NEURAL NETWORKS SIMULATION OF THE FILTRATION OF SODIUM CHLORIDE AND MAGNESIUM CHLORIDE SOLUTIONS USING NANOFILTRATION MEMBRANES

N. A. Darwish1 , N. Hilal2, H. Al-Zoubi2 and A. W. Mohammad3

Department of Chemical Engineering, The Petroleum Institute, Abu Dhabi, United Arab Emirates. Centre for Clean Water Technologies, School of Chemical, Environmental and Mining Engineering, The University of Nottingham, UK. 3 Department of Chemical and Process Engineering, Universiti Kebangsaan Malaysia, Selangor Darul Ehsan, Malaysia.
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Abstract: Articial neural network (ANN) simulation is used to predict the rejection of two salts (NaCl and MgCl2) at typical seawater concentrations in a cross-ow nanoltration membrane process. Rejections are predicted as a function of feed pressure and permeate ux with the salt concentration as a parameter. ANN predictions of the two salts rejections are compared with experimental results obtained using three different nanoltration membranes (NF90, NF270 and N30F) in a cross ow ltration set-up. The experimental program spans a concentration range of 5000 to 25 000 ppm for NaCl solution and of 5000 to 20 000 ppm for MgCl2 solution at pressures covering the range of 2 9 bars. The effects of the training algorithm, neural network architectures and transfer function on the ANN performance, as reected by the percentage average absolute deviation are discussed. A network with one hidden layer comprising four neurones is found to be adequate for mapping input output relationships and providing a good interpolative tool. Algorithms based on the conjugate gradient, regularization and quasi-Newton principles were found to outperform those based on the gradient descent and variable momentum gradient descent. The former algorithms gave an average absolute percentage deviation up to 5% whereas deviations up to 20% are obtained from the latter algorithms. For most of the cases considered, the ANN proved to be an adequate interpolation tool, where an excellent prediction was obtained for some concentration levels not represented in the training data set. For very limited cases, the ANN predictive performance was poor. However, the networks performance in these extreme cases didnt improve even with increasing the data points in the training data set.
Correspondence to: Dr N. Darwish, Department of Chemical Engineering, The Petroleum Institute, Abu Dhabi, UAE. E-mail: ndarwish@pi.ac.ae

Keywords: nanoltration; membranes; articial neuron networks; rejection; permeate ux.

DOI: 10.1205/cherd06037 02638762/07/ $30.00+0.00 Chemical Engineering Research and Design Trans IChemE, Part A, April 2007 # 2007 Institution of Chemical Engineers

INTRODUCTION
Nanoltration (NF) membranes are a type of pressure driven membranes that have properties in between those of ultraltration (UF) and reverse osmosis (RO) membranes. NF membranes have the advantages of providing a high water ux at low operating pressure and maintaining a high salt and organic matter rejection (Raman et al., 1994). The NF process benets from ease of operation, reliability and comparatively low energy consumption as well as high efciency of pollutant removal (Eriksson, 1988). In addition, NF membranes have recently been employed in pre-treatment facilities in both reverse osmosis and thermal processes (Hassan et al., 1998; Al-So et al., 1998). This will enhance
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the production of desalted water, reduces its production cost, and lowers the energy consumption of the desalination processes. Moreover, nanoltration is an environmentally friendly process. Therefore, NF membranes have boosted worldwide interest. A recent comprzehensive review on the use of NF membranes in water treatment has been presented elsewhere (Hilal et al., 2004). The performance of NF membrane separations is important for the design and optimization of ltration processes. This will reduce the number of experiments and subsequently save time and money. Since most commercial NF membranes are electrically charged, their performance depends heavily on the sieving (steric-hindrance) effect and Donnan (electrostatic) effect. Therefore, the removal of neutral
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model based on the Maxwell Stefan transport equations. This model is claimed to predict permeate ux and rejections of multi-component liquid feeds as a function of membrane properties (mean pore size, porosity, thickness, surface charge characteristic) and feed pressure. The above mathematical models were derived from physical descriptions and understanding of the NF process. These models are mathematically complex, computationally expensive and they ideally require a very detailed knowledge of ltration process as well as characterization of the membranes (Bowen et al., 2000). Therefore, there is a need to nd an alternative means for predicting process performance by exploiting available process data and extending it to unavailable data. Linear and nonlinear regression methods are examples of what are known as black box models. However, this is a signicant problem in this approach since numerous types of non-linearity get scrambled together with no clue as to which of these nonlinearities is predominant. Articial neural networks (ANNs) are another type of black box models. ANNs, however, are capable of modelling highly complex and non-linear systems with large numbers of inputs and outputs. Therefore, ANNs offer a more attractive alternative to conventional black box models in dealing with complex phenomena (Bowen et al., 2000). From the early 1990s, ANNs have been widely applied in many research areas such as modelling (Trichard et al., 1995), prediction, fault detection and process control (Dirion et al., 1996; Fakhr-Eddine et al., 1996). In the eld of membrane separation processes ANNs have successfully been applied to different types of the membranes; microltration (Dornier et al., 1995; Piron et al., 1997; Hamachi et al., 1999), ultraltration (Bowen et al., 1998a, b; Delgrange et al., 1998a, b; Teodosiu et al., 2000), nanoltration (Bowen et al., 2000). Dornier et al. (1995) used ANNs to predict the evolution of membrane fouling during crossow microltration of cane sugar and gum streams. Their results showed a good prediction of time evolution of the resistance. Recurrent ANNs and a hybrid model (combining a physical model with an ANN) were used to predict the performance of the dynamics of bakers yeast crossow microltration (Piron et al., 1997). Results obtained from the hybrid model were found to be more accurate than those coming from pure ANN modelling. The hybrid model, however, is limited and its assumptions need to be veried for other applications. Hamachi et al. (1999) used the recurrent ANNs to predict ux and deposition thickness in bentonite suspension microltration. In another study, Bowen et al. (1998a, b) applied ANNs

components (such as organics) results from size exclusion (solute and pore size), or differences in diffusion rates in a non-porous structure, which depends also on molecular size (Van der Bruggen and Vandecasteele, 2003; Chellam and Taylor, 2001). The polarity and the charge of organics might inuence the separation processes (Van der Bruggen et al., 1999), especially in large-pore membranes. In addition to the sieving effect, rejection of ionic components (salt solutions) in NF membranes occurs as a result of charge interaction between the membrane surface and the ions (Donnan exclusion), as well as differences of diffusivity and solubility of the ionic components or a combination of these (Peeters et al., 1998). These interactions depend, in addition to temperature and pressure of the ltration processes, on the characteristics of the electrolyte solution (such as the concentration, pH level and the composition for the electrolyte solution) and the membrane itself (e.g., surface charge, pore size and the roughness of the membrane). These factors will affect the efciency and cost of membrane processing which is dependent on the ux and rejection of permeates. Therefore, permeation ux and solute rejection data are necessary for the design, operation and optimization of new membrane separation processes. Towards this objective, many mathematical models have been used to predict the rejection of ionic solutes, as well as other variables such as permeate ux, feed concentration and pressure. One of these models is Spiegler Kedem model (Spiegler and Kedem, 1966; Jitsuhara and Kimura, 1983; Perry and Linder, 1989; Schirg and widmer, 1992; Levenstein et al., 1996; Pontalier et al., 1999; Diawara et al., 2003; Hilal et al., 2005; Xu and Spencer, 1997). This model treats a membrane as a black box and characterises it in terms of two parameters; salt permeability, Ps and reection coefcient, s. These two parameters are obtained from the experimental data of rejection versus permeate ux by a best-t method. Donnan steric-pore model (DSPM) (Van der Bruggen and Vandecasteele, 2003; Bowen et al., 1997; Schaep et al., 2001) is another model that is based on the extended Nernst Planck equation. This model describes the transport of ions in terms of an effective membrane thickness, porosity ratio and an effective membrane charge density. This model has undergone several modications by taking into account the hindrance effect of the ions through the pores in the membranes (Bowen and Mukhtar, 1996), concentration polarization (Bowen and Mohammad, 1998), and dielectric constant (Bandini and Vezzani, 2003). Furthermore, Straatsma et al. (2002) developed a NF membrane

Figure 1. Architecture of feed-forward neural network with a single hidden layer of S neurons. Trans IChemE, Part A, Chemical Engineering Research and Design, 2007, 85(A4): 417 430

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Figure 2. The average absolute percentage deviation for different training algorithms for the 4,1 net using log-sigmoid transfer function (algorithms acronyms as per Matlab 6.5).

with single hidden layer for proteins and colloids crossow ltration using UF membrane. It was found that the careful selection of input variables and training points helps in optimizing the ANN training process and in achieving very accurate predictions of the experimental results. For the same membrane, ANNs have been applied to predict trans-membrane pressure in a drinking water process and time evolution of membrane fouling (Degrange et al., 1998a, b). Different network structures have been checked and some of them allowed prediction of pressure with very good accuracy. In another study employing ANN approach, a model was developed to predict the ux during ultraltration of wastewater (Teodosiu et al., 2000). The trained networks were able to accurately capture the non-linear dynamics for initial uxes. On the other hand, ANNs have been used successfully to simulate reverse osmosis of ethanol and acetic acid and ultraltration of bleach plant efuent (Niemi et al., 1995). It has therefore been possible to estimate the permeate ux and the rejection rate from the process variables. The study of Bowen et al. (2000) is among very few studies in the open literature about utilizing ANN in modelling nanoltration processes; Toward this end, ANN has been used to predict the rejections of single salts (NaCl, Na2SO4, MgCl2 and
Table 1. Percentage average absolute deviations for different network architectures operated with two different training algorithms and two different transfer functions. Percentage average absolute deviation Trainbr Network architecture 2:1 3:1 4:1 5:1 3:3:1 2:2:1 logsig 2.8 2.8 2.5 2.5 8.9 11.3 tansig 6.6 2.7 2.5 2.5 11.5 11.4 Traincgp logsig 2.9 2.8 2.6 2.5 3.1 3.3 tansig 3.1 2.9 2.5 2.8 4.4 2.9

Figure 3. Reproducibility of ANN prediction from 10 different runs using the same training data set (a) trainbr: at each pressure the 10 predicted R% coincide with each other (b) traingdx: at each pressure the predicted R% differ from one trial to another (data set: 5000 ppm NaCl).

MgSO4) and mixtures of these salts at a nanoltration membrane. The predictions have been compared to pilot plant rejection data obtained with a spiral-wound membrane. The overall agreement between ANN predictions and experimental data was very good for both single salts and mixtures. In this study, ANN analysis will be applied to provide a means of modelling NF process performance. In particular, the rejections as a function of pressure and permeate ux of single salts (NaCl and MgCl2) at three nanoltration membranes will be predicted using ANN model. In addition, the affect of the input training dataset, the training algorithm and network architecture on the efciency of ANN predictions, as reected by percentage average absolute deviation, will be investigated.

ARTIFICIAL NEURAL NETWORKS APPROACH

ANNs may be described as a group of simple processing elements called neurons arranged in parallel layers that are fully interconnected by weighted connections. There are several types of ANNs mentioned in the literature (Hagan et al., 1996) such as feed-forward networks (or perceptron

(Input: system pressure, P and salt concentration, C; output: rejection percentage, R%; data set: NaCl).

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Figure 4. Performance of ANN in correlating the rejection-pressure data of NaCl nanoltration using NF90 membrane: (a) training using 12 data points, (b) training using 16 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

Figure 5. Performance of ANN in correlating the rejection-pressure data of NaCl nanoltration using NF270 membrane: (a) training using 12 data points, (b) training using 16 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

network), competitive networks (Hamming network) and recurrent networks (Hopeld network). Most recently, stacked neural networks have been applied to solve complex problems (Shuang-Quang et al., 2006; Wolpert, 1992). The most famous type of ANN in use is the feed-forward networks, particularly, the multi-layer perceptron network. In this type of ANNs, information ows in the forward direction only. ANNs interface independent variables through the neurons of an input layer and transmit output of dependent variables through the neurons of an output layer. The number of independent and dependent variables, therefore, dictates number of neurons in the input and the output layers, respectively. In between the input and the output layers there is at least one hidden layer that can have any number of neurons. According to the universal approximation theory (Tambe et al., 1996), an ANN with a single hidden layer with enough number of hidden neurons can map any input to any output to any degree of accuracy. Additionally, bias is an extra input added to neurons, which always has a value of 1 and treated like other weights. The

reason for adding the bias term is that it allows a representation of phenomena having thresholds (Delgrange et al., 1998b). Neurons in the hidden and the output layers calculate their inputs by performing a weighted sum of the outputs they receive from the previous layer. Their outputs, on the other hand, are calculated by transforming their inputs using a non-linear transfer function. The most widely used transfer functions are the S-shaped log-sigmoid (logsig) transfer functions, the S-shaped tan-sigmoid (tansig) transfer functions, and the pure linear transfer function (purlin). The logsig transfer function produces outputs in the range of 0 to 1. The tansig function, on the other hand, produces output in the range of 21 to 1. Outputs in the range of 21 to 1 can be produced from the linear transfer function (Niemi et al., 1995; Delgrange et al., 1998b). The architecture of the feed-forward ANN with a single hidden layer of S neurons is shown in Figure 1. In this gure, the input vector P is represented by the solid vertical bar at the left. The dimension of P is displayed below the variable as R 1 indicating that the input is a single vector of R elements. These inputs go to the S R weights matrix W 1 in

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Figure 6. Performance of ANN in correlating the rejection-pressure data of NaCl nanoltration using NF30 membrane: (a) training using 12 data points, (b) training using 16 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

Figure 7. Performance of ANN in correlating the rejection-pressure data of MgCl2 nanoltration using NF90 membrane: (a) training using eight data points, (b) training using 12 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

the hidden layer. A constant 1 enters the neurons as an input and is multiplied by a bias b i and represented as b vector. This vector is summed with the weighted inputs (W 1) to form the net input n 1 vector with S dimension as seen in equation (3): n1 W1 P b1 (1)

The neurons output vector a 1 with S dimension is then obtained by operating the transfer function on n 1. The same procedure is repeated in the output layer. The net inputs of the output layer are shown in equation (4), while a 3 represents the overall output of the network. This output could be a scalar or a vector, depending on the case under study. n2 W2 a1 b2 (2)

There are usually four steps involved in ANN modelling: (1) assembling the training data of input (independent variables)

and output (dependent variables), (2) deciding the network architecture, (3) training the network, and (4) simulating the network response to new inputs. The training process is simply an optimization process which aims at nding the set of weights and biases associated with each layer that will minimize the error objective function related to the deviations of the ANN predictions from the target values. The error objective function is usually the sum of squared errors between the targets and ANN outputs. ANN weights and biases in this process are updated in a systemic way by means of minimizing an error function using any of the wellknown optimization techniques. The most widely used is the back propagation algorithm (Rumelhart et al., 1986), which is based on the steepest-descent principle. There are several input variables to this algorithm, such as the learning rate (h), the momentum coefcient (a), number of hidden layers (L) and the number of hidden neurons (H) that have an effect on the ANN training. The predictions, also, can be judged by a combination of some parameters such as absolute errors and number of training cycles or epochs (C).

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Figure 8. Performance of ANN in correlating the rejection-pressure data of MgCl2 nanoltration using NF270 membrane: (a) training using eight data points, (b) training using 12 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

Figure 9. Performance of ANN in correlating the rejection-pressure data of MgCl2 nanoltration using NF300 membrane: (a) training using eight data points, (b) training using 12 data points, solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

The algorithms used here fall in four categories: (1) Training algorithms based on the batch steepest descent (traingd): The weights and biases here are updated in the direction of the negative gradient of the performance function in which the learning rate is held constant throughout training. Based on the same algorithm but with variable learning rate, another training algorithm (traingdx), which is another example of high performance batch steepest descent training algorithms, is used. This algorithm is known to converge from 10 to 100 times faster than the previous traingd. (2) Training algorithms based on the quasi-Newton (secant) method, which, in minimizing the error objective function, track the steepest descent direction but do not require calculations of the Hessian matrix. The one-step-secant algorithm (trainoss) have been utilized as an example of this algorithm. (3) Training algorithms based on the conjugate gradient principle, which follow a path in the direction of conjugate

gradient in their search for the minimum. The Polak Ribiere algorithm (traincgp) has been as a representative for this family of algorithms. (4) Training algorithms based on modifying the performance function by adding a term to the sum of squares of the network errors. This term consists of the mean sum of squares of the network weights and biases. Automated regularization (trainbr) is an example of this training algorithm, which is based on Baysian principles (Hagan et al., 1996). Here, the weights and biases of the network are assumed to be random variables with specied distributions. The regularization parameters are related to unknown variables associated with these distributions. These parameters, then, are estimated using statistical techniques.

EXPERIMENTAL Filtration Experiments

The experimental set-up used in this study for the cross ow ltration experiments has been described in a previous

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Figure 10. Performance of ANN in correlating the rejection-ux data of NaCl nanoltration using NF90 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

published paper (Hilal et al., 2005) on the ltration of sodium chloride salt solution using three NF membranes, i.e., NF90, NF270 and N30F. The same set-up with the same kind of NF membranes are employed for the ltration of magnesium chloride (MgCl2) at the same pressure levels previously encountered but with different salt concentrations. The setup, which was designed to carry out the experiments in a laboratory scale, consisted of a circular disc membrane with an effective ltration area of 12.6 cm2 and a stainless steel gear pump. The pump was used to circulate the feed solution of MgCl2 at ambient temperature in a total re-circulation mode, i.e., both the concentrate and the permeate streams are recirculated into the feed tank, so that the feed concentration is kept approximately constant. The pressure was varied between 2 and 9 bars while the concentrations varied from 5000 to 20 000 ppm. These concentrations cover the salinity range of MgCl2 in seawater where NF membranes have recently been used in the pretreatment operations in desalination processes. The MgCl2 salt was obtained from Fisher scientic-UK with purity better than 99.5%. The permeate ux and rejection were determined by varying the applied feed pressure at different feed concentrations. In order to determine the concentration of salt in the feed and the permeate solutions, the conductivity of these solutions were

measured at 258C by a conductivity meter (Hand-Held Meter, LF 330/340, WTW-Germany). Three commercial NF membranes were used in this study, two of which were supplied by FILMTEC and manufactured by DOW chemical company (USA). These two membranes are NF90 and NF270, which are made from polyamide. The third membrane was NADIR N30F, obtained from MICRODYN-NADIR Gmbh (Germany), which is made of polyethersulfone. Further details to the ltration experiments can be found elsewhere (Hilal et al., 2005).

Application of Neural Network

The feed-forward ANN (perceptron network) has been used in this work with single hidden layer and using pure linear transfer function for the output layer. Different network architectures and two sigmoidal transfer functions (logsig and tansig) for the hidden layers have been studied in seeking the best network in describing the experimental data. The network architectures investigated are 2 : 1, (i.e., one hidden layer with two neurones and one output layer) 3 : 1, 4 : 1, 5 : 1, 3 : 3 : 1 and 2 : 2 : 1. Towards the same objective, different back propagation training algorithms have been explored.

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Figure 11. Performance of ANN in correlating the rejection-ux data of NaCl nanoltration using NF270 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

In this work, ANN algorithms as programmed in the neural network toolbox of Matlab 6.5 have been used to predict rejections versus pressure and rejections versus permeate uxes for NaCl and MgCl2 solutions using three different nanoltration membranes (that is NF90, NF270 and N30F). The network prediction is compared with the data obtained from a carefully conducted experimental program using the aforementioned three membranes in a cross ow membrane set-up. The experimental study covers pressures in the range of 29 bar and concentrations in the range of 5000 25000 ppm. The network was trained using two different input training sets of data. In both cases, the input data to the ANN are feed pressure, permeate ux and the concentration of the salts while the output is rejection. The computer program used in this paper was written using Matlab programming language and executed on a PC.

of applying ANN in the modelling of NF membranes using two training algorithms as programmed in Matlab.

ANN: Training Datasets

In all ANN analysis performed in this study, the output sought was the rejection percentage (R%) of the salt and membrane under consideration. The neural net, however, was operated on two different inputs; in one case, a column vector of the operating pressure and a column vector of the salt concentration were employed. In the second case, a column vector of the permeate uxes and a column vector of the salt concentration were utilized as inputs. In each case, two different partial training datasets were used; the rst training set contained only 12 training data points from some of the available constant-concentration experimental data, i.e., 5000, 15 000 and 25 000 ppm at pressures of 2, 4, 7 and 9 bar. The remaining (18) points represent the validation points for the ANN. The second data set included training points from all studied concentration (5000 25 000 ppm) with a total number of 16 points, which represents the rst dataset in addition to four other points at concentrations of 10 000 and 20 000 ppm and pressure of 2 and 9 bar. Again, the remaining (14) points represent

RESULTS AND DISCUSSION

Salt ltration using membranes is a highly complicated and non-linear phenomenon due to the complex ion membrane and ion ion interactions that occur near and through the membrane. In the following sections, we present our results

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Figure 12. Performance of ANN in correlating the rejection-ux data of NaCl nanoltration using NF30 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

the validation points of ANN. For MgCl2 salt, the rst set contained eight training data points at concentrations of 2000 and 5000 ppm and pressures of 2, 4, 7 and 9 bar for all studied membranes leaving 16 experimental data points for the validation process, while the second set contains four more points at concentrations of 1000 ppm and 15 000 ppm and pressure 2 and 9 bar. The points remaining for validation are 12 data points.

Effect of Architectures and Training Algorithms on the ANN Performance

Figure 2 shows the percentage average absolute deviation (PAAD) for ve training algorithms used in combination with a 4-1 network employing a logsigmoid transfer function. It is clear that algorithms based on the conjugate gradient, regularization and quasi-Newton principles (traincgp trainbr and trainoss, respectively) outperform those based on gradient descent and variable momentum gradient descent (traingd and traingdx) The former algorithms give an average absolute percentage deviation of up to 5% whereas deviations up to 20% are obtained from the latter algorithms. The best algorithms are then utilized to determine the optimum

network architecture and the best transfer function. The results of this study are presented in Table 1. It is clear that the network architecture with one hidden layer such as (4,1) and (5,1) give lower PAAD than network architecture with two hidden layers especially for trainbr algorithm. Single hidden layer network with trainbr and traincgp algorithms give comparable values of PAAD. However, trainbr algorithm was found to be of more stability towards different initial guesses in weight and biases. Traincgp algorithm on the other side was found to be sensitive towards initial guesses in weights and biases, i.e., results differ from one run to another depending on the random initial guesses generated by Matlab. Furthermore, the runtime using trainbr is less than that using traincgp. The effect of transfer function was also addressed as shown in Table 1. It is clear that logsig give PAAD values lower than those using tansig. Another positive point for trainbr has been concluded throughout Figures 3(a) and (b). The sensitivity of two training algorithms (trainbr and traingdx) towards initial guesses in weights and biases is presented in Figure 3, which shows the results of 10 different iterations for the case of NaCl ltration at a concentration of 5000 ppm and pressure in the range of 2 9 bar using NF90 membrane Reproducibility of

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Figure 13. Performance of ANN in correlating the rejection-ux data of MgCl2 nanoltration using NF90 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

trainbr results is quite obvious in Figure 3(a) and the sensitivity of traingdx is also evident in Figure 3(b).

ANN Prediction of Salt Rejection with Pressure Sodium chloride salt

The ANNs prediction of salt rejection as a function of pressure for NaCl solutions using the three investigated membranes will be considered in this section. The ANN prediction, as well as the experimental data, is shown in Figures 4 6. Salt concentration spans the range of 5000 to 25 000 ppm, whereas pressure covers the range of 2 9 bars. In all of these gures, solid symbols are used to identify experimental data points which are used in the training phase of the ANN while open symbols are used for data points not included in the training phase, i.e., points used in the validation phase. Note also that solid lines in these gures represent a polynomial t of the ANN prediction. It can be seen that the ANN successfully predicts the nonlinear behaviour of rejection versus pressure. As shown in Figure 4(a), the ANN performs well in the training phase where a good prediction is obtained for concentrations levels from which

some data points have been included in the training phase. The concentration levels represented in the training phase are the 5000, 15 000 and 25 000. The ANN interpolative performance for the 10 000 and 20 000 ppm concentration levels (which were not represented in the training phase) is shown to be of less quality. For the 10 000 ppm concentration, ANN prediction worsens with pressure with a tendency to overestimate the actual salt rejection. A maximum deviation of up to 10% is observed along this concentration level. However, for the other concentration level of 20 000 ppm, the ANN performance is much better with a maximum deviation of about 5%. When these concentration levels are represented in the training phase by including two extreme data points from each concentration level, the ANN predictions do not improve much beyond the previous case as shown in Figure 4(b). Figures 5 and 6 show the experimental rejection data and the results of ANNs predictions for NF270 and N30F membranes, respectively. It is evident from these gures that the interpolative capability of the ANN is quite impressive. With some data at three concentration levels (5000, 15 000 and 25 000 ppm) used in the training phase, the ANN

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Figure 14. Performance of ANN in correlating the rejection-ux data of MgCl2 nanoltration using NF270 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

successfully predicts data at the other two intermediate concentration levels of 10 000 and 20 000 ppm. For the NF270 membrane, the ANN tends to slightly overestimate the rejection versus pressure data for the 20 000 ppm with a growing deviation with pressure up to about 5% at the highest studied pressure. The interpolative prediction for the 10 000 ppm is almost perfect as shown in Figures 5 and 6 for both membranes. By including some data from these two concentration levels in the training stage, the ANN makes a perfect job as evident in Figures 5(b) and 6(b). The ability of the ANN to quantitatively describe data at high salt concentrations without recourse to sophisticated descriptions of non-ideal solutions seems here a signicant advantage. It is worth mentioning that the N30F membrane, as compared to the other two membranes, gave the lowest rejection (in the range of 3 6%) for the same NaCl concentration at 9 bar, with this rejection decreasing down to around zero at 2 bar.

Magnesium chloride salt

The experimental rejection data, as well as the ANN predictions for MgCl2 salt solutions for all studied membranes with different pressures and concentrations are shown in Figures 79. Salt concentration covered the range of 5000

to 20 000 ppm with the same range of pressure used in the NaCl case, i.e., 29 bars. Experimentally, NF90 and NF270 membranes give higher rejection of MgCl2 than of NaCl. However, rejection of MgCl2 was found almost the same as that of NaCl for the N30F membrane. From Figures 79 it can be seen that the ANN has an excellent interpolative capability. In most cases so far considered, it is sufcient to train the net on a partial set of data belonging to the extreme concentration levels. Training the net using four experimental data points from each of the 5000 and the 2000 ppm is seen to be sufcient for the net to correctly predict rejection versus pressure data at the other two concentration levels of 1000 and 15 000 ppm. This is evident in Figures 7(a), 8(a) and 9(a) where including data points from the inner concentration levels seems unnecessary. On the contrary, comparison of the ANN prediction for the 10 000 ppm concentration level in the case of NF90 [Figures 7(a) and (b)] shows that the ANN performs better for less data points in the training set. This can be interpreted in terms of the network architecture; low number of weights and biases can lead to over-tting problems in cases of large size of training data. For the NF270 membrane, the ANN slightly overestimates salt rejection data with a maximum percentage deviation of about 5% especially

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Figure 15. Performance of ANN in correlating the rejection-ux data of MgCl2 nanoltration using NF30 membrane; solid symbols: training data set, open symbols: validation data set, solid lines: ANN prediction.

at lower pressures [Figure 8(a)]. However, as shown in Figures 8(a) and (b), the performance is improved by including the inner concentration levels in the training phase of the net. The ANN can be condently applied in making a good interpolation for inner concentration levels. The experimental rejection data and ANNs prediction for the N30F membrane are presented in Figures 9(a) and 9(b). This membrane gives the lowest rejection among the studied membranes for the same experimental conditions (range of the salt concentration and operating pressure). The ANNs is shown to have the capability of predicting the experimental rejection data for this membrane even at low values of salt rejection and pressures. The network performance is only marginally improved by including data from the inner concentration levels and thus can be condently applied towards interpolation for other concentration levels not included in the training data sets. It is thus evident that the ANN technique, which is an easyto-use black box method of correlation, is able to quantitatively describe the rejection data of the two investigated salts using three different membranes without the need for analysis in terms of effective pore radius, effective thickness/porosity ratio and effective membrane charge which may be difcult to relate to real physical parameters.

ANN Prediction of Rejection with Permeate Flux Sodium chloride salt

The ANN predictions of salt rejection as a function of permeate ux for NaCl solution and the experimental data for the three investigated membranes at different salinity levels are shown in Figures 10-12 (each is composed of four sub-gures, a, b, c and d). Again, NaCl Salt concentration spans the range of 5000 to 25 000 ppm. Figure 10 shows the ANN predictions for the NF90 membrane. Except for the 1000-ppm concentration level, there is an excellent agreement between ANN prediction and the experimental data. At the 1000-ppm level, the ANN model overestimates the experimental data with a deviation more than 20%. Salt rejection versus ux is shown to be not heavily dependent on salt concentration in the range of 15 000 25 000 ppm for NF90 membrane, as shown in Figure 10. The ANN predictions of rejection with permeate ux and the experimental data using NF270 and N30F are shown in Figures 11 and 12, respectively. It can be seen that ANN predictions for both membranes are excellent. Further improvements in the ANN prediction is obtained by including some experimental data points from the inner concentration levels. In particular, the 3% deviation appearing in

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NEURAL NETWORKS SIMULATION OF THE FILTRATION OF NACL AND MGCL2 SOLUTIONS

Figure 11(a) is shown to diminish in Figure 11(c) by including two data points on that concentration level. The ANN model perfectly describes the rejection data for the N30F membrane as shown in Figure 12. It is worthwhile mentioning that this membrane has low rejection at high ux in comparison to NF90 membrane.

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Magnesium chloride salt

The experimental rejection data, as well as the ANN predictions for MgCl2 salt solutions for all investigated membranes with different concentrations are shown in Figures 13 15. Salt concentration covered the range of 500020 000 ppm. High permeate uxes with high rejection of MgCl2 were obtained from all investigated membranes at low salt concentration. However, at high concentration the ux and rejection were relatively low. It is worthwhile mentioning that the ANN prediction using (trainbr) algorithm was not able to t the experimental data in this case. Alternatively, (traincgp) has been used, which gave good predictions. Furthermore, (traincgp) algorithm gave low value of PAAD similar to the value of (trainbr), see Figure 2. The ANN prediction of MgCl2 rejection versus permeate ux using NF90 membrane is shown in Figure 13. It can be seen from this gure that the ANN prediction using a limited number of data points in the training phase works except for 1000 ppm concentration level at pressure higher that 5 bar. The ANN prediction, in this case, lies below the experimented results. However, this underestimation in the ANN prediction is much alleviated by including extra data points from the inner concentration levels as shown in Figure 13. Figures 14 (a) (d) show the ANN prediction using NF270. Again, this membrane produced relatively high ux with low rejection. It can be seen here that the complex behaviour (non-linearity) of rejection with ux is well reproduced by ANN for all studied conditions and for the two training data sets with neglected overestimated at concentration 10 000 ppm using the limited training data set. Finally, predictions of the rejection with experimental data using N30F are shown in Figures 15(a) (d). As in the case of NaCl, N30F produced permeate with low rejections and uxes. Good ANN predictions have been obtained for this membrane with overestimation not more than 5%.

up to 20% are obtained from the latter algorithms. Rejection versus pressure and rejection versus permeate ux, for both salts and for all three membranes have been simulated using the ANN approach. ANN successfully tracked the nonlinear behaviour of rejection versus pressure and rejection versus ux. For most of the cases considered, the ANN proved to be an adequate interpolation tool, where an excellent prediction was obtained for some concentration levels not represented in the training data set. For very limited cases, the ANN predictive performance was poor. However, the networks performance in these extreme cases did not improve even with increasing the data points in the training data set.

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CONCLUSION
The application of articial neural networks to the modelling of crossow nanoltration of NaCl and MgCl2 has been investigated to predict the membrane rejection versus pressure and permeate ux at different concentrations and pressures using three NF membranes (NF90, NF270 and N30F). The concentrations levels were in the range of (5000 25 000 ppm) for NaCl and (5000 25 000 ppm) for MgCl2, while the pressure spanned the range of 29 bar. In additions, the effect of the training algorithm, net work architectures and transfer function on the ANN predictions has been discussed. It was found that a network with one hidden layer of four neurons is sufcient for prediction purposes. Different training algorithms have been explored. Algorithms based on the conjugate gradient, regularization and quasi-Newton principles were found to outperform those based on the gradient descent and variable momentum gradient descent. The former algorithms gave an average absolute percentage deviation up to 5% whereas deviations

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ACKNOWLEDGEMENTS
This work has been accomplished as part of a research project sponsored and funded by the Middle East Desalination Research Center (MEDRC).
The manuscript was received 31 March 2006 and accepted for publication after revision 11 December 2006.

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