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Chemical Engineering Department, University of Castilla-La Mancha, Campus Universitario s/n, 13004 Ciudad Real, Spain
Faculty of Chemical Engineering and Environmental Protection, Department of Chemical Engineering, Gh. Asachi Technical University Iasi
Bd. D. Mangeron, No. 71A, 700050 IASI, Romania
b
article info
abstract
Article history:
This article shows the application of a very useful mathematical tool, artificial neural
networks, to predict the fuel cells results (the value of the tortuosity and the cell voltage, at
a given current density, and therefore, the power) on the basis of several properties that
11 May 2010
define a Gas Diffusion Layer: Teflon content, air permeability, porosity, mean pore size,
hydrophobia level. Four neural networks types (multilayer perceptron, generalized feed-
forward network, modular neural network, and Jordan-Elman neural network) have been
applied, with a good fitting between the predicted and the experimental values in the
Keywords:
polarization curves. A simple feedforward neural network with one hidden layer proved to
GDL
be an accurate model with good generalization capability (error about 1% in the validation
PEMFC
phase). A procedure based on inverse neural network modelling was able to determine,
Neuronal networks
with small errors, the initial conditions leading to imposed values for characteristics of the
PBI
fuel cell. In addition, the use of this tool has been proved to be very attractive in order to
predict the cell performance, and more interestingly, the influence of the properties of the
gas diffusion layer on the cell performance, allowing possible enhancements of this
material by changing some of its properties.
2010 Professor T. Nejat Veziroglu. Published by Elsevier Ltd. All rights reserved.
1.
Introduction
and the second one is in fuel cells. A fuel cell is an electrochemical device that directly converts the chemical energy
contained in a fuel into electricity, promising power generation with high efficiency and low environmental impact. The
basic physical structure of a fuel cell consists of an electrolyte,
in contact with an anode and a cathode on either side.
The proton exchange membrane fuel cells (PEMFCs) are
one type of fuel cell suitable for portable, mobile and even
residential applications, due to their advantages, such as
high-power density, simple and safe construction, and quick
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
start-up, even at low operating temperatures [1]. PEMFC technology differs itself from other fuel cell technologies in the use of
a solid phase polymer membrane as cell separator/electrolyte.
PEMFCs are widely based on the use of perfluorosulphonated materials (Nafion and similar) as electrolyte.
Some of their qualities are high ionic conductivity when fully
hydrated (z0.1 Scm1), excellent mechanical strength, and
a demonstrated reliability during operation for more than
50,000 h [1]. However, Nafion membranes need to be hydrated
in order to be proton conductors, limiting the operational
temperature to 90 C at atmospheric pressure. This leads to two
important limitations: (i) the CO tolerance of the Pt catalyst
(tens of ppm), and (ii) a sluggish cathodic kinetic.
In order to overcome these drawbacks, it is advisable to
increase the operational temperature above 120 C. An appropriate material for working under these conditions is Polybenzimidazole (PBI). This material has certain advantages such
as high proton conductivity when impregnated with a nonvolatile acid (phosphoric acid), and an exceptional thermal and
chemical stability [2e6]. These properties have driven the rapid
development of PBI-based PEMFC systems since 1995, when it
was first proposed by Wainright and co-workers [7].
PBI-based PEMFCs are composed by the classical PEMFC
elements: electrolytic membrane (PBI), catalytic layer (Pt/
C PBI), gas diffusion layer (carbon substrate) and monopolar/
bipolar plates. It is evident that an optimum design, configuration and/or composition of all of these elements is fundamental in order to attain the highest and most stable possible
cell performance [8]. However, this work implies a large
number of experiments, resulting in a highly time, energy and
material consuming process.
Modelling can be used as an alternative in order to simplify
this experimental work, assisting in the prediction of the
experimental results. However, a simple look to rigorous
analytical models shows how complex is the modelling of
a PEMFC, due to the large number of variables and processes
affecting the performance [9e11]. In these conditions, an
empirical modelling is an appropriate opportunity. The use of
artificial neural networks (ANN) has become increasingly
recommended for applications where the mechanistic
description of the interdependences between variables is
either unknown or very complex. Direct neural network
modelling can be a powerful and accessible tool for determination the fuel cell characteristics as function of working
conditions. In addition, inverse neural network modelling
could give the initial conditions, which lead to pre-established
properties, substituting the complex modelling and optimization processes with a simple and rapid technique, supplying
reliable results. Some examples of the application of ANN to
the fuel cell field are collected in literature [1,12e15].
Generally, there are some specific issues for neural
networks which potential users should be aware of. The
neural networks have the capability to learn what happens in
a process, without modelling the physical and chemical laws
that govern the system. Consequently, they are very useful in
approximation of any continuous non-linear functions [16].
Parallel organization permits solutions to problems where
multiple constraints must be satisfied simultaneously, and
the high functionality and the rules are more implicit than
explicit. On the other hand, neural networks need large
2.
Method of approach
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
Topology
MLP
GFF
MNN
JEN
6:15:2
6:12:4:2
6:12:4:2
6:6:2
MSE
Correlation
Epochs
0.000113
0.000081
0.00022
0.000071
0.99999
0.99987
0.99972
0.99988
11000
18000
5000
5000
data sets. Six input variables were considered: PTFE (Polytetrafluoroethylene) content (%), porosity from Hg-porosity
(%), mean pore diameter (mm), air permeability (m2), hydrophobia level (%), and current density (mA/cm2). The outputs of
the neural model are cell voltage (mV), and tortuosity.
Experimental data come from the paper corresponding to
the reference 8 of this manuscript. In this article [8], the influence of the Teflon content of the gas diffusion layer on the cell
performance was studied, carrying out physical characterization and electrochemical measurements. Tables 1 and 2 of this
manuscript, along with the polarization curves, are the feed for
the current work. The explanation of the experimental techniques which characterize the gas diffusion layer, the operational protocol for obtaining the fuel cell results, and the
significance of each parameter have been described in the
experimental section of the previous paper [8].
The inverse neural network modelling answers to the
following problem: What are the initial working conditions
when the tortuosity and the cell voltage values are imposed?
Therefore, changing the outputs with the inputs in the first
problem, there is a high probability to determine the real
adequate parameters, in order to operate the fuel cell system
in good conditions.
Fig. 1 presents schematically the neural network-based
strategies in direct and inverse neural network modelling.
The next task in the modelling technique is to develop the
neural network topology. To determine the optimum network
configuration, different elements were tested within a trialand-error procedure: neural network types, number of hidden
layers and neurons, learning rules and activation functions.
In the present article four types of neural networks that
have as common characteristic the supervised learning
control (Multilayer Perceptrons, MLP, Generalized Feedforward Networks, GFF, Modular Neural Networks, MNN and
Jordan-Elman Networks, JEN) have been tested.
Multilayer perceptron, the most common neural network
architecture, can approximate any input/output map, but it
trains slowly and requires lots of training data. Generalized
3.
Table 2 e The performances of the neural models in the training and validation stages.
Network type
Training stage
Potential
MLP(6:15:2)
GFF(6:12:4:2)
MNN(6:12:4:2)
JEN(6:6:2)
Validation stage
Tortuosity
Potential
Tortuosity
Correlation
Average
error
Correlation
Average
error
Correlation
Average
error
Correlation
Average
error
1.000
0.999732
0.99958
0.999775
2.525
2.747
3.168
3.404
1.000
0.999998
0.99999
0.99999
0.007
0.020
0.048
0.046
0.99879
0.99929
0.999268
0.98371
1.269
0.954
1.245
10.983
1.000
0.999998
0.999991
0.99611
0.006
0.027
0.053
1.199
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
18
(1)
i1
MLP(6:15:2)
GFF(6:12:4:2)
MNN(6:12:4:2)
JEN(6:6:1)
16
14
-4
20
MSE x 10
3.1.
the outputs of the neural networks. The training time is represented by the number of epochs (a cycle for considering the
whole set of training data).
Fig. 2 shows the decrease of the error (MSE) during the
training process for the considered neural network types,
according to the Table 1, where the values at the end of the
training stage are given. This Figure shows the small errors at
the end of the training stage, similar for the four types of neural
networks (MLP, GFF, MNN, JEN). In addition, JEN benefits of the
shorter training time. But the decision regarding the choice of
the best model will be done after the validation stage.
In order to determine the best model, it is required a validation stage. In this phase, it was selected ten data from the
experimental set (not included in the training set). Figs. 3 and 4
show the validation stage for the cell voltage and the tortuosity,
respectively, for the models developed in this work. One can see
from these Figures that the MLP network provides the best
results for both modelled parameters (potential and tortuosity),
so this type of network has the best generalization capability.
In Figs. 3 and 4 the predictions of the neural networks are
grouped as followed: MLP and GFF in 3a and 4a for the potential
and tortuosity, respectively, and MNN and JEN in 3b and 4b.
Average relative errors (Equation (2)) were computed for
the two output parameters in the training and validation phases as one of the criterion of choosing the best neural models.
12
10
8
6
4
2
0
0
5000
10000
15000
20000
Epochs
Fig. 2 e The evolution of mean square errors for different
neural networks during the training process.
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
900
800
700
600
500
400
300
Tortuosity_MLP
3.5
Tortuosity_GFF
3
2.5
2
1.5
200
100
0.5
0
0
1
10
900
10
800
Potential_exp
700
Potential_MNN
Tortuosity_exp
Tortuosity_MNN
Tortuosity_JEN
3.5
Potential_JEN
600
5
4.5
Tortuosity
Potential, mV
Exemplars
Exemplars
Tortuosity_exp
4.5
Tortuosity
Potential, mV
Potential_exp
Potential_MLP
Potential_GFF
500
400
3
2.5
2
1.5
300
200
0.5
100
10
10
Exemplars
Exemplars
Er %
Oexp Onet
$100
Oexp
(2)
900
0% PTFE_exp
800
0% PTFE_net
10% PTFE_exp
700
10% PTFE_net
20% PTFE_exp
20% PTFE_net
600
Potential, mV
40% PTFE_exp
40% PTFE_net
500
400
300
200
100
0
0
250
500
750
1000
1250
1500
1750
Current density,mA/cm
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
76.3
73.9
69.6
61.6
3.2.
39.4
36.7
33.9
31.6
9.21
7.77
6.36
3.46
80.3
97.3
98.5
99.5
5
4
Tortuosity
3.3.
3
2
1200
1000
800
600
400
200
Tortuosity_exp
1
Current_density_net
Tortuosity_net
0
10
20
30
40
50
PTFE, %
Fig. 6 e A comparison between the experimental and
predicted tortuosity with MLP(6:15:2) in the training stage.
200
400
600
800
1000
1200
Current density_ex p
Fig. 8 e Current density obtained experimentally and by
MLP(2:10:6) prediction in validation phase of inverse neural
network modelling.
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
Table 4 e Prediction of the values of the cell voltage and power peak for intermediate Teflon percentages in the range
between 0 and 10% Teflon using MLP (6:15:2).
%
Porosity
Mean pore
Hydrophobia
PTFE
(%)
diameter (mm)
level (%)
0a
2.5
5
7.5
10a
76.3
76.0
75.1
74.1
73.9
a Experimental data.
39.4
38.7
37.9
37.1
36.7
80.3
90.2
92.5
95.4
97.3
Air
Permeability
1012 (m2)
9.21
8.85
8.50
8.14
7.77
309
312
316
324
325
247.2
249.4
252.5
259.4
260.0
1508.8
1502.3
1494.9
1487.2
1480.0
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 5 ( 2 0 1 0 ) 7 8 8 9 e7 8 9 7
900
porosity=60%; =30m
porosity=70%; =35m
porosity=80%; =40m
700
600
500
400
300
900
700
600
500
400
300
200
200
100
100
Hydrophobia level=80%
Hydrophobia level=90%
Hydrophobia level=100%
800
Cell voltage (mV)
800
900
permeability=4.5 m
permeability=6.5 m
permeability=8.5 m
800
700
600
500
400
300
200
100
0
Fig. 9 e Polarization curves obtained by predictions performed with MLP(6:15:2). (a) for different porosities (hydrophobia
level [ 90%, 1012 air permeability [ 8.5, average pore diameter [ F); (b) for different hydrophobia level (porosity [ 80%,
1012 air permeability [ 8.5, average pore diameter [ 40 mm); (c) for different air permeability (porosity [ 80%, hydrophobia
level [ 90%, average pore diameter [ 40 mm).
4.
Conclusions
This paper has shown the utility of the neural network tool for
the prediction and simulation of the fuel cell performance,
applied to the particular case of the influence of the gas
diffusion layer on the cell performance of a PBI-based PEMFC.
Firstly, the neural network was trained with available experimental data, learning about the behaviour of the system, with
a subsequent validation stage, concluding that the neural
network has satisfactorily reproduced it. In addition, the
inverse neural network has demonstrated the possibility of
inversely obtained the properties of the GDL for a given cell
performance, postulating it as an attractive optimization tool.
Thus, it can be concluded the neural network has shown its
Acknowledgements
This research has been supported by the Project PBI08-01512045 from the JCCM (Junta de Comunidades de Castilla-La
Mancha, Spain), and the Project CTM2007-60472 from the
Spanish Government, Ministry of Education and Science. This
work was also done by financial support provided by Romanian Ministry of Education and Research through Program
IDEI, Grants ID_592, Contract 59/2007.
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