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**ARRAY OF TIN OXIDE GAS SENSORS TO DETECT CARBON MONOXIDE A N D METHANE.
**

P. Van Geloven, M. Honore, J. Roggen, R. Mertens

IMEC (Inter Universitary Microelectronics Center) Kapeldreef 75 B-3001 Heverlee Belgium tel.: 16/281211 fax.:16/229400 wants to measure. A possible solution to this problem might be the use of arrays of sensors with partially overlapping sensitivities. Algorithms then have to be developed to extract the desired quantities from the responses of the sensors of the array. Once these algoritms are obtained, they should be implemented in harware or software. Especially in gas sensing systems, the problem of selectivity is hard to overcome. The reason is that in most applications, a large number of interfering substances, such as other gases, are present. The algorithm and the electronic circuits described here, were originally developed to improve the selectivity of an array of tin oxide gas sensors. Their applicability is however not limited to the use in combination with tin oxide gas sensors. The interfacing circuits are well suited to decrease the influence of interfering substances (e.g. ambient humidity in gas sensing systems) through the use of heterogeneous sensor arrays. One sensor should be added to the array for each additional interfering substance that one wants to eliminate. Moreover, no extra effort is required if one wants to measure the interfering substance quantitatively. Consequently, if one wants to eliminate the influence of relative humidity on an array of gas sensors, one also obtains an additional output signal, namely the relative humidity itself. The only requirement for the additional sensor is that it is sensitive to the interfering substance. It is not necessary that the additional sensor only responds to the interfering substance, i.e. selectivity with respect to the interfering substance is not required. Drift of the charwteristics of sensors is a serious problem. A prerequisite of the sensors is that their drift with respect to time is known. If this is not the case, drift problems can only be solved by means of short term recalibration. As stated before, the algorithm described here is able to eliminate the influence of an interfering substance (e.g. the influence of humidity on a gas sensor system). It can be demonstrated that drift of sensors, can be considered as an additional interfering substance. Building an integrated sensor system with tin oxide gas sensors involves the solution of two basic problems. The first problem is that one has to select a proper array of gas sensors. This set of sensors should theoretically allow the simultaneous detection of the gases present in a mixture. This requirement imposes restrictions on the specifications of the individual sensors as well as on the number of sensors that is required. In order to detect

Abstract

Tin oxide gas sensors are widely used to detect explosive and toxic gases in domestic and industrial environments. With respect to these applications, there is a need for sensors having better performances. Especially if the sensors are submitted to real life conditions, the response of tin oxide sensors becomes ambiguous due to the presence of ambient water vapour. Besides the problem of selectivity, there is the problem of non-linearity of the electrical conductivity of tin oxide gas sensors with respect to the gas concentration to be measured. Finally, drift of tin oxide gas sensors is a problem which has not been overcome yet. The interface described in this paper results in a spectacular improvement of the selectivity of an array of tin oxide gas sensors. In contrast with pattern recognition techniques, where it is difficult to predict concentrations of gases, it becomes possible not only to predict the gases present in a mixture, but also to determine their concentrations. The output signals of the interface vary linearly with the gas concentrations to be measured. The interface also enables to solve the problem of drift. The only requirement is that the drift of the characteristics of the sensor as a function of time are known. The described sensor system, i.e. sensor array plus interface electronics, is cheap, easy to produce, has a low power consumption, can determine the concentration of each gas in a gas mixture. The complexity of the system, i.e. sensor array plus interfacing circuits, increases like n" with n the number of gases in the mixture to be analysed and 1 < a < 2. The use of the algorithms and the circuits to implement these algorithms is not limited to the use in combination with tin oxide gas sensors. They can also be used to measure mechanical quantities, biochemical quantities, etc. A prototype is built for the detection of carbon monoxide and methane concentrations in mixtures of these gases and in the presence of ambient humidity. The first output signal varies linearly with the carbon monoxide concentration. The second one varies linearly with the methane concentration.

Introduction

It is well known that it is very difficult to meet industrial selectivity specifications if only one single sensor is being used. This is true for almost every sensor application. The reason is that single sensors often are not selective enough to the quantity one

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a more elegant method will be discussed here.g. The DDC algorithm converts the measured data.. the first stage operational amplifier is followed by a diode-resistor network. g2. For the network of figure 2b. with the electrical conductivity in pure air..PL.. Pj is the concentration of gas j in the gas mixture and fk is a function that expresses the electrical conductivity of sensor k as a function of the gases present in the gas mixture. If the conductivity U of the sensor varies as : Figure 1 : Experimental results. resulting in an output signal that is directly proportional to the gas concentration to be measured.P.. If ordinary diodes are used. able to implement the functions g.P..J.. The output of this diode network is connected to a virtual ground.7 volts.Pz. concmtr. one needs at least n different sensors. By adjusting the values of the resistors RI. The second problem is to implement these functions in an electronic interface. n.. In this paper. The first stage operational amplifier converts the electrical conductivity of the sensor to an output voltage...the concentration of n gases.&.) (1) where U. 6 1 Diode converters Figure 2b is an illustration of a general interface for tin oxide gas sensors resulting in an output signal that varies linearly with the gas concentration to be measured. It is a two dimensional experimental result. the restriction is that the input voltage should be negative and that the output current should be a monotonously decreasing function of U. The result of solving the set of equations is that one obtains n functions g. it is possible to realize an output current that is a function of the input voltage. In figure 2b... g‘. 1 6 o . as a function of “1 .) in order to obtain the concentration [CO] and [CHI].... the gas concentration to be measured and a and b constants. Figure 2c represents the case if non-ideal diodes are used. P. is the conductivity of sensor number i. it remains possible to realize the desired function by adjusting the resistors..P.J = fdPI 1 P2.6. electronic circuits. then we can use the first stage amplifier of figure 2b to convert the electrical conductivity U to an input voltage of the diode network that is If directly proportional to -(Pz)”. The output of the DDC algorithm is implemented by means of diode converter networks ( 1 1 .l) = f2(P. namely the input of the last stage operational amplifier. Figure 2a represents the output current of the diode converter circuit for ideal diodes.P2. This is illustrated in figure 2c. will be discussed. If the voltage references (diodes in figure 2b) are non-ideal voltage references. *r CO and cn.lu. Once an adequate set of sensors has been choosen. = fl(Pl...P. the reference voltage is more or less 0. Figure 1 is an illustration of an integrated sensor system built according to this strategy.rd ..I runctlon c k qrnrnr 1 runrim CO and cn. giving the concentration P. obtained from a prototype.R2. The range of this voltage can be adjusted by means of trimming resistors to the range of 0 to -10 volts for example. we now realize the function : i d = (U*$ (3) 323 .(P. .. Figure 2a illustrates the principle of operation if ideal diodes are used.twn soncmtrrtion JO C rc1 Dum Sensor2 IO C rc1 hum 1 DDC 1 algorithm Figure 2 : Interface circuit. The diodes have to be seen as voltage references.. Instead of solving the set of equations analytically. one has to solve the following set of non linear equations for P I .....) 6 2 63 V#L = f.*..

) arbitrary functions f can be realired : iorl realized or approximated. can also be stored in a digital computer. In this way. The response of an array of 3 sensors can be treated as depicted in figure 4. U ~ etc. The last two elements of the vector are the signal of sensor 1 and sensor 2. The output of the acnaom is converted to three gw concentrations (Concentration 1 to 3). = f(ui. The functions g. If we take the concentration of gas 1 together with the two sensor signals out of a vector. In other words. In fact the diode networks oncentration 2 p2 oncentration 1 1 1 Figure 4 :Example of an array of three sensors. then we obtain 100 vectors.Q3) 2 s = 93(Q1. arbitrary functions can be connected to the first stage amplifiers of figure 4. the diode network can be used as a linearizing network. In figure 5 we measure the leftmost graphs and we want to obtain the two rightmost graphs. In other words: Let us consider a two dimensional array of gas sensors.Qz.~ with the diode network. The function P I M a function of U I and u2. then we obtain one point and similarly. ( A n extension to n gases is straight forward. If we measure the response of the two sensors to 100 gas mixtures. Measured graphs Desired graphs Fuure 6 : The Direct Data Conversion algorithm (DDC). one obtains a four dimensional vector for each gas mixture that flows over the two sensors. The restrictions that the input voltage should be negative and that the function should be a monotonous decreasing function. This graph can be constructed directly by means of the set of vectors. and if we plot this point. (See the upper right graph in figure 5: this is the solution of the non linear set of equations for PI). With this circuit. This remains true if cross terms like ( Q . is a graph expressing the concentration of gas 1 as a function of the two sensor signals. 324 I I r III I 7 7' li I i I I 1 . One can prove that the complexity of an optimized interface circuit increases with n" with n the number of gases to be detected and l < Q < 2.and the function Pz M a function of u and u l 2 can be deduced directly from the two measured functions. If fact. Q3) (5) The functions 91. What we are interested in. then one obtains two graphs. the concentration PIof gas 1 is a function g1 of the responses of the three sensors. then the output voltage of the last stage amplifier is directly proportional to Pv. The first two elements of the vector are the concentration of gas 1 and gas 2. g2 and gJ can be realized by means of diode networks of figure 3. The first one gives the response of sensor 1 as a function of the two gas concentrations and the second graph gives the response of sensor 2 as a function of the two gas concentrations. are present in the functions gi. partially overlap. The diode network of figure 2b can be extended to networks represented in figure 3. If one measures the response of two sensors as a function of two gases. The direct data conversion algorithm (DDC) 1 4 Figpre 3 : Extension of the diode network of figure 2b.Q2. can be omitted now. This is illustrated in figure 5. the leftmost graphs represent the non linear set of two equations with two unknown values (namely the independent variables PI and Pi). ) ' . Each of them concentrations represents the concentration of one gss i the g~ mixture to n be analysed. In fact. we can write for the other concentrations of figure 4: p = 9Z(QL.) In general.

In the same way we can construct the graph expressing the concentration of gas 2 as a function of the two sensor signals. . The complexity of the electronic part is proportional to n" with n the number of gases to be detected and 1 < CY < 2.]. The influence of drift of the sensors can be eliminated. Two tin oxide gas sensors are used t o detect concentrations of carbon monoxide and methane in mixtures of these gases. As in figure 5 . namely a time sensor (i. . Figure 1 is a two dimensional experimental example. namely the output of the gas sensor U and the output of the time sensor t . In fact. is the time as measured by the time sensor. C H I and H z O . as measured by the TO Sensor 1 TPi Time t \ Ls Conclusion It has been demonstrated that the DDC algorithm in combination with diode converter networks provides an easy way to build n dimensional sensor systems. able to detect the concentrations of n gases. Doing the same with the other vectors results in additional points in the desired graph. the characteristics of which drift with time. and the second one at 480 degrees C. usually is independent of the gas concentration P. is not limited to the use of tin oxide gas sensors. This procedure of constructing the desired graphs from a set of vectors is called the Direct Data Conversion algorithm (DDC). The concentration of CO varies between 0 and 300 ppm. output of the system will The provide the concentration of CO. the requirement for the two sensors is that they are independent of each other.u2. Drift of the characteristics of sensors Let us consider a one dimensional case. This is not a disadvantage compared with the analytical solution of the set of equations. This example can be extended to n dimensional arrays of sensors. The only requirement for the sensors is that they form a set of independent sensors.5%. for both sensors. we can plot the gas concentration P. The symbol t in figure 6 is the time. they can be implemented by means of diode converter circuits. PI is the gas concentration to be measured. It is evident that the real time is independent of the sensor signal U.of the desired graph. it provides a way to solve the set of non linear equations ( I ) in a discrete number of points. and the sensor output signal U. Let us for illustrative purposes assume that the sensitivity of the sensor to gas PI decreases with time.e. as a function of the two sensor signals t . This is accomplished by using a different operating temperature for each sensor. ([CO].. The first sensor operates at 400 degrees C. Suppose we have a gas sensor. (Quartz crystals do not suffer from gases). namely the real time as a function of the measured time t . Relative humidity is kept constant at 50 % at ambient temperature. As already stated before.u. we can construct a set of four-dimensional vectors. and U. Using the set of vectors. the measured time t . The upper left graph of figure 6 represents the drift characteristics of the sensor.[CH. If one wants to eliminate the influence of water vapour. a clock). The second output of the system is the value of the interfering variable. This results in different sensitivities for CO and C H . t is the real time and t . time sensor.[HzO). U is the response of the gas sensor. applied to eliminate the influence of drift.). Moreover. Desired graphs Time t Measured graphs tS Figure 6 : The Direct Data Conversion algorithm (DDC). this method to construct sensing systems. then we would have to approximate the obtained functions in a discrete number of points if we implement the functions with the diode converter circuits. 325 . then water can be considered as a third gas. If we now add a second sensor to the system. even if we would be able to obtain an analytical solution. Compare this figure with figure 5 . because. The only requirement for this method is that the sensors are independent of each other. namely the time t . The concentration of CHI varies between 0 and 0.uI. As depicted in the lower left graph of figure 6. A third sensor has to be used in that case. The first two elements of each vector are the real time t and the gas concentration P . Realization of a sensor system Once the desired functions are obtained with the DDC algorithm. The last two elements are the outputs of the sensors. The DDC algorithm then has t o be applied to a set of vectors each of which will have 6 elements. then we obtain an additional sensor signal.

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