ECS Transactions, 58 (1) 1601-1611 (2013) 10.1149/05801.1601ecst ©The Electrochemical Society Pressure Drop and Voltage Response of PEMFC Operation under Transient Temperature and Loading Conditions Rupak Banerjee; Evan See; Satish G. Kandlikar Department of Mechanical Engineering, Rochester Institute of Technology 76 Lomb Memorial Drive, Rochester, New York – 14623 Transportation powertrains need to be versatile in power generation to meet the varying vehicular dynamic loads. The PEM fuel cell stacks within vehicles are therefore designed to meet this additional requirement under part-load and varying-load driving conditions. The size of the on-board energy storage systems can be reduced significantly if the fuel cell powertrain is able to generate the load faithfully in corresponding to the varying demand load. The voltage and pressure drop variations in response to changes in the temperature and load conditions are experimentally studied in the current investigation for characterizing the dynamic system behavior. Temperature of the cell was changed over 20°C - 80°C in short time periods (<600 seconds) and the load conditions were changed by 400 mA/cm2 in 300 seconds. It was observed that changes in load at lower temperatures have a significant impact on the pressure drop in the channels. Additionally, a rapid increase or decreases in temperature have an adverse effect on the cell performance. Rapid increase in cell temperature results in dehydration of the membrane, thereby reducing the performance; while rapidly decreasing the cell temperature may result in increased condensation. Introduction Proton Exchange Membrane Fuel Cells (PEMFCs) are seen as a viable replacement for IC engines for automotive transportation. The PEM fuel cell stack within vehicles often operates under part load and varying load conditions. Load conditions change based on the driving, and can be very dynamic in nature. Designing the PEMFC powertrain to follow the load faithfully would reduce the requirement for large energy storage systems on board the vehicle (1, 2). Uzunoglu and Alam (2) presented a solution to replace the large battery systems by designing a control system with an ultra-capacitor in conjunction with the fuel cell to meet the surge in power demand during acceleration of the vehicle. If the difference between power generation and power demand is small, the ultra-capacitors would be able to meet the power requirements. The ability of the fuel cell to closely match the power demand will thus reduce the power requirement from the capacitor during transients. Most studies reported in literature investigate and quantify the steady-state behavior of Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1601subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) fuel cells. Although the steady state behavior is important, automotive conditions are transient in nature and therefore a clear understanding of the transient response of PEM fuel cells needs to be developed. Very few experimental studies have been reported on the performance characterization under transient conditions. In this regard, pressure drop offers a good diagnostic tool for the two-phase flow in PEMFCs (3) with distinct pressure drop signatures for each flow regime (4, 5), and can be utilized for characterizing the transient performance. Hamelin et al. (6) used a Ballard fuel cell stack, and showed that the response time of load changes on the output voltage is less than one second. The theoretical time for the electrochemical cell to respond is about 10 µs. He et al. (7) used pressure drop to predict the flooding of electrodes and the porous media. They used interdigitated electrode configurations in their study. Lu et al. (4) also showed that the pressure drop could be used to identify flow patterns in the flow channels. Pressure drop is thus seen to be a good diagnostic tool in characterizing the PEM fuel cells. Wang and Wang (8) numerically investigated the transient effect of change in inlet relative humidity on the water transport in the channels, GDLs and the membrane. They varied the inlet humidification of both anode and cathode gas streams, and observed water saturation in the GDLs and the membrane. The drying effect was studied; a lag of about 20 seconds was reported for the membrane to dry. The anode side dried faster due to the high diffusivity of water in the anode GDL. Rabbani and Rokni (9) used a commercial fuel cell stack by Ballard Power Systems to investigate the effect of transients. They varied the load on the stack from 60A to 100A, effectively changing the current density from 0.21 A/cm2 to 0.35 A/cm2 in the process. They observed that the voltage response was very rapid, matching with their original hypothesis. However, the temperature increased due to the increased heat generation, which resulted in transient temperature profiles. The temperature fluctuated between 60°C and 70°C, and did not reach steady state even after 5 minutes. An increase in the load results in an increased heat generation within the cell. The coolant system is supposed to regulate the temperature, but the lag in response leads to this transient behavior. In a fuel cell vehicle, changing load conditions would affect the temperature of the stack, and may lead to a lag in the power delivery. A fuel cell starts at the ambient temperature, which varies from sub-freezing to midthirties in most regions. However, the optimal operating temperature for PEMFCs is between 60°C and 80°C (10 – 14). The stack needs to reach this optimal operating temperature range at the earliest to improve the efficiency as well as to meet the demand. Auxiliary heaters are used along with the coolant circulation to raise the temperature rapidly. In some cases, this causes a rapid change in temperature, which may also have an adverse effect on the cell performance. Rabbani and Rokni (9) noted that the heat generated in the cells also changes with the power output, and there is a time lag before the coolant is able to bring the temperature back to the desired steady state value. The gases entering the channels are partially humidified, while they are mostly saturated Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1602subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) towards the exit. Any rapid change in the temperature of the cell may result in unexpected condensation of liquid water in the gas channels resulting in an increased two-phase pressure drop, and a reduced performance of the cell. Also, the response from the stored water in the GDL is dependent on the local conditions before and during the transients. In the present work, the different conditions and cases discussed above are investigated. Each test is designed to simulate a specific case discussed above. Different load and temperature transients are imposed on the cell, and the response in terms of voltage as well as two-phase pressure drop in the channels is observed. Experimental Setup An in-situ setup is used for the current investigation into the transient effects of varying temperature and load conditions. A Greenlight Technology G40 fuel cell test stand is used to control the flow of reactants and the load conditions to the cell. The test stand is capable of controlling the flow rates, humidity, and gas temperature and is operated in stoichiometry mode. This ensures a constant stoichiometry to be maintained as the air flow is modulated according to the load being applied. The reactant supply line and dew point temperature are controlled independently for the hydrogen and air lines. Figure 1 shows the test setup with the different components outlined. Figure 1: In situ fuel cell setup showing the test stand, fuel cell, and the heated gas lines. The fuel cell is built and assembled in-house, and has an active area of 50 cm2. A Gore Membrane is used with MRC (Mitsubishi Rayon Corporation) 105 GDL on both sides. The GDLs have an MPL coating on one side. Although wavy channels have been used in the earlier steady state tests, Straight reactant channels are used in the present study to deliver the reactants to the cell as described in Owejan et al. (15). The gas lines are heated with separate controls to ensure that the gases arrive at the cell inlet at the specified test conditions and avoid condensation of water from the humidifier in the gas lines. Automated testing using the HyAl Fuel Cell Automated Testing System (FCATS) Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1603subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) has been used employed to implement ramped changes in load conditions over different time segments. Coolant loops are integrated into the compression plates on both the anode and cathode sides, allowing for control of the cell temperature. Eight 0.8 kW powered in-line heaters are used to control the coolant temperature and heat the cell with coolant loops. A 2 kW heat exchanger cooling system is placed in-line for rapid cooling of the cell at a fast rate, along with a temperature controlled water bath with 0.5 kW of additional cooling. These controls are used to change provide the ramp changes in the cell temperature for the investigation of transient temperatures. Figure 2: In situ fuel cell setup showing the thermocouples and differential pressure gauges. Two-phase pressure drops in the reactant channels are measured with differential pressure sensors from Honeywell®. The sensors have a range of 0 – 34 kPa with an accuracy of 0.25% of the range, resulting in an uncertainty of ±0.08 kPa. The cell also incorporates individual channel pressure drop measurement in the entrance region for measuring the instantaneous gas flow rate through each channel using the Hornbeck equation, as described in Kandlikar et al. (15). However, the individual channel flow rates are not presented in the current work. Two arrays of five thermocouples each on the anode and cathode sides (in the compression plates) monitor the temperature of the cell. The coolant lines have thermocouples at the end of the in-line heaters to regulate the power supplied to the inline heaters for controlling the cell temperature. The gas lines have separate thermocouples to control the temperature of the incoming reactants. Figure 2 shows the cell with the control thermocouples. The thermocouples have been calibrated to read within an uncertainty of less than ±1°C. Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1604subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) Load and cell voltages are recorded by the G40 test stand at a rate of 1 Hz. Temperature of the cell and the pressure drop in the channels on the cathode and anode sides of the cell are recorded on an auxiliary computer through a DAQ comprising of a PXIe series chassis from National Instruments. Test Matrix and Test Protocol In order to improve the repeatability of the test results, a standard operating procedure was utilized with a 2.5 hour cell conditioning routine, performed at the start of every testing day. This ensured the membrane was adequately hydrated, and the cell was at a steady state condition prior to the testing. For transient load testing, the cell was operated at steady state before changing the load through a ramp up or ramp down procedure. Different load changes were implemented over a 300 second period using the HyAl FCATS automation system. The voltage response and the two-phase pressure drop response were recorded. Tables 1 and 2 show the different test conditions investigated in this study. Table 1: Tests for transient effect from changing temperatures Temperature Start Temperature End (°C) (°C) 40 60 40 80 60 40 80 40 Table 2: Tests for transient effect from changing load Load Start Load End 2 (A/cm ) (A/cm2) 1.0 0.6 0.6 1.0 Current Densities (A/cm2) 1.0 1.0 1.0 1.0 Temperature of Test (°C) 40, 60, 80 40, 60, 80 In addition to the above mentioned tests, additional experiments were performed to check the repeatability of the results. Long duration tests were run to understand the time scale over which the transients play a role. These are discussed in the results section. Results Figure 3 shows the cathode channel pressure drop over a period of about 3 hours. After operating the cell at 0.8 A/cm2 for the first 2 hours, the load condition is changed to 0.1 A/cm2 to investigate the time it requires for the system to return to steady state in terms of the two-phase pressure drop in the channels. Although the pressure has been allowed to stabilize for over 6000 seconds (1.6 hours), there are still some inherent fluctuations in the pressure drop signature (Region A). As soon as the load is changed, from 0.8 A/cm2 Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1605subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) to 0.1 A/cm2, the flow rate of reactants is reduced, and the pressure drop decreases in the channels. Although there is an initial dip in the pressure drop (Region B), it slowly starts to increase, and reaches a new steady state value. The time required for the pressure drop to regain its steady state behavior is the time duration over which the transient behavior is relevant. Figure 3: Time required for the two-phase pressure drop to reach steady state after the system undergoes a change in load. The load was reduced from 40A to 5A. Next, the results from transient load conditions are discussed. The load changes have been implemented using a ramped profile over a period of 300 seconds. Figure 4 shows three different cases where the current density is reduced from 1.0 A/cm2 to 0.6 A/cm2. The response is noted from the voltage behavior and the two-phase pressure drop signature. The three different figures compare the results from the tests conducted at temperatures of 40, 60 and 80°C. In each of the tests, the stoichiometry is held constant at 1.5 for anode and 2.0 for cathode. It can be seen that the voltage response and the twophase pressure drop responses are almost instantaneous. This is expected, and is in line with the results of Hamelin et al. (6). The pressure drop decreases as consumption and air flow rate decrease, while the voltage increases with a decrease in the ohmic resistance due to lower current being drawn. It can also be seen that the pressure drop response with time is much steeper at higher temperatures, as the final pressure drop remains higher at the lower temperatures. There is significant water in the channels which results in the higher pressure drop. However, at the higher temperatures, most of the water is transported in the vapor phase and therefore the pressure drop is lower. Thus the pressure drop slope is much steeper at the higher temperatures. Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1606subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) Figure 4: Effect of decreasing load on the two-phase pressure drop and the voltage response. The load was reduced from 50 A to 30 A for each case shown. a) Response at 40°C, b) response at 60°C and c) response at 80°C. Figure 5 shows the effect of increasing load on the voltage response and the two-phase pressure drop in the reactant channels, as the load is increased from 0.6 A/cm2 to 1.0 A/cm2. The plots show the response at three different temperatures of 40, 60 and 80°C. Similar to the observations for decreasing current density (Figure 4), the results show here as well that the pressure drop slopes are steeper when the load transition takes place at the higher cell temperatures. Additionally, it may be noted that at 40°C, there is a distinct peak at the end of the transition after which the two-phase pressure drop decreases and approaches the steady state value. This is similar to the trough observed in Figure 3. However, with a significantly lower amount of liquid present in the channels, the same peak is no longer observed at the higher temperatures. Therefore, transient load changes have a greater impact on two-phase flow at the lower temperatures as compared to the higher temperatures. Next, the impact of a change in temperature is studied on the fuel cell performance. The optimum PEM operation is in the range of 60 – 80°C. A higher temperature results in reduced activation losses, and therefore improves the voltage response from the cell. Thus, it would be beneficial to operate the fuel cell at higher temperatures. However, at startup, the temperature of the cell is at the ambient conditions. Therefore, at the start of Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1607subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) operation for a PEMFC powered vehicle, the cell would need to transition from the ambient temperature to the optimum temperature of 80°C. The following discussion brings forth the issues that may arise, and the transient behavior that needs to be understood during the transition of cell temperature from ambient to 60 or 80°C. Figure 5: Effect of increasing load on the two-phase pressure drop and the voltage response. The load was increased from 30 A to 50 A for each case shown. a) Response at 40°C, b) response at 60°C and c) response at 80°C. Figure 6 shows the effect of dynamically increasing temperature on the cell performance, and the two-phase pressure drop in the cathode reactant channels. Figure 6(a) shows the response for a temperature change from 40 to 60°C, which is accompanied by an increase in voltage response for the steady load. The pressure drop in the channels decreases as more of the water is removed in the vapor phase, and therefore liquid blockages are reduced. Figure 6(b) shows the response for a temperature change from 40 to 80°C. The voltage reaches a peak just before 60°C, and then starts to decrease. The pressure drop also decreases at first, and then begins to increase. This reversal, as the cell temperature continues to increase beyond 60°C, may be attributed to the loss in hydration of the membrane. The rapidly increasing cell temperature results in an increased saturation temperature. Therefore most of the water is removed from the cell. The humidification systems respond to the change in temperature at a slower rate, and therefore cannot provide the necessary humidification required for the cell to operate at 80°C. The increase in pressure drop is due to the increased gas velocities, resulting from a lower gas Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1608subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) density at 80°C. There is no more liquid water in the channels, and therefore the increase in saturation temperature has a less significant effect on the two-phase pressure drop. Figure 6: Effect of increasing temperature on the voltage response and the two-phase pressure drop in the channels. The cell is operated at a constant load of 50A with a stoichiometry of 1.5 on the anode side and 2 on the cathode side. a) cell temperature increases from 40 to 60°C b) cell temperature increases from 40 to 80°C. Figure 7: Effect of decreasing temperature on the voltage response and the two-phase pressure drop in the channels. a) Cell temperature decreases from 80 to 40°C and b) cell temperature decreases from 75 to 55°C. Figure 7 shows the effect of dynamically decreasing temperature on the cell performance, and the two-phase pressure drop in the cathode reactant channels. Figure 7(a) shows the decrease in temperature from 77°C to 40°C, while figure 7(b) shows the decrease in temperature from 75°C to 55°C. It can be observed from these figures that the decrease in temperature from 77°C to 40°C causes a significant decrease in voltage, and thus the performance suffers due to the rapid decrease in temperature. The pressure drop however does not drop as quickly. This can be attributed to condensation in the channels for the humidified inlet conditions. Additionally, the cell is cooled at the compression plates, while the MEA remains hotter due to the reactions resulting in temperature gradient driven water transport into the channels. These two factors result in the pressure drop remaining high in the channels, even though the temperature has decreased. However, for Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1609subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) a temperature transition from 75°C to 55°C, i.e. a drop of 20°C, the effect is not as significant. There is a negligible drop in the voltage response and a very small reduction in the pressure drop in this case. Summary The current investigation explores the impact of two-phase flow on the transient performance of PEM fuel cells. Previous works have shown that the electrochemical reaction has a transient behavior lasting less than 1 second. However, transient response in two-phase flow lasts for time periods on the order of several minutes. Therefore, the effect of the transient behavior of two-phase flow on the performance of a PEM fuel cell is investigated here. The key findings are summarized as follows: In response to a change in operating conditions in a PEMC, time durations on the order of several minutes are required for the two-phase flow in the reactant channels to return to steady state behavior. Transient load changes have a greater impact on two-phase flow at the lower temperatures. Decreasing temperature rapidly below 60°C results in a loss of performance from the cell, and increased pressure drop due to increased liquid water from condensation within the cell. Increasing temperature rapidly beyond 60°C results in a loss of performance that could be attributed to the membrane dryout due to inability of the humidification system to respond quickly as the cell temperature increases. Temperature fluctuations between 60 and 80°C are not significant, as the water remains mostly in vapor phase in both cases. The effect of two-phase pressure drop on the transient performance of a PEM fuel cell needs to be explored further. A detailed investigation is required to establish the time constant for the transient response, and the parameters affecting the time constant. Acknowledgments This work was conducted in the Thermal Analysis, Microfluidics and Fuel Cell Laboratory at the Rochester Institute of Technology. The work was supported by the US Department of Energy under the award number DE-EE0000470. The authors would like to thank Wenbin Gu and Jeffrey Gagliardo from the Electrochemical Energy Research Laboratory at General Motors for supplying the GDL samples tested in this work and for general technical discussions facilitating this work. References [1] P. Corbo, F. E. Corcione, F. Migliardini, and O. Veneri, “Experimental study of a fuel cell power train for road transport application,” J. of Power Sources, vol. 145, no. 2, pp. 610–619, Aug. 2005. [2] M. Uzunoglu and M. S. Alam, “Dynamic modeling, design, and simulation of a combined PEM fuel cell and ultracapacitor system for stand-alone residential Downloaded on 2013-12-06 to IP 129.21.102.159 address. Redistribution 1610subject to ECS license or copyright; see ecsdl.org/site/terms_use ECS Transactions, 58 (1) 1601-1611 (2013) applications,” Energy Conversion, IEEE Transactions on, vol. 21, no. 3, pp. 767– 775, Sep. 2006. [3] J. Wu, X. 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