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Investigation of Thermodynamic Properties of Refrigerant/Absorbent Couples

Using Artificial Neural Networks

Article  in  Chemical Engineering and Processing · October 2004

DOI: 10.1016/j.cep.2003.12.008

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 Chemical Engineering and Processing 43 (2004) 1253–1264

Investigation of thermodynamic properties of refrigerant/absorbent

couples using artificial neural networks
Adnan Sözen a,∗ , Mehmet Özalp a , Erol Arcaklioğlu b
a Technical Education Faculty, Mechanical Education Department, Gazi University, Teknikokullar, 06503 Ankara, Turkey
b Engineering Faculty, Mechanical Engineering Department, Kırıkkale University, 71450 Kırıkkale, Turkey

Received 11 March 2003; received in revised form 1 December 2003; accepted 2 December 2003

Available online 25 March 2004

Abstract

This paper presents a new approach to determine the properties of liquid and two phase boiling and condensing of two alternative refrig-
erant/absorbent couples (methanol–LiBr and methanol–LiCl), which do not cause ozone depletion for absorption thermal systems (ATSs)
using artificial neural networks (ANNs). The back-propagation learning algorithm with three different variants and logistic sigmoid transfer
function were used in the network. In order to train the neural network, limited experimental measurements were used as training and test data.
In input layer, there are temperatures in the range of 298–498 K (with 25 K increase), pressures (0.1–40 MPa) and concentrations of 2, 7, and
12% of the couples; specific volume is in output layer. After training, it is found that maximum error is less than 3%, average error is about 1%
and R2 values are 99.999%. As seen from the results obtained the thermodynamic properties have been obviously predicted within acceptable
errors. This paper shows that values predicted with ANN can be used to define the thermodynamic properties instead of approximate and
complex analytic equations.
© 2004 Elsevier B.V. All rights reserved.

Keywords: Artificial neural network; Thermodynamic properties; Ozone safe refrigerants; Methanol–LiBr; Methanol–LiCl

1. Introduction proposes two alternative refrigerant/absorbent fluid couples

Environment-friendly refrigerants with zero ozone deple-
tion potential are required to be used in refrigerators and
heat pumps according to Montreal Protocol signed in 1987
to regulate production and trade of the ozone-depleting
substances such as CFC and HCFC. Because of using
ozone safe fluid couples, an absorption thermal system
(ATS) that is easily adapted to solar-powered, gas-fired,
or waste-heat operations can be preferred [1,2]. Continued
research in this field depends on analysis of the alternative
fluid couples, which are thermodynamically acceptable and
harmless for the environment [3–12]. Fluid couples used
in these systems are required to have the properties of
thermal resistivity, high evaporating heat at relatively low
pressure values, low specific volume of vapor, low solidifi-
cation temperature and high critical temperature. This paper
∗ Corresponding author. Tel.: +90-312-2126820/1873;
fax: +90-312-2120059.
E-mail address: asozen@gazi.edu.tr (A. Sözen).
(methanol–LiBr and methanol–LiCl), which have these
thermal properties for ATSs and also do not cause ozone
depletion.
Thermodynamic analysis of the ATSs is too complex
because of thermodynamic properties equations of these
fluid couples, involving the solution of complex differen-
tial equations. To simplify this complex process, this paper
proposes a new approach (artificial neural network, ANN)
to determine of thermodynamic properties of two alter-
native refrigerant/absorbent fluid couples (methanol–LiBr
and methanol–LiCl). The advantages of ANN compared
to classical methods are speed, simplicity, and capacity to
learn from examples. In the last decade, some works about
the use of ANNs in the energy systems have been pub-
lished [13–24]. This technique can be used in the modeling
of complex physical phenomena. Instead of complex rules
and mathematical routines, ANNs are able to learn the
key information patterns within multidimensional informa-
tion domain. So, engineering effort can be reduced in the
areas.

0255-2701/$ – see front matter © 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2003.12.008
1254 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264
2. Artificial neural networks
Neural networks have been trained to perform complex
functions in various fields of application including pattern
recognition, identification, classification, speech, vision, and
control systems. Today neural networks can be trained to
solve problems that are difficult for conventional computers
or human beings. During the past 15 years there has been a
substantial increase in the interest on ANNs. The ANNs are
good for some tasks while lacking in some others. The ad-
vantages of ANNs compared to classical methods are speed,
simplicity, and capacity to learn from examples. So, engi-
neering effort can be reduced in the areas. They can learn
from examples and are able to deal with non-linear prob-
lems. Furthermore, they exhibit robustness and fault toler-
ance. The tasks that ANNs cannot handle effectively are
those requiring high accuracy and precision, as in logic and
arithmetic. ANNs have been applied successfully in a num-
ber of application areas [14–24]. Some of the most impor-
tant ones are:
• function approximation;
• pattern association and pattern recognition;
• associative memories;
• generation of new meaningful pattern.
The fundamental processing element of a neural network
is a neuron. Basically, a biological neuron receives inputs
from other sources, combines them in some ways, performs
generally a nonlinear operation on the result, and then out-
puts the final result.
ANNs are collections of small individual interconnected
processing units. Information is passed between these units
along interconnections. ANNs operate such as a ‘black box’
model, requiring no detailed information about the system.
On the other hand, they learn the relationship between the
input and the output. The network usually consists of an in-
put layer, some hidden layers, and an output layer [15]. An
artificial neuron and neural network architecture are shown
in Fig. 1. Each input is multiplied by a connection weight. In
the simplest case, products and biases are simply summed,
then transformed through a transfer function to generate a
result, and finally obtained output. Networks with biases
can represent relationships between inputs and outputs more
Fig. 1. Schematic diagram of an artificial neuron and neural network architecture for thermal properties.
easily than networks without biases. A transfer function con-
sisted generally of algebraic equations is linear or nonlinear
[20]. There are many useful transfer functions. Use of a non-
linear transfer function makes a network capable of storing
nonlinear relationships between input and output. Choice of
the function depends on problem that will be solved.
An important stage of a neural network is the training
step, in which an input is introduced to the network to-
gether with the desired output and the weights are adjusted
so that the network attempts to produce the desired output.
The weights, after training, contain meaningful information
whereas, before training they are random and have no mean-
ing. If it has reached a satisfactory level, the train stops, and
the network uses the weights to make decisions, to identify
patterns, or to define associations in test data.
There are different learning algorithms. A popular algo-
rithm is the back-propagation algorithm, which has different
variants. Standard back-propagation is a gradient descent al-
gorithm. It is very difficult to know which training algorithm
will be the fastest for a given problem.
ANN with back-propagation algorithm learns by chang-
ing the weights, these changes are stored as knowledge.
Some statistical methods, in fact RMS, R2 , cov, maximum
error (%), average error (%) values, were used for compari-
son. Error during the learning is called as root-mean-squared
(RMS) and defined as follows:
 1/2
1 
RMS =  |tj − oj | 
2
(1)
p
j
In addition, absolute fraction of variance (R2 ) and coef-
ficient of variation in percent (cov) are defined as follows
respectively:
 
j (tj − oj )
2
R =1−
2  (2)
j (oj )
2
RMS
cov = × 100 (3)
omean
where t is target value, o is output value, p is pattern, and
omean is the mean value of all output data [22]. Input and
output layer are normalized in the range of (−1, 1) or (0, 1).
 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264 1255

3. Modeling of the thermodynamic properties using Table 1

neural network Experimental samples for input and output data
T (K) P (MPa) X (%) V (cm3 /g)
Calculation of the thermal properties of fluid couples Methanol–LiBr Methanol–LiCl
used in absorption cooling and absorption heat pump is one
of the important problems. Determination of these prop- 298.15 1 2 1.23610 1.23600
298.15 30 7 1.14139 1.14924
erties of liquid and two phase boiling and condensing of 298.15 40 12 1.18912 1.09414
two alternative working fluid couples (methanol–LiBr and 323.15 10 2 1.26475 1.25864
methanol–LiCl), was done by an experimental set up, which 323.15 5 7 1.19160 1.20330
operates on the principle of a constant volume piezome- 323.15 20 12 1.10590 1.12807
ter by Bulgan et al. [25]. Experiments were done in the 348.15 30 2 1.22319 1.26579
348.15 20 7 1.20077 1.21033
ranges 298–498 K of temperature, 0.1–40 MPa of pressure 348.15 10 12 1.11470 1.15980
and 2–12% concentration of salt. In order to train the net- 373.15 20 2 1.32810 1.31550
work, these experimental results were used. Inputs for net- 373.15 10 7 1.24678 1.25678
work are temperature, pressure and concentration of fluid 373.15 5 12 1.19368 1.19124
couples; output is specific volume. 398.15 10 2 1.39194 1.38577
398.15 30 7 1.25000 1.25500
The back-propagation learning algorithm has been used 398.15 1 12 1.20382 1.22514
in feed-forward, single hidden layer. Variants of the al- 423.15 10 2 1.40943 1.44652
gorithm used in the study are scaled conjugate gradi- 423.15 30 7 1.27680 1.28753
ent (SCG), Pola–Ribiere conjugate gradient (CGP), and 423.15 40 12 1.19510 1.19830
Levenberg–Marquardt (LM). Inputs and outputs are nor- 448.15 2.4 2 1.59340 1.58240
448.15 10 7 1.37716 1.38329
malized in the (0, 1) range. Neurons in input layer have no 448.15 30 12 1.20792 1.24124
transfer function. Logistic sigmoid (logsig) transfer function 473.15 5 2 1.66672 1.70481
has been used. The transfer function used: 473.15 4 7 1.48730 1.49340
1 473.15 20 12 1.29236 1.29873
f(z) = (4) 498.15 30 2 1.59499 1.58582
1 + e−z 498.15 10 7 1.54019 1.55331
498.15 6.3 12 1.41760 1.41560
where z is the weighted sum of the input.
Computer program has been performed under MATLAB.
In the training, we used an increased number of neurons
(from three to eight) in hidden layer to define the output

Fig. 2. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiBr couple in SCG algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.
1256 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264

Fig. 3. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiBr couple in LM algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.

accurately. The neurons within the hidden layer perform two
tasks: they sum the weighted inputs connected to them and
then pass the resulting summations through a non-linear ac-
tivation function to the output neuron or adjacent neurons
of the corresponding hidden layer (in case of more than one
hidden neuron layer). There are 174 patterns from experi-
ments for fluid couples. To train the ANN, no more patterns
are necessary. The aim of ANN is to estimate the interval
values accurately. According to statistical values such as R2
and RMS, the training can be achieved with sufficient data.
In our application, we used 174 data. The data covers all
working conditions for absorption systems. So, when we
give the temperature and pressure values to ANN, specific
volume can be estimated easily.
When network training was successfully finished, network
was tested with test data. Since test results were also suit-
able, specific volume values in the ranges 293–498 K of tem-
perature, 0.1–50 MPa of pressure, and 1–13% concentration

Fig. 4. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiBr couple in CGP algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.
 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264
Table 2
Statistical values of thermodynamic properties for methanol–LiBr fluid couple
Algorithm RMS RMS for R2 R2 for Cov Cov for Maximum Max. error for Average Average error
neurons test data test data test data error (%) test data (%) error (%) for test data (%)
LM-3 0.00161 0.0004 0.99985 0.99999 0.01251 0.00329 3.48 0.59 0.94 0.27
LM-4 0.00159 0.00043 0.99985 0.99999 0.01238 0.0036 3.29 0.63 0.93 0.29
LM-5 0.00164 0.00047 0.99984 0.99999 0.01274 0.0039 2.91 0.54 0.97 0.36
LM-6 0.00145 0.00100 0.99987 0.99993 0.01129 0.0083 3.03 1.36 0.86 0.69
LM-7 0.00149 0.00114 0.99987 0.99991 0.01161 0.0094 2.71 1.62 0.88 0.78
LM-8 0.00113 0.00131 0.99992 0.99988 0.00881 0.0109 2.28 1.93 0.64 0.88
SCG-3 0.00176 0.00074 0.99981 0.99996 0.01369 0.00615 3.58 1.13 1.09 0.57
SCG-4 0.00164 0.00062 0.99984 0.99997 0.01276 0.0051 3.19 0.93 0.99 0.45
SCG-5 0.00180 0.00054 0.99981 0.99998 0.01402 0.0045 3.53 0.79 1.08 0.38
SCG-6 0.00169 0.00076 0.99983 0.99999 0.01310 0.0063 3.12 0.99 1.03 0.55
SCG 0.00161 0.00062 0.99984 0.99997 0.01254 0.0052 3.10 0.80 0.99 0.45
SCG-8 0.00161 0.00057 0.99985 0.99998 0.01250 0.0047 3.20 0.66 0.98 0.45
CGP-3 0.00245 0.00188 0.99964 0.99976 0.01905 0.01562 7.30 2.60 1.43 1.32
CGP-4 0.00213 0.00085 0.99973 0.99995 0.01656 0.007 7.47 0.92 1.17 0.59
CGP-5 0.00210 0.00130 0.99974 0.99988 0.01630 0.0108 6.96 1.47 1.19 0.88
CGP-6 0.00236 0.00149 0.99967 0.99985 0.01835 0.0124 7.64 1.73 1.34 1.18
CGP-7 0.00210 0.00059 0.99974 0.99998 0.01628 0.0049 6.42 0.67 1.24 0.47
CGP-8 0.00235 0.00136 0.99967 0.99987 0.01825 0.0113 7.52 1.97 1.35 1.01

1257
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A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264
Table 3
Statistical values of thermodynamic properties for methanol–LiCl fluid couple
Algorithm RMS RMS for R2 R2 for test Cov Cov for Maximum Maximum error Average Average error
neurons test data data test data error (%) for test data (%) error (%) for test data (%)
LM-3 0.000499 0.000238 0.999985 0.999996 0.003839 0.001896 2.949 0.380 0.221 0.151
LM-4 0.000503 0.000232 0.999985 0.999997 0.003868 0.001842 2.836 0.348 0.227 0.147
LM-5 0.000470 0.000314 0.999987 0.999994 0.003616 0.002494 2.857 0.544 0.205 0.172
LM-6 0.000471 0.000211 0.999987 0.999997 0.003623 0.001681 2.935 0.285 0.207 0.137
LM-7 0.000442 0.000269 0.999989 0.999995 0.003399 0.002139 2.567 0.386 0.182 0.164
LM-8 0.000472 0.000233 0.999987 0.999997 0.003627 0.001857 2.602 0.371 0.180 0.146
SCG-3 0.000716 0.000348 0.999970 0.999992 0.005504 0.002771 2.439 0.503 0.340 0.224
SCG-4 0.000734 0.000308 0.999969 0.999994 0.005641 0.002446 2.711 0.478 0.331 0.212
SCG-5 0.000734 0.000407 0.999969 0.999990 0.005641 0.003237 2.583 0.539 0.338 0.276
SCG-6 0.000717 0.000482 0.999970 0.999985 0.005517 0.003837 2.475 0.835 0.331 0.317
SCG-7 0.000630 0.000385 0.999977 0.999991 0.004844 0.003061 2.737 0.786 0.287 0.211
SCG-8 0.000728 0.000531 0.999969 0.999982 0.005601 0.004221 2.616 0.958 0.312 0.315
CGP-3 0.001692 0.001351 0.999833 0.999885 0.013014 0.010744 6.012 1.974 0.838 0.891
CGP-4 0.001571 0.001192 0.999856 0.999911 0.012079 0.009479 6.475 1.699 0.695 0.798
CGP-5 0.001622 0.001113 0.999846 0.999922 0.012475 0.008851 6.562 1.452 0.762 0.707
CGP-6 0.001750 0.001119 0.999821 0.999921 0.013456 0.008901 7.410 1.536 0.787 0.730
CGP-7 0.001802 0.001146 0.999810 0.999917 0.013857 0.009115 7.230 1.501 0.873 0.739
CGP-8 0.001364 0.000830 0.999891 0.999957 0.010485 0.006598 5.364 1.066 0.652 0.562
CGP-8 0.00235 0.00136 0.99967 0.99987 0.01825 0.0113 7.52 1.97 1.35 1.01
 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264 1259

of salt have been predicted with 5 K, 2 MPa, 0.3 increase
for each couple, respectively. In Fig. 1, an artificial neuron
and selected neural network architecture are schematically
shown. Sample patterns are shown in Table 1 in which there
are selected samples for fluid couples.
4. Results and discussions
In this work, selecting an alternative working fluid cou-
ples (methanol–LiBr and methanol–LiCl), which do not
cause ozone depletion for ATSs, ANN was used for PVT
representations of refrigerant in ranges 273–400 K and
0.1–50 MPa. Results have been demonstrated in Figs. 2–4
for methanol–LiBr fluid couple and in Figs. 7–9 for
methanol–LiCl fluid couple using four, and seven neurons
in the hidden layer of all algorithms. Graphics of other neu-
rons are similar to the four, and seven neurons in the hidden
layer. Statistical values such as RMS, R2 , and deviation (%)
are given in Table 2 for methanol–LiBr fluid couple and in
Table 3 for methanol–LiCl for all algorithms and 3–8 neu-
rons in the hidden layers. Comparison of statistical values
between some experimental and ANN predicted data are
also given in Tables 2 and 3. Tables 2 and 3 show that R2 is
very close to 1 for all data, average errors are about 1 and
RMS values are very small.
Maximum R2 value of 99.987% for methanol–LiBr is ob-
tained at LM algorithm with six and seven neurons in the hid-
den layer. For test data, this value of 99.999% is obtained at
LM algorithm with four and five neurons in the hidden layer

Fig. 5. Comparison of the experimental and ANN results for SCG algorithm with four neurons in the hidden layer for methanol–LiBr.
1260 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264

Fig. 6. Comparison of the experimental and ANN results for SCG algorithm with seven neurons in the hidden layer for methanol–LiBr.

and SCG algorithm with six neurons in the hidden layer and
CGP algorithm with four neurons in the hidden layer. Maxi-
mum and minimum errors are 7.63 and 2.28% at CGP algo-
rithm with six neurons in the hidden layer and LM algorithm
with eight neurons in the hidden layer, respectively. For test
data, maximum and minimum errors are also 1.97 and 0.54%
at CGP algorithm with eight neurons in the hidden layer
and LM algorithm with five neurons in the hidden layer, re-
spectively. It is shown in Table 2 and Figs. 2–4 that CGP
algorithm gives worse results than SCG and LM algorithm.
The most approach is of SCG algorithm with all neurons in
the hidden layer, but LM algorithm is better than SCG algo-
rithm for test data. Figs. 5–6 show a parity plot between the
compressibility factors generated by experimental data and
those computed by the neural network models for a learning
database of about 174 data points. It is clear (Table 2) that
the neural model gives a very accurate representation of the
statistical data over the full range of operating conditions and
indicates the good accuracy of the neural network to repre-
sent volumetric properties of refrigerant/absorbent fluid cou-
ples.Maximum R2 value of 99.9989% for methanol–LiCl is
obtained at LM algorithm with seven neurons in the hidden
layer. For test data, this value of 99.9997% is obtained at
LM algorithm with four, five and eight neurons in the hidden
layer. Maximum and minimum errors are 7.41 and 2.43%
at CGP algorithm with six neurons in the hidden layer and
SCG algorithm with three neurons in the hidden layer, re-
spectively. For test data, maximum and minimum errors are
 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264 1261

Fig. 7. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiCl couple in SCO algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.

also 1.97 and 0.28% at CGP algorithm with three neurons
in the hidden layer and LM algorithm with six neurons in
the hidden layer, respectively. It is shown in Table 3 and
Figs. 7–9 that CGP algorithm gives worse results than SCG
and LM algorithm. The most approach is of SCG algorithm
with all neurons in the hidden layer, but LM algorithm is
better than SCG algorithm for test data.
Table 3 and Figs. 10 and 11 indicate the good accuracy
of the neural network to represent volumetric properties of
refrigerant/absorbent fluid couples. As seen from the results

Fig. 8. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiCl couple in LM algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.
1262 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264

Fig. 9. The variation of specific volume with pressure and concentration ratio at different temperatures for methanol–LiCl couple in CGP algorithm: (a)
four neurons in the hidden layer; (b) seven neurons in the hidden layer.

Fig. 10. Comparison of the experimental and ANN results for SCG algorithm with four neurons in the hidden layer for methanol–LiCl.
 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264 1263

Fig. 11. Comparison of the experimental and ANN results for SCG algorithm with seven neurons in the hidden layer for methanol–LiCl.

obtained, the thermodynamic properties are obviously cal-
culated within acceptable uncertainties.
5. Conclusion
In this paper, ANN was used for PVTx representations
of ozone safe refrigerant/absorbent fluid couples from 293
to 498 K, up to 50 MPa and 1–13% concentration of salt.
Under the same working conditions and for the same con-
centration ratios, statistical errors in the methanol–LiCl fluid
couple are smaller than methanol–LiBr fluid couple, so it
will give better results for ATSs. This paper shows that val-
ues predicted with ANN can be used to define the ther-
modynamic properties instead of approximate and complex
analytic equations. Because the ANN approaching (R2 =
99.999%) are better approximation properties than the ana-
lytical equation approaching (R2 = 99.2%) [25]. Promising
results have been obtained for each fluid couples within ac-
ceptable errors. PVTx properties predicted are in valid re-
gion for working conditions of the refrigeration systems. So,
the thermodynamic simulation of ATSs using ANN will be
easier than using complex analytic equations.
Acknowledgements
This study was supported as the Research Projects of Gazi
University (Projects no. 07/2001-16 and 07/2003-47). The
author thanks to Michigan State University (MSU) for gives
 1264 A. Sözen et al. / Chemical Engineering and Processing 43 (2004) 1253–1264

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