Sensitivity Analysis of a 500 W Proton Exchange Membrane Fuel Cell Stack by Design of experiments

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In this paper, the influences on fuel cell performance of gas pressure and flow rate parameters are studied. The fuel cell is operated at various pressure and gas flow rates are regulated by mass flow controllers placed upstream of the stack. In this study, four types of control factors considered are pressures of the fuel and oxidant and the flow rates of the fuel and oxidant to select the optimized conditions for fuel cell operation. Each factor has two levels, leading a full factorial design requiring 24 experiments leading to 16 experiments and fractional factorial experiments, 24-1, leading to 8 experiments. The experimental data collected were analyzed by statistical sensitivity analysis by checking the effect of one variable parameter on the other. The mixed interaction between the factors was also considered along with main interaction to explain the model developed using the design of experiments. From the analysis maximum fuel cell performance was found to be hydrogen flow rate, oxygen flow rate and the interaction between the hydrogen pressure and oxygen flow rate compared to all other factors and their interactions. These fractional factorial experiments, presently applied to fuel cell systems, can be extended to other ranges and factors with various levels, with a goal to minimize the variation caused by various factors that influence the fuel cell performance but with less number of trials compared to full factorial experiments.

Keywords: PEMFC, statistical analysis, ANOVA, factorial design, stack.

1. Introduction: Polymer electrolyte membrane fuel cell (PEMFC) is the most promising system among several different kinds of fuel cells due to their various advantages such as easy start-up, room temperature operation, no liquid electrolyte, and high current density. To achieve high current density, the optimal operating conditions need to be identified for fuel cell systems in addition to design parameters such as membrane, catalyst particle size, quantity, and nature of gas diffusion layers. There are many variables in the operation of fuel cell systems, viz., fuel cell temperature, reactant pressure, reactant flow, relative humidity, and load. These parameters are related among themselves to nonlinear relations, leading to an impact on the fuel cell voltage [1, 4]. This is concerned with minimizing the effect of uncertainty or variation in design parameters on a design without eliminating the source of the uncertainty or variation. The robust design is less sensitive to variation in uncontrollable design parameters than the traditional optimal designs. Robust design has found many successful applications in engineering and is presently expanded to fuel cell systems with a goal to minimize the variation caused by uncontrollable noise factors such as ambient temperature, operating environment, and natural phenomena that are difficult to control [5-8]. The robust design can also help to minimize the caused by control factors such as pressure, flow rate and humidity. Improvement of power and stabilization of cell performance under different operating conditions are important for developing a practical PEMFC system. In general these desirable parameters combinations were decided by one factor experiments and the analysis is done by fixing the other parameters, where the influence of other parameters is not considered. In addition, a large number of experiments are needed to analyze the performances of a given fuel cell system are to identify the parameters of a physical model. In order to evaluate the impacts of the physical control parameters on the fuel cell operation, the design of experiment (DOE) method, developed by Fisher [9, 10], is being used, in particular, to reduce the number of tests when many parameters were considered.

Recently, this method is being used by many researchers in fuel cell technology for the development of fuel cells, materials for fuel cells, and optimal solution for operating conditions, which determine the most significant parameters [11-14]. Grujicic et al. [15] studied the cathode and optimized the distributor geometry by analysis of variance (ANOVA) method. The effect of material and manufacturing variations on membrane electrode assembly pressure distribution has been analyzed by Vlahanos et al. [16]. The experimental analysis of combined heat and power performance of a PEMFC stack of 800 w capacity has been studied by factorial design method and showed that cathode stoichiometry has a positive effect on electrical power and negative effect on thermal power [17]. In another detailed study by Guvelioglu and Stenger [18], the main and interaction effects of PEMFC design parameters have been studied with five factors such as channel width, GDL thickness, GDL conductivity, and GDL porosity. They found that the strongest interaction occur between the channel size and the GDL conductivity, while the weakest interaction effects are observed between the GDL thickness and the porosity. 2. Experimental 2.1 Experimental setup: The Proton Exchange Membrane Fuel Cell (PEMFC) stack was developed at the GASHUB, Singapore by making use of 20 membrane electrode assemblies [MEAs] made by a proprietary process and graphite plates with triple serpentine channel geometry. The MEAs were made using a treated Toray paper as a gas diffusion electrode and 20% Pt/C as electro catalysts for both anode and cathode and NafionTM membrane 111 from DuPont denomour as an electrolyte. The area of each electrode was found to be 100 cm2. The coolant circuit was also introduced in the system manifold for the removal of heat. The heat developed by the stack is removed by the water cooled system. The details of the stack are given in table 1. 2.2 Test station: The PEMFC test bench, used for the cell management, was developed by K-Pas Instronic Engineers, Chennai which has partially designed in our laboratory. Table 1 Technical specifications of fuel cell Number of cells 20

Cell area(cm2) Operating temperature(0C) Operating pressure Media inlet: Cathode Anode cooling

100 30 max. 3 bar

humidified oxygen humidified hydrogen Demineralised water

The apparatus consists of gas flow control systems, temperature control, pressure control and humidifier systems, electronic-load bank, milliohm meter for the resistance measurement and a icomputerized data acquisition system. All the settings of the test bench concerning gas flow, temperature, humidity and gas pressure were controlled through the data acquisition system connected to the computer. Fig. 1 presents a schematic diagram of the experimental apparatus. Hydrogen in the anode side and oxygen or air in the cathode side was provided from a pack of pressurised gas tanks. The fuel gas flow rates were regulated with electronic thermal mass flow controllers. Both the anode and cathode fuel gases were humidified by forcing the gas through a gasliquid equilibrium stage. In order to maintain uniform cell and humidifiers temperatures, three heaters driven with a National Instruments Field Point controller were used. The temperatures of the cell, the anode and of the cathode humidifiers were measured through three thermocouples. Furthermore, two thermocouples were also located near the gas inlet lines. The electric load bank was a semiconductor device that allows high currents to be drawn at low voltages. The load was air-cooled and rated at 2000W. A digital AC milliohm meter was placed in parallel both to the electric load and the fuel cell. This device provided a quick and accurate measurement of the total impedance magnitude of the cell and the load at a specific frequency. The ohmic resistance of the cell can be extracted after correction of the impedance of the load. During the fuel cell operation, the wet gases were fed to the fuel cell and then diffused to the MEA through the gas diffusion layers (GDLs) while circulating in the gas channel. The un-reacted gases and the water produced during the electrochemical reactions were released from the fuel cell. The exhausted gases pass through the backpressure regulators and then exit through the vent. A personal computer running Windows XP2000 and a Scadabased software with a variety control, data logging

and displaying features were employed for the experimental monitoring and controlling. Table 2 Measurement ranges and accuracy of measurement devices of test facility

Measurement devices
(Make:K-Pas Instronic Engineers) Power station electronic load

Measurement accuracy

range

and

Input:230v, AC50Hz Voltage: 0-100ADC Capacity:2000Watts Features: 3 Digital meter for volts19.99volts 4 Digital meter for Amps19.999 Amps Control range: 2100% of full scale Accuracy: 1 % of full scale Temperature controller with sensors Range:0-1000C Operating voltage: 230v AC Type of thermocouple : J Type

Flow measuring device (Mass flow controller) PID controller

Figure 1 Diagram of Experimental Apparatus for the PEMFC Testing

Figure 2 Experimental setup of fuel cell test station Range of parameters studied in the experiments: In this study considered the effect of four variables, pressures of the fuel (H2), pressure of oxygen (O2), flow rate of the fuel and flow rate of the oxidant. Levels Factors A : hydrogen pressure (bar) B: oxygen pressure (bar) C: hydrogen flow rate(lpm) D: oxygen flow rate (lpm) Low 1.7 2.15 0.88 0.95 High 2.15 2.78 1.81 1.91

These variables are studied an objective to select the optimized conditions for fuel cell operation. For each variable experiment were conducted at lower and

higher levels (two levels). A full factorial design required 2n experiments, where 2 is the level of the variable and n is the number of variables considered, leads to 16 experiments and the fractional factorial experiments, 24-1, leading to 8 experiments. The range of parameters is listed in Table 3. Table 3 The range of parameters studied in the experiment 2.2. Experimental procedure: The 500 W Proton Exchange membrane Fuel cell stack was connected to the power station and the gas connections were given to the stack. Test station was turned on and gas lines were opened. Before starting the process Fuel cell was purged with Nitrogen gas to remove any impurities in the stack. Initially from the literature and by conducting the preliminary tests the variable levels were found as, the fuel (H2) pressure range 1.702.15 bar, oxidant (O2) in the pressure range 2.15 2.78 bar, the fuel (H2) flow rate is ranging from 0.88 to 1.81 lpm and flow rate of oxidant (O2) ranging from 0.95 to 1.91 lpm. These four factors were considered at two levels i.e... Low level and high level, like wise 16 experiments were conducted and temperature of stack was maintained at 300c. After continuous operation of stack by supplying fuel and oxidant at given levels, open circuit voltage (OCV) was reached to 18 volts without load for about 1 hr. When we draw the load as a current mode by step by step for given current set point for the given ranges of flow rates and pressures of fuel and oxidant. It was observed that, when current increases the voltage decrease proportionally and increase the power. To maintain the temperature at 300C heat was removed by water circulation system showed in figure 2. When it reached the minimum voltage 10 volts, it was trip off and the load was off. Like wise 16 experiments were carried out to maximize the performance of fuel cell stack. Experimental data was analyzed by using design of experiment technique - full factorial design and fractional factorial design methods. 2.3 Design of Experiments. The design of Experiments (DOE) method has been adapted to achieve the objectives by setting the limits for the pressure and flow rate for the reactants. The influence of these parameters on the fuel cell is critical. For the method of factorial design the experiments were conducted for four variables at two different levels. The four factors are fuel pressure, fuel flow rate, oxidant pressure, and oxidant flow rate. The DOE experiments were conducted for

the fuel (H2) pressure range 1.702.15 bar, oxidant (O2) pressure range 2.15 2.78 bar, the fuel (H 2) flow rate range from 0.88 to 1.81 lpm and flow rate of oxidant (O2) range from 0.95 to 1.91 lpm. The observations were made at all the combinations of 24 experiments that can be formed for different levels of the factors, called treatment combinations. The factors that were set at the low level, indicated as (1) and those at the high level as (+1). The particular combination of treatments was made using the Yates notation. In the fractional factorial method, the number of observations was reduced to 241 (eight) treatment combinations. The response of the observations was power (watts) with factors such as reactant pressure and flow rate at two different levels.

3. RESULTS AND DISCUSSIONS The fuel cell stack of 500 W capacities was presented with humidified reactants (hydrogen and Oxygen) at the open circuit potential for about 1 hr. The stack was operating when the stack was reached the open circuit voltage as 18 volts. Load was turned on with increase of current step by step for 30mts and subsequently voltage was decreased with increasing the power. The polarization data were collected for the stack at the stack temperature of 300C. The current voltage characteristics of 500W stack are shown in figure 1 at a hydrogen operating pressure of 2.15 bar with 1.9Lpm. From the figure one can see that the stack can deliver a power of around 205 W with oxygen. The full factorial and fractional factorial design of experiments are conducted for a 500 W PEMFC stack.
19 Volatge VS Current density Power VS Current density 200 250

18

Voltage (Volts)

150 16 100 15 50

14

13 0 20 40 60 80 100
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0 120 140 160

Current density (mA/cm

Figure 3 current, voltage - power characteristics of the fuel stack at 300c, H2 flow = 1.81 lpm, O2 flow= 1.91 lpm 3.1 Full Factorial design:

Power (watts)

17

For the Design of experiments (DOE), the response considered here is the fuel cell power output as a function of pressure and flow rates of reactants (Hydrogen and Oxygen). Four types of control factors namely, the pressure of the Hydrogen, the pressure of the oxygen, the flow rate of the Hydrogen and the flow rate of the oxygen are considered to select the optimized conditions for fuel cell operation as given in table 3. The levels and factors were chosen by taking into account the limits of the fuel cell stack and also the test bench. However, the linearities for these factors and levels are considered in the specified range. The full factorial design for the four factors with various treatment combinations is shown in table 4. The Analysis Of Variance (ANOVA) is a commonly used tool to study and estimate the factor that influence the process. Initially, ANOVA is performed for the main effects, pressure of the Hydrogen (A), pressure of the oxygen (B), flow rate of the Hydrogen (C) and the flow rate of the oxygen (D). Then analysed for interaction effects of two factors like AB, AC, AD, BC, BD, CD, interaction effects of three factors, ABC, BCD, CDA, DAB and interaction effects of four factors, ABCD and analysis results are summed in table 5. Table 4. Full Factorial design format for four factors
S.NO. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 Hydrogen Pressure (A) 1.7 2.15 1.7 2.15 1.7 2.15 1.7 2.15 1.7 2.15 1.7 2.15 1.7 2.15 1.7 2.15 Oxyge Pressure Hydrogen oxygen Flow (B) Flow rate (C) rate (D) 2.15 2.15 2.78 2.78 2.15 2.15 2.78 2.78 2.15 2.15 2.78 2.78 2.15 2.15 2.78 2.78 0.88 0.88 0.88 0.88 1.81 1.81 1.81 1.81 0.88 0.88 0.88 0.88 1.81 1.81 1.81 1.81 0.95 0.95 0.95 0.95 0.95 0.95 0.95 0.95 1.91 1.91 1.91 1.91 1.91 1.91 1.91 1.91

called
220 200

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effects.

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Figure 4 Influence of Four Factors on Power(Y) Table 5 Analysis of variance for power including main and interaction effects for 24experiments

Degrees Sum of % of Mean Source Effect squares contribution Freedom Square A B C D 11.375517.5625 2.155707 -2.625 27.5625 0.114801 64.12516448.06 68.50807 14.875885.0625 3.686387 0.002343 1 1 1 1 1 1 1 1 1 1 5

517.56252.853746 0.152 27.5625 0.151975 0.712 16448.0690.69164 0

885.06254.880074 0.078 0.5625 0.003102 0.958 742.56254.094355 0.098 855.56254.7174170.0819 33.0625 0.182301 0.687 0.5625 0.003102 0.958 742.56254.094355 0.098 181.3625

AB -0.375 0.5625

AC 13.625742.5625 3.092858 AD 14.625855.5625 3.563516 BC -2.875 33.0625 0.137709 BD 0.375 0.5625 0.002343

CD 13.625742.5625 3.092858 Error 906.8125

The main eight effects of the four factors are shown in figure 4 for comparison

The four graphs represent the maximum power obtained from the 16 experiments as well as the average of these 16Y values and the average of the stack power, when the x factor is at two levels, namely, low and high. From these graphs we can observe that the factor with a greater slope is the most significant factor for getting maximum power.

It can be seen from the graphs that the slope of factor C, which is Hydrogen flow, is higher compared to all other factors and hence it is very significant on the cell performance. The most insignificant factor in this set of experiments is the oxygen pressure (B), as the graph is almost parallel to X axis. The contribution from each factor can be obtained from the ANOVA table as shown in table 5 representing the source of variability, degrees of freedom associated with each factor, sum of squares, and mean squares due to each factor. Fisher statistics shows the ratio of mean squares with the factor and the p value for the Fisher statistics. The p value determines whether the factor is statistically significant or not. Generally, the mean values are significant if the p value is less than 0.05. From the table 5 we can see that the C factor contribution is more around 68% and the next contributor is Oxygen flow rate (D) factor, which is around 4%. From the p value one can also find that the C factor is statistically significant, as it is less than 0.05. The model equation can be written as equation (3.1) shows the fitted parameters for the analysis of mean interactions. Hence the first order interactions effects were also considered and are tabulated in table 5. The average two factor interactive effects are shown in figure 5. It is observed that the interactive effects of Hydrogen pressure - Hydrogen flow (AC), Hydrogen pressure - oxygen flow (AD) and hydrogen flow - oxygen flow (CD) are significant compared to the other two factor interactive effects, AB, BC and BD.
A B in tera c tio n
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Figure 5 Interaction effects of four factors at two levels on the fuel cell stack Performance. Figure 6 (a) and 6 (b) shows the normal probability plots of the data collected i.e. effect and for residual respectively, considering both the main and interaction effects. It can be inferred from the above figures that the data follow the normal distribution and the interaction effects in the residual plots are random.

99.999 99.99 99.95 99.9 99.8

Normal %probability

99 98 95 90 80 70 50 30 20 10 5 2 1 0.5 0.2 0.1 0.05 0.01 0.001

BCD ABD ABCD ABC BD

ACD D AD CD

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(b) Figure 6(a) Normal probability plot of the effects of the 24

Factorial, 6 (b) Normal probability plot of Residuals

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From table 6 it can be observed that the average three factor interactive effect of Hydrogen pressure - Hydrogen flow - oxygen flow (ACD) is contribute 3.686 % and the remaining three factor interactive effects, ABC, ABD and BCD contribute less than 0.1%. Hence ACD effect will be significant

P rc n e et

compared to the remaining factors. The four factor interactive effect of Hydrogen pressure oxygen pressure - Hydrogen flow - oxygen flow (ABCD) is contributed 0.006508 %. Hence its effect is insignificant. Hence it can be concluded that the effect of C and D are significant compared to A and B. The ANOVA is also carried out by using MINITAB statistical software. The data developed from this MINITAB statistical software was presented in the figures 7, 8 and 9. The data collected for the fuel cell power response followed the normal distribution as shown in figure 7 (a) and the graphical summary shown in figure 7 (b). The box plot shows the pattern of variation in the experimental data and also shows that there are no outliers or extreme values or unusual observation. Table 6 Analysis of variance data for the factors A, C and D
% Degree s Of
Frequency

Probability Plot of power

Normal
99 Mean StDev N AD P-Value 1 52.4 3 7.56 16 1 .834 <0 .005

95 90 80 70 60 50 40 30 20 10 5

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Figure 7 (a) Probability plot of the fuel cell power (b) Box plot of the experimental data.
Residual Plots for power
Normal Probability Plot of residuals
99 90 50 10 1 -40 -20 0 Residual 20 40 -40 100 125 150 Fitted Value 175 200 Residual Percent 0 -20 20

residual versus Fitted values

Square

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Sum Of Contributio Freedo n Source Squares m A C D AC AD CD 517.5625 2.155707 16448.06 68.50807 885.0625 3.686387 742.5625 3.092858 855.5625 3.563516 742.5625 3.092858 1 1 1 1 1 1 1 8

Histogram of residuals

residual Versus Order of the data

20 0 -20 -40

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6.0 4.5

517.5625 49.58683 0.000108 16448.06 1575.862 0

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5 6

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Observation Order

885.0625 84.79641 0.000016 742.5625 71.14371 0.00003

Figure 8 Residual plots of the main and interaction effects of a 500W stack Figure 8 shows the residual, histogram, and probability plots of the data collected, considering both the main and interaction effects. It can be inferred from the figure that the data follow the normal distribution and the interaction effects in the residual plots are random. The graph effects using the ANOVA general linear model also show that the factors C and D are significant compared to A and B, as shown in Figure 9.

855.5625 81.97006 0.000018 742.5625 71.14371 0.00003

ACD 885.0625 3.686387 ERROR 83.5

885.0625 84.79641 0.000016 10.4375

Main Effects Plot for power

Data Means
A 180 165 150 135 B

20

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stack potential, Volts

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E erim ta xp en l E ctro e A a - 10 cm le d re 0 sta size = 20 ce ck lls K . D ath th ya e al. .S h a re n t E ctro e A a - 10 cm le d re 0

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Figure 10 Comparison of voltage current Characteristics of experimental data with K.S.Dhatatreyan et al. 4. Conclusions The Design of experiment methodology with its statistical techniques is then well-suited to analyse the tests conducted on Fuel cells. Indeed, the DOE methodology offers a wide range of practical tools, graphical representations and techniques that can be suitable mediums for FC experimenters and developers. The DOE approach leads to simple and precise models which highlight the impacts of the factors on the response and detect possible parameters. Factorial method C interactions+ between the 500W PEMFC stack for /*2( X ) * ( X3 ) ) has 1 been applied to statistical ) sensitivity analysis. The conditions for (3 .1 operating the stack with respect to pressure and flow rate of the reactants were identified by design of experiments method. The effects of interactions among the various factors at two different levels were also identified along with the major contributor by sensitivity analysis by statistical methods. From the experiments and statistical analysis method, it has been observed that Hydrogen flow plays a major role for getting the maximum performance from the fuel cell stack and this has got a physical significance in terms of water removal and un reacted nitrogen blanket removal from the reaction site. In the fractional factorial experiments the number of experiments was reduced, also showed the same results revealing that fractional factorial experiments can be applied for getting the major contributor among the various variables for fuel cell stack performance with respect to obtaining maximum power. It is also observed that the number of experiments can be reduced to evaluate the robustness of the stack with respect to operating conditions, thereby saving time and materials. It is also observed that the experimental design methodology is a suitable tool for the improvement of fuel cell systems.

120

. Figure 9 Main and interaction effects of the four factors at two levels on the fuel cell stack performance The model equation can be written after inclusion of interaction effects as

Y =

15 2 .4 3 7 5+ ( A / 2 ()X1 ) + ( C / 2 () X3 ) + ( D / 2 ()X4 ) + ( A * * * ( A D /*2 ()X1 ) * ( X4 )

Here estimated power is calculated from the model using three significant terms A, C and D. X1, X3 and X4 are levels of the factors A, C and D corresponding to experiments. This model accounts for 99.6% variation and also one can see that the main interaction contributor arises from the C and D factors, which are Flow rate of the Hydrogen and the flow rate of oxygen. Present experimental data of voltage current characteristics is compared with the experimental data of K.S.Dathatreyan et al. [19] and is shown in Figure 10. It shows the good agreement with the data of K.S.Dathatreyan et al. for the fuel cell stack with electrode area of 100 cm2 with 9 cell stack.

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