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PII: S0167-7322(16)33661-3
DOI: doi: 10.1016/j.molliq.2017.06.088
Reference: MOLLIQ 7534
To appear in: Journal of Molecular Liquids
Received date: 18 November 2016
Revised date: 15 June 2017
Accepted date: 17 June 2017
Please cite this article as: Ali Barati-Harooni, Adel Najafi-Marghmaleki, Armin Mohebbi,
Amir H. Mohammadi , On the prediction of viscosity of Newtonian nanofluids, Journal of
Molecular Liquids (2017), doi: 10.1016/j.molliq.2017.06.088
This is a PDF file of an unedited manuscript that has been accepted for publication. As
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Young Researchers and Elite Club, Ahvaz Branch, Islamic Azad University, Ahvaz, Iran
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Young Researchers and Elite Club, South Tehran Branch, Islamic Azad University, Tehran, Iran
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Discipline of Chemical Engineering, School of Engineering, University of KwaZulu-Natal, Howard College
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Campus, King George V Avenue, Durban 4041, South Africa
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Institut de Recherche en Gnie Chimique et Ptrolier (IRGCP), Paris Cedex, France
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Corresponding author:
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1. Email Address: alibarati.2012@yahoo.com (A. Barati-Harooni)
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2. Email Address: a.h.m@irgcp.fr and amir_h_mohammadi@yahoo.com (A. H. Mohammadi)
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Abstract - One of the important properties of nanofluids is their viscosity which is required in
various applications. Despite the importance of this property, there is no general model for
prediction of viscosity of nanofluids. Hence, developing accurate and general models for
prediction of this property is of great importance. The purpose of this work is to develop four
accurate and reliable models based on Multilayer Perceptron Neural Networks (MLP-NNs),
Least Square Support Vector Machine (LSSVM), Adaptive Neuro Fuzzy Inference System
(ANFIS) and Gene Expression Programming (GEP) technique for prediction of viscosity of
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Newtonian nanofluids with different nanoparticles and different base fluids. An extensive
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number of 1140 data points of viscosity of nanofluids were utilized for development of the
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models. The predictions of the proposed models were examined with the predictions of various
techniques. Moreover, the accuracy of the proposed models was also examined by comparing
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their predictions with several well-known literature correlations. Results show that the developed
models provide accurate and reliable predictions and outperform literature correlations and
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present better results. Moreover, the predictions of CSA-LSSVM model are better and accurate
than the predictions of other developed models.
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1 Introduction
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concentrations below 4%vol) and a base fluid that normally includes conventional cooling fluids
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[1]. Thermal conductivity of these novel fluids were found to be appreciably higher than the base
fluid value, so that even in the low concentration of dispersed particles, anomalous heat transfer
Viscosity is one of the most significant thermo physical properties of nanofluids, especially
in thermal applications that involve heat transfer and fluid flow. The amount of required
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pumping power and the convective heat transfer coefficient are affected by the variation of
importance [3]. Over the past two decades, several researches have been conducted on the
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conductivity [6, 7], improvement of thermal conductivity [8] and estimation of thermal
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conductivity [9]. However, despite the importance of nanofluid viscosity in practical usages,
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only few researches have been carried out in this area [4, 10]. First, viscosity of nanofluid that
contained Al2O3, SiO2, and TiO2 as nanoparticles dispersed in water was measured by Masuda et
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al. [11]. In the next studies, the viscosity of different nanofluids was measured by several
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researchers [2, 5, 12-14]. In addition, the impact of various factors like shape, particle size,
volume fraction of nanoparticles and temperature over viscosity of nanofluid was studied [15].
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Process models allow generalizing experimental data and formulating results included in
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the processes [17]. Einstein model [18] nf = bf (1+2.5)) is the first nanofluid viscosity
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prediction model that is generally used at low volume fraction of nanoparticles (normally <0.02)
[19]. On the other hand, power law based models [20, 21] are more applicable for the prediction
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of the nanofluid effective viscosity at higher volume fraction (>0.02). Mehrabi [3] summarized
the most significant viscosity correlations of nanoparticles [3]. However, because of applying
some simple assumptions in development of these models, their reliability and validity are quite
limited.
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Recently, soft computing techniques like neural networks, fuzzy logic, and genetic
programming have been used in various data processing applications without conducting
Neural networks [25] and Adaptive neuro-fuzzy inference system (ANFIS) [3] have been
employed to model the viscosity of nanofluids. However, the number of fluids and contained
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nanoparticles and the range of input parameters used to drive former models are limited.
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Developing general models for precise prediction of nanofluid viscosity is the chief
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objective of the present study. In this work, four models based on MLP-NN, LSSVM, ANFIS
and GEP concepts are presented for prediction of viscosity of Newtonian nanofluids with
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different nanoparticles and different base fluids by using 1140 data points collected from
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literature. The outcomes of the developed models are compared with the literature models and
correlations. Results show the accuracy, superiority and higher generalization ability of the
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2 Theory
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MLP-NNs are one of the well-known and applicable types of Artificial Neural Networks
(ANNs) which are applied in nonlinear regression and fitting problems. These networks have a
three layer structure. Each layer has several units known as neurons. These neurons are the main
processing parts of MLP-NN networks. The first layer is the input layer which accepts the input
data points [26]. The number of neurons of this layer is identical to the number of input
parameters of the model. The second layer is known as hidden layer. This layer could have
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several sub layers. The number of neurons of this layer plays an important role in the prediction
capability of the model. Normally, the number of neurons of this layer is determined by using a
trial and error approach and by minimizing a cost function. The third layer is called output layer
which has a single neuron which delivers the output parameter of the model. The neurons of the
hidden layer contain a specific function which is called activation function or transfer function.
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Each neuron accepts an input vector and multiplies it by a weight vector and sums the result with
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a constant bias term and delivers it to the transfer function [24, 26]. The outputs of transfer
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functions are summed up and are delivered to the output layer as the output parameter of the
model. There are several types of activation functions including the linear, tansig and
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logsig types which are the most commonly applied ones. The weight terms in a MLP-NN
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model are optimized by an internal training algorithm such as Levenberg-Marquardt (LM)
algorithm to provide better performance for the model. By using the LM algorithm, the error is
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back propagated through the layers of model by minimizing of a cost function until the optimum
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weight vectors are evaluated and the output parameter is calculated by the model [27].
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The LSSVM modeling technique is a machine learning algorithm which has found
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extensive applicability in various fields. This algorithm was developed by modifying the original
concept of support vector machine (SVM). In SVM algorithm, the modeling of experimental
data leads to a quadratic programming problem which brings complexities in the optimization
and calculation process of the model [28, 29]. The LSSVM approach overcomes to these
complexities by solving the nonlinear fitting problem by using linear programming approach
which simplifies the calculation process of the model. Modeling a problem by using the LSSVM
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approach requires the optimization of two tuning parameters namely and 2 . These
parameters are required during solving the linear programming problem by using LSSVM
method. The optimum values of the aforementioned tuning parameters are normally determined
swarm optimization (PSO) [29, 30]. These parameters are optimized by minimizing a cost
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function between predicted data and target data. In the present work, these parameters were
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optimized using the CSA algorithm by minimizing the mean square error (MSE) between
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experimental data and predicted values. Further information about the performance of LSSVM
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algorithm is available in literature.
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2.3 Adaptive Neuro Fuzzy Inference System
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The ANFIS modeling technique is another soft computing approach which is useful for
nonlinear data modeling and fitting problems. This algorithm uses the combined abilities of
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Fuzzy Logic (FL) and Artificial Neural Networks (ANNs) [31, 32]. This algorithm has a five
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Layer 1: There are certain functions in this layer which are called membership functions
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(MFs). The number of these MFs is identical to the number of input parameters. Each MF
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accepts the individual inputs and applies a transformation on it. There are various types of MFs
which can be utilized in the nodes of first layer. However, the Gaussian type MFs is more
popular because they provide a smoother behavior for model. These MFs are formulated as
follows:
1 (X i Z j )
2
ij (X i ) exp( ) (1)
2 j2
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In which ij is the membership degree of j-th MF for i-th input parameter, Xi is the i-th
input parameter, Zj is the center of j-th Gaussian MF and j is the variance parameter of j-th
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MF.
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Layer 2: This layer determines a parameter known as firing strength (Wi) by multiplying the
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membership degrees of MFs for each input parameter as follows:
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m
W j ij (X j ) (2)
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i 1
Layer 3: In this layer, the calculated firing strengths in the previous layer are normalized
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between 0 and 1which is shown by W i as below:
Wi
Wi
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W i
i
(3)
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Layer 4: In this layer, the normalized firing strengths in the previous layer are multiplied by a
first order (linear) Takagi-Sugeno-Kang (TSK) type Fuzzy Inference System (FIS) as follows:
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m
W i f i W i ( nij X j rij ) (4)
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j 1
In which fi represents the first order TSK type FIS. The nij and rij parameters are adjustable
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variables of TSK FIS which should be optimized by a reliable algorithm to provide a better
Layer 5: The sum of all calculated values in the previous layer is the output parameter of the
Y W i f i (5)
i
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using optimization abilities of Genetic Algorithm (GA). The main applications of GEP are for
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regression and data fitting purposes. GEP is similar to GA in its operation and performance. This
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technique was developed by Koza [33] for the first time and was gradually modified after him.
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Among various computer-based techniques which are used to solve complex and nonlinear
problems, the GEP is one of the popular ones. In addition, an important drawback of other
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computer-based approaches such as Artificial Neural Networks (ANNs) is that, the final solution
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of these models for a problem is in a black-box form, which brings limitations on their
interpretation and applicability. However, GEP fits the input data and results in a final
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mathematical model for the problem, which provides higher generalization ability compared to
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The symbolic regression term is normally attributed to GEP because it finalizes its
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consideration. In classical data regression and fitting techniques, first it is needed to construct a
mathematical formulation and then tune and adjust the parameters and coefficients of the
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the mathematical form and the coefficients are constructed and adjusted simultaneously.
GEP conducts the fitting procedure in two stages. First, it combines the functions (the
functions that are characterized and defined by user to be implemented in the fitting process)
based on a random decision process and then it adjusts and optimizes the coefficients of each
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constructed model by minimizing a cost function which is normally the Mean Square Error
In the next step, GEP uses its operators such as cross over and mutation to construct a new
population of better and fittest solutions. Mutation operator replaces a bad performance sub-tree
with a new sub-tree with better performance. Cross over is also the process of combining two
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better and fittest expressions to generate a new offspring.
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Generally, GEP uses two approaches to process a fitting problem called Standard Genetic
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Programming (SGP) and Multi-gene Genetic Programming (MGP). In SGP technique, just one
gene is created and used, while in MGP technique, several genes are created to handle the fitting
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problem. Every gene in MGP method is generated by weighted linear combinations of results of
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several SGP trees and each tree is considered as a gene in the total fitting process [36].
The mathematical formulation of MGP fitting procedure can be represented as below [37]:
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N
Y P b0 w i G i (6)
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i 1
where YP is the estimated value by the GEP model, Gi is the ith gene in model, N represents
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the number of genes utilized in GEP fitting process, wi denotes the weight term of the ith gene
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and b0 is the bias term. The optimum values of weight terms for each gene are evaluated by least
square fitting of estimations of the proposed GEP model versus experimental data. For instance,
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Y d 0 d1 (a b Sin(c )) d 2 (d e f g ) (7)
This figure represents a symbolic regression which composes of two genes and a
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3 Data acquisition
in recent years [2, 3, 10, 38-41]. According to these works, it can be concluded that the viscosity
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nanoparticle, bulk density of nanoparticle and viscosity of the base fluid. Hence, these
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parameters were utilized as input parameters for development of the models. Moreover, as the
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viscosity of base fluid was not reported in some data points, this parameter was calculated by
using an appropriate correlation for each system. These correlations are summarized in Table 1.
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In the present study, an extensive number of 1140 experimental data of viscosity of
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different nanofluids with various mixtures of nanoparticles and base fluids were collected from
several published works in the literature [2, 3, 13, 38-49]. The statistical details of the gathered
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data points which were used in the present study are listed in Table 2. Moreover, the name and
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type of base fluid and nanoparticle as well as the number of data points gathered from each
4 Model development
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An important parameter which greatly affects the performance of the MLP-NN model is
the number of neurons in the hidden layer of this network. In the present study, a single hidden
layer network with tansig type transfer function in the hidden layer and purelin transfer function
in the output layers is utilized. The number of neurons in the hidden layer was changed from 4 to
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25 and the MSE value of the model was monitored for different models. Figure 2 shows the plot
of the MSE value of different models against the number of neurons of the hidden layer. As is
clear from this figure the network with 18 neurons in the hidden layer exhibits the lowest MSE
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4.2 CSA-LSSVM model
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As mentioned earlier, modeling a non-linear data fitting problem by LSSVM model
requires optimization of two tuning parameters namely and 2 which are related to structure
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of these models. In the present study, the CSA algorithm was utilized to obtain the optimum
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values of these parameters. Using this algorithm, the optimum values of and 2 were
viscosity data first a TSK type FIS was constructed by using the training data. The TSK type FIS
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was constructed using the genfis 2 function of MATLAB. This function employs the subtractive
clustering method for development of the initial FIS. After construction of the initial FIS it
should be trained by using an appropriate algorithm. In the present work, the hybrid method was
utilized to train the initial constructed FIS. The parameters of the Hybrid-ANFIS model are listed
in Table 4.
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great effort was put forward to apply different GEP based correlations using trial and error
process. Throughout these trial and error approaches for development of GEP based model, it
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was found that an increase in the number of genes for a model leads to an increase in the depth of
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expression trees (ETs) and as a result leads to complexities in solution domain of problem and
final correlation and increases the run time of the model. As a result, in the present study, three
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genes were used for the final form of the GEP based model. Moreover, the Mean Square Error
(MSE) was used as a cost function to optimize the coefficients of final model. The operators and
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functions of , +, -, / and power ( ab ) were used for development of GEP based model. The input
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nanoparticle ( S (nm)), viscosity of base fluid ( bf (cp (centipoise))) and density of nanoparticle
( (g/cm3)). The output parameter was the viscosity of nanofluid ( nf (cp)). The optimum
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mathematical model which was achieved using GEP model for prediction of viscosity of
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nanofluid is as follows:
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nf ( A B C )10 (8)
2.708472(10 T 10 )
A 1.461570 10 bf (9)
16.484304
0.112396(10 10 bf ) (10)
B 10
S 10
S 4.872
C 31.49091107 (11.208771
10
)
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(11)
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5.1 Evaluation of the developed models
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Different statistical quality measure techniques were utilized to evaluate the accuracy of
predictions of the developed models. First, the estimated viscosity data were plotted versus the
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target viscosity data as shown in Figure 3. According to this figure, the experimental data and
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estimated data are acceptably distributed around the unit slope line (Y=X line) for all models.
This indicates that there is an acceptable agreement between predictions of the developed models
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and target viscosity data. The correlation coefficient of estimations of the developed models are
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0.9942, 0.9991, 0.9892 and 0.9505 for MLP-NN, CSA-LSSVM, Hybrid-ANFIS and GEP
models, respectively, which is another indication for the accuracy of the developed models.
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Figure 4 shows the relative deviation plot of outcomes of the proposed models. This figure also
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reveals that the relative deviations of the models are mostly concentrated in the region between
relative deviations of 20%. This indicates that the developed models are able to estimate most
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of target viscosity data with low relative errors. This figure also shows that the CSA-LSSVM
model exhibits better predictions in comparison with other models as the relative error in
utilizing three statistical parameters including correlation factor (R2), Average Absolute Relative
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Deviation (AARD%) and Root Mean Square Error (RMSE). The formulation of these
( Pr ed (i ) Exp (i )) 2
R2 1 i 1
N (12)
(
i 1
Pr ed (i ) Exp ) 2
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100 N ( Pr ed (i) Exp (i ))
AARD % (13)
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N i 1 Exp (i)
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N
( Pr ed (i ) Exp (i )) 2
(14)
RMSE ( i 1
) 0.5
N
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In which Pred denotes the estimated viscosity of nanofluid, Exp is the experimental value
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of viscosity, N denotes the number of data points and Exp is the average value of experimental
viscosity. The statistical parameters of the developed models are listed in Table 5. This table also
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confirms the accuracy of the developed models thanks to low values of AARD% and RMSE
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At this part, the predictions of the developed models will be compared with outcomes of
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the literature correlations for prediction of viscosity of nanofluids. Table 6 presents the
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formulation of these correlations. The cross plot of these correlations are shown in Figure 5.
Comparison between this figure and Figure 3 reveals that the estimations of these correlations
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diverge from unit slope line more than the developed models as well as lower R2 values which
confirm that the estimations of the developed models are more accurate and dependable than
these correlations. Moreover, Figure 6 shows the relative deviation plot of literature correlations.
According to this figure, the relative errors of these correlations are higher than the proposed
models. In addition, the cumulative absolute relative error plot of the proposed models and the
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literature correlations is shown in Figure 7. According to this figure, the predictions of the
models are accurate and dependable than other methods because most of data points predicted by
these models (about 80%) exhibit an error less than 20%. However, the literature correlations of
Batchelor [50], Wang et al. [51], Chen et al. [4], Abedian et al. [52], Ward [53], Brinkman [54],
Einstein [18] and Krieger and Dougherty [49,50] are capable of predicting about 36%, 57%, 58%,
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24%, 24%, 24% and 24% of data points, respectively, with an error less than 20%. This Figure
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also shows that the predictions of the CSA-LSSVM model are better than other developed
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models and literature correlations as this model is able to predict all of data points with relative
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The statistical parameters of these literature correlations are listed in Table 7. According to
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this table, these correlations exhibit higher AARD% and RMSE values and lower R2 values
compared to the proposed models which reveal that the developed models effectively
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In addition to these correlations, Meybodi et al. [55] recently developed a correlation for
prediction of viscosity of water based nanofluids. This correlation is also provided in Table 6. A
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comparison was also conducted between the predictions of the developed models and this
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correlation. However, as the correlation developed by Meybodi et al. [55] is just valid for water
based nanofluids, it was applied to data points in which the base fluid was water (907 data out of
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1140 data points). Figure 8 shows a graphical comparison between R2, AARD% and RMSE
values of the developed models in the present work and the correlation developed by Meybodi et
al. [55]. This figure also shows the accuracy of the proposed models because they exhibit higher
R2 values and lower AARD% and RMSE values compared to Meybodi et al. [55] correlation.
Another advantage of the developed models in the present work over Meybodi et al. [55]
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correlation is the higher generalization ability of the proposed models in this study. The newly
introduced models are not limited to water based nanofluids and in addition to water and
deionized water based fluids, are valid for other base fluids including mixture of ethylene glycol
and water, pure ethanol, pure ethylene glycol, mixture of propylene glycol and water, pure R11
refrigerant and toluene. Moreover, it should be mentioned that the developed correlation in the
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present work is just applicable for prediction of viscosity of nanofluid with Newtonian behavior
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(i.e. the viscosity of nanofluid is independent of shear rate).
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5.2 Sensitivity analysis of the input and output data
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To understand the relation between individual input parameters and the value of viscosity
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of nanofluid, a sensitivity analysis was performed on the effect of input data on the target
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viscosity value. For this purpose, the relevancy factor (r) was utilized. An input parameter with a
higher r value has greater influence on the value of output parameter (viscosity in the present
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work). However, it is better to use directional form of relevancy factor which contains a value
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with a certain direction and provides a better judgment about the influence of an input parameter
(Inp
i 1
k ,i Inp k ) 2 ( nf ,Pred (i ) nf ,Pred ) 2
i 1
In which nf ,Pred (i ) and nf ,Pred are the value of i-th predicted nanofluid viscosity and
average value of predicted nanofluid viscosity, respectively. Inp k ,i represents the i-th value of k-
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th input parameter and Inp k is the average value of k-th input parameter. Figure 9 depicts the
influence of individual inputs on viscosity of nanofluid for different nanoparticles. This figure
shows that the temperature has positive effect on the viscosity value of Al2O3, CuO, carbon nano
tube (CNT) and graphene based nanofluids and a negative effect on the viscosity of SiO2 and
TiO2 based nanofluids. This figure shows that the particle volume fraction has the largest effect
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on the viscosity of Al2O3 based nanofluids but for CuO, SiO2, TiO2 and graphene based
nanofluids the viscosity of base fluid has the largest impact on the viscosity of nanofluid. For
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CNT based nano fluids the size of nano particle has largest impact on the viscosity value.
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4. Conclusion
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In order to estimate the viscosity of Newtonian nanofluids, four models namely MLP-NN,
CSA-LSSVM, Hybrid-ANFIS and GEP were developed in the present study. The main objective
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of this work was to provide accurate and general models to improve the generalization ability
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and accuracy of previous literature correlations. The error analysis of predictions of the
developed models shows their acceptable accuracy and reliability of them. The comparison
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between statistical quality measure parameters of the developed models and the literature
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correlations also shows the superiority and higher accuracy of the models developed in the
present work. Moreover, the predictions of CSA-LSSVM model are more accurate and reliable
than the predictions of other developed models. As the developed models exhibit acceptable
generalization ability and accuracy, they could be effectively utilized for prediction of viscosity
of Newtonian nanofluids.
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Figure 1. Schematic structure of a MGP structure with two genes.
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Figure 5. Cross plot of predictions of the literature correlations: (a) Batchelor [50], (b) Wang et
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100
Einstein
90 Batchelor
Brinkman
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Ward
70 Wang et al.
Chen et al.
Frequency (%)
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Abedian et al.
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Absolute Relative Error (%)
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Figure 7. Cumulative frequency of data points versus absolute relative error.
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Figure 9. Sensitivity analysis of effect of different parameters on the viscosity of nanofluids
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Table 1. Literature correlations used to determine the viscosity of base fluid in each system.
1.12646 0.039638T
exp( )
bf (cp ) 1 0.00729769T Deionized Water (DIW) [40]
1000
247.8
2
bf (cp ) 2.414 10 T 140 Water [49]
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bf (cp ) exp(0.01797T 1.0305) [49]
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water (50:50)
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Table 2. Statistical details about gathered data bank in the present work.
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Density of nanoparticle (g/cm3) 0.2 6.31 4.40 1.44
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Viscosity of base fluid (cp) 0.39 6.03 1.08 0.96
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Viscosity of nanofluid (cp) 0.44 6.48 1.63 1.16
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Al2O3 Water 506 42, 43]
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CuO Ethylene glycol and water mixture 60:40 weight 11 [44, 45]
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Propylene glycol and water mixture, 30:70 [46]
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CuO volume 53
Carbon nanotube
DI water 2 [60]
(CNT)
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(SDBS)
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Parameter Description/Value
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Number of inputs 5
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Number of outputs 1
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Number of fuzzy rules 15
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Radius of influence/Radius of cluster 0.4
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All data
4.28 1.46 5.05 9.92
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Test data
AARD% Train data 3.82 1.36 4.55 9.58
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All data 3.92 1.44 4.95 9.85
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All data 0.088 AN 0.035 0.121 0.26
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bf
nf
(1 )2.5
Brinkman [54]
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Ward [53] nf bf (1 2.5 (2.5 )2 (2.5 )3 (2.5 ) 4 )
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nf bf (1 2.5 6.2 2 )
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Batchelor [50]
nf bf (1 7.3 123 2 )
Wang et al.
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[51]
[52] (1 2.5 )
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Krieger and
nf bf (1 ) 1.625
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0.65
57]
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Batchelor [50] 0.4589 30.38 1.9455
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Wang et al. [51] 0.6084 14.89 0.8387
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Chen et al. [4] 0.5992 14.93 0.8714
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Krieger and Dougherty
0.5421 25.32 0.9309
[56, 57]
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Research Highlights
Four viscosity models based on MLP-NN, LSSVM, ANFIS and GEP techniques have
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been developed for Newtonian nanofluids.
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1140 literature data were utilized for development of the models.
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The accuracy of the models has been examined by comparing their predictions with
several literature correlations.
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The models provides accurate predictions and outperforms literature correlations and
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presents better results.
The predictions of CSA-LSSVM model are better and accurate than the predictions of
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