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Engineering Science and Technology, an International Journal 18 (2015) 229e234

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Engineering Science and Technology,


an International Journal
journal homepage: http://www.elsevier.com/locate/jestch

Full length article

Quantitative recognition of flammable and toxic gases with


artificial neural network using metal oxide gas sensors in
embedded platform
B. Mondal a, *, M.S. Meetei a, J. Das b, C. Roy Chaudhuri c, H. Saha d
a
Department of Electronics and Communication Engineering, Tezpur University, Tezpur 784028, India
b
Department of Physics, Jadavpur University, Kolkata 700032, India
c
Department of Electronics and Telecommunication Engineering, Indian Institute of Engineering Science and Technology, Howrah, India
d
Centre of Excellence in Green Energy and Sensors Systems, Indian Institute of Engineering Science and Technology, Kolkata 711103, India

a r t i c l e i n f o a b s t r a c t

Article history: Artificial Neural Network (ANN) based pattern recognition technique is used for ensuring the reliable
Received 15 November 2014 evaluation of responses from an array of Zinc Oxide (ZnO) based sensors comprising of pure ZnO nano-
Received in revised form rods and composites of ZnOeSnO2. All the sensors were fabricated in the lab. The paper first reports the
19 December 2014
development of an artificial neural network based model for successfully recognizing different con-
Accepted 31 December 2014
Available online 31 January 2015
centration of hydrogen, methane and carbon mono-oxide. Feed forward back propagation neural
network was used for the classification of the gases at critical concentrations. The optimized ANN al-
gorithm is then embedded in the microcontroller based circuit and finally verified under lab conditions.
Keywords:
Neural network
© 2015 Karabuk University. Production and hosting by Elsevier B.V. This is an open access article under
Reliable detection the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Sensor array

1. Introduction attractive material for the detection of toxic, hazardous and


combustible gases. A wide range of sensors based on semi-
Qualitative and quantitative detection of flammable and toxic conductor metal oxides including ZnO, TiO2, SnO2, WO3, In2O3, etc.
gases like hydrogen (H2), methane (CH4) and carbon mono-oxide were used for the detection of gases like H2 [3], CH4 [4], LPG [5], CO
(CO) in coal mines, petroleum industries and gas storage plants [6] etc. Both ZnO and SnO2 are n-type wide band semiconductors
are of great importance for the safely of workers, health hazards which have attracted remarkable attention as highly sensitive
and to avoid risk of accidental explosion. H2 is a potential source of sensor material. These material were expected to be superior ma-
energy of future and is used in fuel cell [1], H2 engine cars, chemical terial for sensing gases like H2 [7,8], CO [9,10], and CH4 [10,11]. In
industry etc. H2 is a colorless, odorless and highly explosive gas spite of the high response, metal oxide semiconductor (MOx) based
having flammability in the range (4e75%) in air [2]. In coal mines sensor presents a serious drawback of poor selectivity, which hin-
presence of methane is always expected, which has caused most ders their commercial application. Therefore, MOx sensors fall
loss of life than any other gas. Methane in the range (5e14%) in air is short when a precise detection of specific concentration of gaseous
flammable [2]. CO is also a colorless and tasteless gas which is component is required or when they are used to discriminate a
believed to be the most dangerous gas in mine. CO in the range of mixture of gas. Drift in the sensor output due to ageing, poor sta-
50 ppm is fatal and is also flammable and explosive [2] in higher bility or high sensitivity to humidity of the ambient environment
range of concentrations. are also serious drawbacks of metal oxide based sensors. Both drift
Oxide based semiconductor sensors present advantages like and poor selectivity make the sensor output unreliable [12].
high sensitivity to low concentration of gases, less fabrication cost, Many authors have suggested various ways to overcome the
long term stability, low power consumption etc. which makes them problem of cross-sensitivity to achieve selective sensor which may
include, a) addition of noble catalytic metal to promote the reaction
to specific gas [13], b) operating the sensor in dynamic mode [14], c)
* Corresponding author. Tel.: þ91 03712 267007/8/9x5266. surface modification [15] and d) use of multi-compositional sensing
E-mail address: biplobm@tezu.ernet.in (B. Mondal).
film [16,17]. However, extremely selective sensors are very
Peer review under responsibility of Karabuk University.

http://dx.doi.org/10.1016/j.jestch.2014.12.010
2215-0986/© 2015 Karabuk University. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).
230 B. Mondal et al. / Engineering Science and Technology, an International Journal 18 (2015) 229e234

expensive and operating the sensor in dynamic mode makes the communications [29,30]. In a typical procedure, sol for pure ZnO is
measurement system complex. Although, the problem of cross- prepared by mixing 0.6 g of zinc acetate di-hydrate
sensitivity can be addressed with any of the above mentioned [Zn(CH3COO)2$2H2O] with aqueous solution of PVA under con-
ways, the troubles of reliability due to the drift in sensor output still stant stirring. The 1.0 M sodium hydroxide (NaOH) solutions was
persist. A potentially more cost effective way to perform such then mixed drop wise to the above solution until a pH value
measurement is to use a sensor array coupled with a pattern clas- reached 7.0. The solution was then stirred at 80  C for 1 h. Sol for
sification system [18e20]. The use of multiple sensors with an ZnOeSnO2 sensor is prepared by mixing appropriate amount of
appropriately modeled pattern classifier is therefore expected to zinc acetate dehydrate (Zn(CH3COO)2$2H2O) and stannic chloride
improve the reliability in the recognition of specific concentration (SnCl4$5H2O) with PVA. 1.0 M NaOH solution was used as reducing
of gaseous components. This will also improve the selectivity for a agent until pH of the solution becomes 7.0. The final solution was
particular gas when there is a mixture of gases. stirred at 110e120  C for 1 h. Finally, the resulting precursors were
Various pattern analysis methods like principle component spin-casted on the cleaned <100> oriented Si/SiO2 substrates fol-
analysis (PCA) [21], partial least square analysis (PLS) [22], and lowed by annealing at 550  C for 30 min in a tube furnace.
artificial neural network [23] etc. can be used with gas sensor arrays
for the classification and identification problem. Among these 3. Measurement techniques
methods artificial neural network is reported to provide superior
performance when quantification or multicomponent mixture A total of six numbers of sensors were used for the collection of
classification is required [24]. Multilayer perceptron (MLP) and data generated from the sensors when exposed to three different
radial basis function (RBF) are the two commonly used neural gases namely hydrogen, methane and carbon monoxide. The sen-
network algorithms used for pattern recognition. However, the sors were exposed to each test gas in different concentrations (0.1,
neuron connectivity in RBF is comparatively lower than MLP. This is 0.3, 0.5 and 1.0%) separately. The sensor types and their operating
the reason why the mean square error of an RBF network is less conditions are given in Table 1. The detail arrangement of the
compared to an MLP one having the same number of neurons. sensor measurement set up and sensor structure were reported
Therefore the parameters for tuning the network are higher in MLP. elsewhere [29,30]. Typically, the sensors were placed inside a
MLP with nonlinear transfer function, like sigmoid function, allow closed test chamber with suitable arrangement for gas inlet and
the network to learn any inputeoutput relationship adjusting the outlet. Measured amount of test gas was fed to the test chamber
weights and biases in the network by a gradient descent of tech- using Alicat® mass flow controllers (MFC). The test chamber was
nique known as back propagation of errors. Many authors have fitted with heating arrangement that would maintain a uniform
reported the successful utilization of ANN in many applications temperature (with an accuracy of ±3  C) inside the chamber. The
including pattern classification, identification, decision making etc. sensors were designed to operate in a resistive mode and Fig. 1
[25e28]. Multilayer perceptron neural network have been used by shows a model of the sensor measuring circuit. PdeAg contact
Joo et al. to identify breast nodule malignancy using sonographic electrodes were made on the top of the sensing layer by e-beam
images [26]. Lv et al. reported the detection of low concentration of evaporation technique in order to provide electrical connection. An
formaldehyde in binary gas mixtures using micro gas sensor array electrometer (Agilent U1253B) was used to monitor the variation of
and a neural network [27]. Lee et al. reported about a combustible sensor resistance. The resistance variation of the sensor is con-
gas recognition system including sensor array and neural network verted into voltage output by the measurement circuit.
based pattern recognition [28].
Most of the commercially available gas recognition systems are
PC based and hence are bulky. Embedded systems can be developed 4. Design of ANN in matlab®
with a suitable training function which can automatically read the
sensor input from the sensor array and produce the neural network A feed forward multilayered neural network (Fig. 2) trained by a
output. This may overcome the drawback of PC based gas pattern gradient descent technique, also called back propagation of errors,
recognizer, making them portable and convenient to the user. In was used to process the data arising from the sensors to investigate
this work, we report the development of a prototype toxic gas the feasibility of discrimination of gases. The network was designed
recognizer using sensor array and multilayer neural network. The in the Neural Network toolbox in MATLAB® with six input neuron
sensors were based on pure ZnO nano-rods and ZnOeSnO2 com- equal to the number of sensors used, two hidden layers with ten
posites which were fabricated in the lab. The sensors were exposed and twelve neurons in the hidden layer 1 and 2, respectively, and
to H2, CH4 and CO in different concentration ranges. The data thirteen output nodes corresponding to a specific concentration of
generated from the sensors were used to train a multilayer neural a specific gas, as shown in Table 2. Sigmoid function was used as the
network with back propagation learning algorithm, which can activation function for the hidden and the output neurons. Training
reasonably produce output to unseen input data. A process flow of the network was performed using supervised back propagation
chart for realization of the ANN in microcontroller is also formu- learning algorithm which was first initialized with random weights
lated and verified by downloading the network in the microcon- and biases. During the training process, weights and biases of the
troller. The use of an array of sensors instead of one or two along network were iteratively adjusted in order to minimize the
with a suitably trained neural network can increase the reliability of
the measurement.
Table 1
Sensor type and operation temperature.
2. Sensor fabrication
Sensor Sensing material Operating temperature ( C)

The sensor used in the experiment consists of pure oxide of zinc S1 ZnO 150
as well as composite oxide of zinc and tin, as the active gas sensing S2 200
S3 250
element. For the fabrication of sensors separate sols were prepared
for pure ZnO and composite ZnOeSnO2 with polyvinyl (PVA) as S4 ZnOeSnO2 150
capping agent. The detail material synthesis and methodical char- S5 200
S6 250
acterization of the sensor materials were reported in our previous
B. Mondal et al. / Engineering Science and Technology, an International Journal 18 (2015) 229e234 231

Table 2
Test gas and sensors designated output.

Test gas Concentration (%) Designated output

No gas 1000000000000

H2 0.1 0100000000000
0.3 0010000000000
0.5 0001000000000
1 0000100000000

CH4 0.1 0000010000000


0.3 0000001000000
0.5 0000000100000
1 0000000010000
Fig. 1. Schematic model of the circuit diagram. CO 0.1 0000000001000
0.3 0000000000100
0.5 0000000000010
performance function of the network. The default performance 1 0000000000001
function for feed-forward networks is mean square error (MSE),
which is the average squared error between the network output
and the target output and is defined as [31], 4.2. Optimization of activation function

1 XN
Two sigmoid (Logsig and tansig) and one linear (pureline)
MSE ¼ ðT  Yi Þ2 (1)
N i¼1 i activation function were studied in this work. These three functions
are defined in eq. (2)e(4) [35]. A set of 27 combinations of these
where T is the target and Y is the network output. activation functions, as shown in Table 3, for the two hidden and
In this study 260 data samples were used out of which 70% data one output layer are investigated for achieving best network per-
were used as training data, 20% as validation and 10% as testing formance. The network performance for the various combinations
data. The performance of a feed forward MLP neural network is of these functions is presented in Fig. 4. For the given set of data one
significantly affected by the network parameters like number of can observe from Fig. 4 that the network gave the best performance
hidden layers, number of neurons in each hidden layer, training when ‘logsig’ activation function is used for both the hidden layers
style and activation function used. The weight matrix for the neu- and the output layer (corresponding to combination code 8 in
rons was initially chosen randomly and the training algorithm used Table 3)
was Resilent Backpropagation (RP).
1
LogsigðnÞ ¼   (2)
1 þ en
4.1. Optimization of neural network structure
2
TansigðnÞ ¼ 1 (3)
MLP with a single hidden layer and nonlinear transfer function 1 þ e2n
like sigmoid function can learn any non-linear relationship. How-
ever, it has been reported earlier by various authors that the
addition of a second hidden layer improves the efficiency of the PurelinðnÞ ¼ n (4)
network to a great extent and also drastically reduces the total
number of hidden neurons [32e34]. A network with two hidden
layers was chosen in the present case and the number of neurons in 5. Implementation of ANN in microcontroller
each layer is varied in search of best performance. The network
gave the lowest MSE (0.005) when the number of neurons in hid- The optimized ANN is implemented in an Arduino due micro-
den layer 1 and layer 2 was ten and twelve, respectively. Fig. 3 plots controller board based on the Atmel (SAM3X8E ARM Cortex-M3
the MSE of the network for different combination of neurons in the CPU) 32-bit ARM core microcontroller. It has 54 digital input/
two hidden layers. output pins, 12 analog inputs, a 84 MHz clock, 2 DAC (digital to

Fig. 2. Structure of neural network.


232 B. Mondal et al. / Engineering Science and Technology, an International Journal 18 (2015) 229e234

Fig. 3. Optimization of number of neurons in the two hidden layers.

Fig. 4. Network performance for various combination of activation function.


analog), 96 Kbytes of SRAM and 512 Kbytes of flash memory and
can be powered by a USB connector or with an external power
supply. The weight and bias matrices are obtained after training the
The required data for implementing the ANN in microcontroller network in MATLAB® environment. For the network under study
are the weight matrix, biases and mean and standard deviation of (six input neuron, ten and twelve neuron in hidden layer one and
the input data set. The mean and standard deviation of the input two respectively and thirteen output neuron), we have [10  6]
data are required for data normalization. The input data are weight matrix for the first hidden layer, [12  10] weight matrix for
normalized using the following relation [36] the second hidden layer and [13  12] weight matrix for the output
layer. In addition, we also have three bias matrices for the two
hidden layers and one output layer.
Xn ¼ ðXi  Mi Þ=Sd (5) The process flow chart for the implementation of the ANN in
microcontroller is shown in Fig. 5. The weights and biases of the
In this equation Xn is the normalized data, Xi is the input data and trained network connections were first stored in the microcon-
Mi, Sd are mean and standard deviation of the given set of data. troller memory. The output of the first hidden neurons is then
computed using the following expression (6)e(8),

Table 3
X
n
Combination of activation function. Pj ¼ flogsig Wji $Xi þ bj (6)
Activation function Activation function i¼1
combination code
First hidden layer Second hidden layer Output layer
where i ¼ 1e6 is the number of input nodes and j ¼ 1e10 is the
1 Purelin Purelin Purelin number of neurons in the first hidden layer.
2 Purelin Purelin Logsig
The output of the second hidden layer is computed using the
3 Purelin Purelin Tansig
4 Purelin Logsig Purelin following expression
5 Purelin Tansig Purelin
6 Logsig Purelin Purelin
7 Tansig Purelin Purelin X
n
8 Logsig Logsig Logsig Qk ¼ flogsig Wkj $Pj þ bk (7)
9 Logsig Logsig Purelin j¼1
10 Logsig Logsig Tansig
11 Logsig Purelin Logsig
where k ¼ 1e12, is the number of neurons in the second hidden
12 Logsig Tansig Logsig
13 Purelin Logsig Logsig
layer.
14 Tansig Logsig Logsig And finally the output of the output neurons is computed using
15 Tansig Tansig Purelin the following expression
16 Tansig Tansig Logsig
17 Tansig Purelin Tansig
18 Tansig Logsig Tansig X
n
19 Purelin Tansig Tansig Ol ¼ flogsig Wlk $Qk þ bl (8)
20 Logsig Tansig Tansig
k¼1
21 Logsig Tansig Purelin
22 Logsig Purelin Tansig
23 Tansig Logsig Purelin where l ¼ 1e13, is the number of output neurons.
24 Tansig Purelin Logsig This course is coded in Arduino software environment “Arduino
25 Purelin Logsig Tansig 1.5.2” based on Cþþ programming language. The code is then
26 Purelin Tansig Purelin converted into a HEX file before downloading into the
27 Tansig Tansig Tansig
microcontroller.
B. Mondal et al. / Engineering Science and Technology, an International Journal 18 (2015) 229e234 233

Fig. 5. Flowchart for ANN implementation.

Fig. 6. Regression values for training, validation and test.


234 B. Mondal et al. / Engineering Science and Technology, an International Journal 18 (2015) 229e234

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