1
2
1
Permeate flux (10 m/s)
0
4
-5
3 (b) pH = 8.3
2
1
0
4
3 (c) pH = 10.0
2
1
0
0 10 20 30 40 50 60 70 80 90 100 110 120
Time (min)
Fig. 3. Experimental data and ANN predictions on the effect of solution pH on permeate flux decline with ionic strength
of 10–3 M KCl. The filtration conditions employed are particle size 47 nm, transmembrane pressure 41.4 kPa (6 psi),
particle volume concentration 0.01%, crossflow velocity 0.246 m/s, and temperature 20°C. At each pH value, the solid
and the hollow symbols represent experimentally observed and ANN-simulated data while × indicates points selected
from the experimental data and used for the training process.
422 H. Chen, A.S. Kim / Desalination 192 (2006) 415–428
Fig. 4. Experimental data and ANN predictions on the effect of ionic strength on permeate flux decline for (a) 47 nm,
(b) 110 nm, and (c) 310 nm particles. The filtration conditions employed are pH 10, transmembrane pressure 41.4 kPa
(6 psi), particle volume concentration 0.01%, crossflow velocity 0.246 m/s, and temperature 20°C. For each particle size,
the symbols × and + indicate the selected experimental data points of ionic strength of 10–4 and 10–1 M, respectively, for
the training process. The solid symbols indicate experimentally observed data of ionic strength 10–4 M (c), 10–3 M ( ),
10–2 M (y), and 10–1 M (d) of KCl, while the corresponding hollow symbols represent the simulation results.
motes more severe permeate flux decline and lying phenomenological mechanisms, i.e., inter-
accelerates the rate of reaching a limiting flux level particle and hydrodynamic interactions.
because the electrostatic double-layer repulsion
is mollified by the increasing ionic strength, caus-
3.3. Effect of transmembrane pressure
ing a dense cake layer of enhanced hydraulic re-
sistance. In Figs. 4a and 4b, the RBFNN closely The ability of RBFNN to simulate the trans-
captures the underlying fundamental effects of the membrane pressure effect on the permeate flux is
double-layer repulsion through various ionic examined in this section. Results shown in Fig. 5
strengths on the permeate flux. On the other hand, demonstrate that the RBFNN model can closely
Fig. 4c reveals quite a different trend of transient predict the permeate flux under different trans-
fluxes from those of Figs. 4a and 4b because the membrane pressures of 62.1, 41.4, and 20.7 kPa
flux profiles of Fig. 4c seem to converge into a [9]. The accuracy is reflected by a correlation coef-
single limiting permeate flux level. This behavior ficient and RMSE of 0.994 and 0.092, respective-
indicates that the influence of larger particle size ly.
(inducing larger pore size) can suppress the effect Fig. 5 shows that the permeate flux tends to
of interparticle interactions, leaving hydrody- reach an almost identical limiting flux under the
namics as the dominating mechanism in flux de- same ionic strength regardless of applied trans-
cline. The trained RBFNN shows its ability to membrane pressure and initial flux. As expected,
predict flux decline for ionic strengths of 10–2 and Fig. 5 confirms that flux decline is accelerated by
10–3 M by learning two different types of under- increasing transmembrane pressure and ionic
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 423
Fig. 5. Experimental data and ANN predictions on the effect of transmembrane pressure on permeate flux decline for
ionic strengths of (a) 10–4 M, (b) 10–3 M, and (c) 10–2 M KCl. The filtration conditions employed were pH 10, particle size
47 nm, particle volume concentration 0.01%, crossflow velocity 0.246 m/s, and temperature 20°C. For each particle size,
the symbols × and + indicate the selected experimental data points of transmembrane pressure of 62.1 kPa (9 psi) and
20.7 kPa (3 psi), respectively, for the training process. The solid symbols indicate experimentally observed data of trans-
membrane pressure 62.1 kPa (9 psi) (c), 41.4 kPa (6 psi) (y), and 20.7 kPa (3 psi) (d), while the corresponding hollow
symbols represent the simulation results.
5
(a) RBFNN
2
Ntrain=96
Ntest=471
2
1 R =0.988
RMSE=0.082
1 2 3 4 5
-5
Measured permeate flux (10 m/s)
(b) BPNN
Predicted permeate flux (10 m/s)
4
-5
2
Ntrain=96
Ntest=471
2
1 R =0.958
RMSE=0.156
1 2 3 4 5
-5
Measured permeate flux (10 m/s)
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 425
(c) MR
Predicted permeate flux (10 m/s) 4
-5
Ntrain=96
1 Ntest=471
2
R =0.719
RMSE=0.371
0
0 1 2 3 4 5
-5
Measured permeate flux (10 m/s)
Fig. 6. (a) RBFNN, (b) BPNN, and (c) MR predictions of permeate flux with experimental measurement under different
operational conditions. The solid straight line represents the line of equality and the dashed lines represent ±10% variance
from it. The R-square and RMSE between the predicted and measured data are also provided.
14 (=N10) out of Ntest = 471 predicted (tested) points the permeate flux under different operational
lie outside the region enclosed by the two dotted status. However, when compared with the
lines, indicating that 97% of the points are within RBFNN prediction in Fig. 6a, BPNN produces a
the ±10% relative error. (N10 stands for the number somehow more scattered plot. Sixty-one (=N10)
of points beyond ±10% relative error.) This ex- out of 471 points are not confined within the two
cellent performance of RBFNN is also quantified dotted lines. (Note that N10 of the RBFNN is 14.)
by an RMSE of 0.082 and an R-square (R2) of Only 87% of the predicted points are within
0.988. In spite of broad variations of feed water acceptable error in this case, whereas 97% were
parameters and operational conditions, which within ±10% relative error in the RBFNN case.
cause complexity to the filtration system, overall To quantitatively prove the superiority of the
the results indicate that employing only 17% (96 neural networks, we do the same calculation using
out of 567 points) of the total data for training the conventional MR method, of which its linear
renders satisfactory prediction of the remaining equation, obtained by the identical training data,
83% (471 out of 567 points) of the data. has the following form:
Previous investigations have suggested that
RBFNNs have multiple advantages in comparison J = 0.943 + 0.025 [∆P ] + 0.1663log10 [IS]
(5)
with the performance of BPNNs. In order to verify − 0.0192 [pH] + 0.0028 [PS] − 0.0133 [t ]
this concept, an identical simulation was carried out
using BPNN, and the result is presented in Fig. 6b. The regression equation is also used to predict the
The hollow circles are crowded near the 1:1 match permeate flux of the remaining data. Results for
line, suggesting that BPNN is also able to predict MR are shown in Fig. 6c. It is clearly evident that,
426 H. Chen, A.S. Kim / Desalination 192 (2006) 415–428
Table 1
Comparison of the performance of RBFNN, BPNN, and MR in terms of R-square (R2), root mean square error (RMSE),
points beyond ±10% relative error (N10), and simulation time, given the same number of total data set (Ntotal), training set
(Ntrain), and testing set (Ntest)
given the same information, MR provides sig- various combinations of operational conditions.
nificantly less accurate performance, which is In this study, the RBFNN is applied to predict the
mainly because the complex nonlinear membrane permeate flux on crossflow membrane filtration
filtration process could not be presented by the as a function of transmembrane pressure, ionic
simple linear method. Compared with those in strength, solution pH, particle size, and elapsed
Figs. 6a and 6b, hollow circles in Fig. 6c are much filtration time. Results show that the transient pro-
more deviated from the 1:1 match line. More than files of the permeate flux during crossflow mem-
half (51.6%) of the predicted points (471) are out brane filtration can be predicted by a single RBFNN
of the ±10% relative error range. with acute accuracy, given a limited number of
Finally, Table 1 compares the performance of training points. Comparison of the performances
RBFNN, BPNN, and MR using four parameters of RBFNN, BPNN, and MR confirms the
— R-square (R2), RMSE, the number of points superiority of RBFNN in terms of the R-square,
beyond the ±10% error (N10) and required simula- RMSE, N10 and simulation time required of higher
tion time with identical conditions of Ntotal, Ntrain, accuracies.
and Ntest. RBFNN predicts the experimental obser- As a consequence, it may not be necessary to
vations much more closely in comparison to BPNN carry out an entire series of expensive pilot or full-
and MR. Additionally, the RBFNN training method scale tests to collect and verify filtration data. The
eventually speeds up the training process of the RBFNN can interpolate the performance of mem-
neural network by as much as 40 times the BPNN brane filtration under other conditions of interest
training rate, providing higher adaptability when by using widely ranged and sparse data points to
a large set of observation data is used to investigate reduce the time and costs required. Although pilot-
more complex filtration systems. scale experimental tests restrict the number of
operating parameters that generally are of import-
ance in larger-scale applications, they still can
4. Conclusions
closely simulate full-scale operations. In the same
Due to the complex physicochemical micro- manner, RBFNN can also serve as potential pre-
phenomena occurring during membrane filtration, diction tools for full-scale operations, possibly
conventional theoretical models have been able combining several trained networks of different
to predict the filtration procedure only under scales into one smart neural network.
limited conditions with specific and/or inevitable
assumptions. An artificial neural network method
Acknowledgement
provides a unified approach for analysis and pre-
diction of the membrane performance under This research was supported by Saehan Indust-
H. Chen, A.S. Kim / Desalination 192 (2006) 415–428 427
ries, Seoul, Korea and the US Geological Survey crossflow microfiltration, Chem. Eng. Sci., 45
(Grant 01HQGR0079), through the Water Re- (1990) 13–25.
sources Research Center, University of Hawaii at [11] P. Bacchin, P. Aimar and V. Sanchez, Influence of
surface interaction on transfer during colloid ultra-
Manoa, Honolulu, HI. This is contributed paper
filtration, J. Membr. Sci., 115 (1996) 49–63.
CP-2005-11 of the Water Resources Research [12] R.M. Mcdonogh, A.G. Fane and C.J.D. Fell, Charge
Center, University of Hawaii at Manoa, Honolulu. effects in the cross-flow filtration of colloids and
particulates, J. Membr. Sci., 43 (1989) 69–85.
[13] W.R. Bowen and F. Jenner, Theoretical descriptions
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