Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) 0013-4651/2013/160(6)/F487/9/$31.00 © The Electrochemical Society F487 Effect of Channel Material on Water Droplet Dynamics in a PEMFC Gas Channel Preethi Gopalana,∗ and Satish G. Kandlikara,b,∗∗,z a Microsystems Engineering, Rochester Institute of Technology, Rochester, New York 14623, USA b Mechanical Engineering, Rochester Institute of Technology, Rochester, New York 14623, USA Water accumulation in the gas channels affects the gas diffusion to the reaction sites and the overall performance of proton exchange membrane fuel cells (PEMFCs). Understanding water droplet growth and detachment from the gas diffusion layer (GDL) inside the channel is critical in developing better water management strategies. It has been reported that the wettability of the channel affects the droplet-wall interaction. Hence, in this study, the behavior of the liquid water droplet within a channel is experimentally investigated from a fundamental perspective. Experiments were conducted for different air velocities (0.2–2.4 m/s), GDL types and channel wall materials which are commercially used in PEMFCs for automotive applications. Experimental results were analyzed through the Concus-Finn condition using instantaneous dynamic contact angle (IDCA) to determine the corner filling behavior, which is a precursor to channel flooding. Droplet detachment is influenced by air flow within the channel and the contact angle hysteresis (CAH) of the wall and the GDL material. Experiments were also performed on the GDLs that have undergone longer test periods in a fuel cell. Results showed much lower static CA and CAH, and a corresponding change in the droplet dynamics on used GDL compared to the new GDLs. © 2013 The Electrochemical Society. [DOI: 10.1149/2.030306jes] All rights reserved. Manuscript submitted January 8, 2013; revised manuscript received February 25, 2013. Published March 8, 2013. This was Paper 1633 presented at the Honolulu, Hawaii, Meeting of the Society, October 7–12, 2012. Proton exchange membrane fuel cells (PEMFCs) have shown tremendous potential in becoming a reliable source for a variety of power generation applications including automotive purposes.1 Despite many advantages, one of the major outstanding issues in the commercialization of the PEMFCs in automotive applications is inefficient water management at the startup and shutdown of the system in the presence of liquid water.2 Water management is of critical importance to enable proper diffusion of gases toward the catalyst layer, as both the liquid water and the air share the same pathways to initiate and sustain chemical reactions within the cell. Accumulation of the liquid water on the cathode side of a PEMFC leads to flooding of the channels, and thereby hinders the reactant flow toward the reaction sites, consequently lowering the efficiency of the system. On the other hand, lack of water in the cell leads to membrane dehydration and reduction of the proton exchange through the membrane, and thus decreasing the efficiency of the system.3,4 Effective and balanced water management in PEMFCs is of utmost importance to realize improved efficiency of the cell prior to commercialization. The primary source of liquid phase in a PEMFC is the water droplet emerging from the GDL into the channel. The analysis of the water droplet emergence, growth, interaction with the channel wall surface, and removal from the channel as a function of gas flow velocity becomes necessary. Having a complete understanding of the liquid droplet behavior on the GDL surface and its interaction with the channel forms the major motivation for the current work. There have been several techniques used to visualize the liquid water emergence and its interaction with the channel walls. Some of the imaging techniques that have been successfully used are neutron radiography,5–9 X-ray radiography,10 fluorescence microscopy,11 nuclear magnetic resonance (NMR) microscopy,12 and magnetic resonance imaging (MRI).13–15 Drawbacks of using such techniques are that these are expensive, have limited availability, and require complex system modifications. One of the reliable imaging techniques that has been used to evaluate the flow regime in the gas channel, water emergence mechanism, and the droplet interaction with the gas channel is the visible light imaging. To use the visible light imaging, the gas channel cover must be transparent or optically clear. Bazylak et al. used an optically clear gas channel to visualize the droplet breakthrough and its growth in the channel.11 Similarly, Yang et al. performed experiments using a transparent fuel cell to observe the droplet emergence pattern on the GDL and its behavior in the gas ∗ ∗∗ z Electrochemical Society Student Member. Electrochemical Society Active Member. E-mail: [email protected] channel.16 It was found that the droplets generally appear at certain preferential pores and grow to a certain size before detaching from the GDL. Tuber et al. were among the first few groups to study the effect of GDL wettability on the water accumulation in the channel using a transparent fuel cell.17 They found that hydrophilic GDLs result in a more uniform spread of water on the GDL surface and a decrease in the fuel cell performance and hence the reduced current densities. To further understand the mechanism of droplet removal, the surface forces that act within the gas channels on the liquid water and their influence on the droplet removal have been studied in literature both experimentally (in situ and ex situ) as well as numerically. Some of these preliminary studies showed that the surface forces are the primary causes for water accumulation and channel flooding in the PEMFCs compared to the viscous, pressure or inertial forces.18 The surface forces are mainly dependent on the advancing and receding contact angles, and the hysteresis on the material surface. In general, different GDL materials used in PEMFCs possess different surface characteristics, and thus differ in their droplet accumulation characteristics within the gas channels.19,20 A few detailed studies have further attempted to evaluate different channel properties, mainly focusing on the liquid water stagnation. It was found that the hydrophilicity of the channel surface facilitates the removal of water by wicking it into the channel corners.21 These results were in agreement with the conclusions derived from the more recent studies performed by Lu et al., who found that the hydrophilic channels help in uniform water distribution along the GDL surface.22 They stated that the hydrophilic channels aid in creating a film flow in the channel, and reduce the pressure drop in the system compared to the hydrophobic channels. Similar study was also conducted by Zhu et al.,23 however their results contradicted the conclusion of Zhang et al.21 They proposed that the spreading of the liquid water near the hydrophilic walls leads to a film flow and blockage of the reactant channel pathway. They also stated that the channel geometry has an important role in the spreading of the liquid water in the channels. To address the effect of channel geometry on the water accumulation, Zhu et al. conducted simulations on different channel geometries and found that the upside down trapezoidal channels had the highest water coverage ratio compared to any other channel configurations.24 It was also noticed that the triangular channels performed more efficiently compared to the rectangular channels. On a similar note, Lu et al. investigated the effect of channel geometry and channel orientation on the water hold up in the cell.22 They concluded that the sinusoidal geometry for the gas channel helps in obtaining lower pressure drop in the system compared to the trapezoidal or rectangular channel. Also, the gravity and the shear forces in the channel affect Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use F488 Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) Figure 1. Experimental test setup used to visualize the channel end to visualize the droplet dynamics with the channel wall and the base. A detailed description of the channel is shown by the image on the right side. the liquid transport in the gas channel. This implies that the PEM fuel cells in vertical orientation would result in a better performance compared to the horizontal orientation. To tackle the water stagnation issue at a much more fundamental level, Rath and Kandlikar analyzed the droplet interactions with the sidewall of the channel at different open angles (angle between the GDL and the channel sidewall).25 The Concus-Finn condition was used to predict the filling behavior of the droplet in the corners of the channel.26,27 They found that 52◦ and lower channel angles would lead to droplet pinning to the sidewall of the channel and result in no corner filling. Gopalan and Kandlikar extended this work by incorporating an air flow into the system to simulate a realistic PEMFC working condition.28,29 It was established that the corner filling of the channel is more dynamic in nature and depends upon the instantaneous dynamic contact angle (IDCA) that the droplet makes with the sidewall and the GDL at a given air velocity. These studies were limited to only one particular channel wall and GDL material. However, investigation of the droplet growth and removal pattern on different pairs of materials that are commercially used for the automotive application would be beneficial for understanding the effect of material properties on the droplet dynamics. To address this fundamental issue, this work focuses on analyzing the effects of four channel wall materials (stainless steel (SS-2205), copper (Cu-110), graphite composite, polycarbonate (Lexan)) and three GDL types (MRC-105, SGL-25BC, TGP-H-060) on the liquid water droplet dynamics in the presence of airflow within the gas channel. Ex-Situ Experimental Experimental set up.— A schematic of the ex-situ setup used in the present study is shown in Figure 1. The test setup consists of a base plate made of polycarbonate, which holds the GDL on top of it. An inlet for the water droplet was made on the base plate near the channel end to allow the water to emerge onto the GDL surface and interact with the sidewall. The channel sidewall plates are made up of different materials. These plates are studied under two different open angles of 45◦ and 50◦ . These plates were placed on top of the GDL layer. The top wall (above the sidewall plates) was attached to this setup forming a complete 100 mm long channel. In our experiments, polycarbonate (Lexan), stainless steel (SS-2205), copper (Cu-110) and graphite composite materials that are commonly used for the bipolar plates in the PEMFCs were used for the channel sidewalls as well as for the top plate. SGL-25BC, MRC-105 with 6% PTFE and TGP-H-060 with 6% PTFE were used as the GDL materials. To evaluate the performance difference due to aging, two MRC-105 GDLs that were run for 40 and 125 hours by Lu et al.22 were compared with a fresh sample. Furthermore, the superficial air velocities were varied between 0.2–2.4 m/s, which corresponded to a current density range of 0.1–1 A/cm2 in a typical fuel cell with an active area of 50 cm2 .6 The Bond number and the Weber number calculated for the given experimental conditions were in the range of 0.1–0.2 and 1–50 respectively. The water flow rate was kept constant at 0.05 mL/min (corresponding to the water generation rate for a current density of 3 A/cm2 for an active area of 2.9 cm2 ). More detailed description of the experimental setup can be found in the paper by Gopalan and Kandlikar.28,30 For each of the materials considered in this study, the advancing and receding contact angles were measured using the VCA Optima Surface Analysis System. The contact angle hysteresis (CAH) was calculated as θhys = θadv – θrec . The detailed values are listed in Table I. The Concus-Finn condition was used for the theoretical estimation of the transition angle from non-filling to filling condition for a given material pair as shown in Table II. The Concus-Finn condition characterizing the contact angle range for which de-wetting of the corner occurs is given by 2α < (θ B + θW ) − π [1] where θB is the advancing contact angle for the base material (GDL), θW is the advancing contact angle for the sidewall and 2α is the channel open angle (angle between the sidewall and GDL). According to the above condition, the channel corner will not be filled if the above inequality is satisfied. It was found from the data that all material combinations had transition angles near 50◦ (48◦ –53◦ ). An open angle smaller than the transition angle showed no corner filling, and any open angle above the transition angle showed corner filling behavior. Since the current study involves several variables, the experimental test matrix was simplified to an extent by only including 45◦ and 50◦ channel open angles as these angles are closer to the transition angle. Experimental procedure.— For each pair of materials used in the experiments, the air flow was set to the desired value and the droplet was allowed to grow on the GDL surface. High speed videos were recorded using Keyence VW-6000 camera at 60–125 fps from the time Table I. Static advancing and receding contact angles of sidewall materials. Material Advancing Contact Angle (θadv ) Receding Contact Angle (θrec ) Hysteresis (θhys ) MRC-105 with 6% PTFE TGP-H-060 with 6% PTFE SGL-25BC 40 hours MRC-105 GDL 125 hours MRC-105 GDL Polycarbonate Copper (Cu-110) Graphite Composite Stainless Steel (SS-2205) 148 145 148 144 132 85 80 84 81 138 127 136 136 123 61 53 34 60 10 17 12 8 9 24 27 50 19 Table II. Transition Angles from Non-Filling to Filling for a Given Material Pair. Material Pair Transition Angles MRC-105 GDL- Polycarbonate MRC-105 GDL – Copper (Cu-110) MRC-105 GDL – Graphite MRC-105 GDL – Stainless Steel (SS-2205) TGP-H-060 – Polycarbonate SGL-25BC- Polycarbonate 40 hours MRC-105 GDL- Polycarbonate 125 hours MRC-105 GDL- Polycarbonate 53◦ 48◦ 52◦ 49◦ 50◦ 51◦ 49◦ 37◦ Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) the droplets appeared on the GDL to the time they were completely removed from the channel. Typically, in all our experiments, the following droplet growth sequence was observed: A droplet appears on the GDL and grows to its full size before contacting the sidewall. Once the droplet touches the sidewall it either fills the channel corner or remains pinned on the sidewall depending on the channel open angle until the pressure inside the channel builds up leading to the removal of the droplet. The high speed videos of the droplet growth and its interaction with the channel wall were post-processed using the Keyence motion analyzer. The IDCA the droplet made with the channel wall and the GDL was measured on each frame. The uncertainty in the measurement of the contact angle was approximately ± 1◦ . Pressure drop across the droplet was measured using a Honeywell FWD differential pressure sensor (0–1 psi range). The uncertainty in the pressure sensor measurement was ± 0.25% of full scale reading. Results Concus-Finn condition.— This condition was used to predict the liquid droplet behavior at the intersection of the GDL and the sidewall surfaces. The contact angles the droplet makes with different surfaces are shown in Figure 2a, and these angles are plotted on a 2D graph as shown in Figure 2b. It can be inferred from this graph that if the contact angle points lie in the shaded region, the droplet will fill the channel corners. Otherwise, the droplet will remain pinned at the channel sidewall without filling the channel corners.27 In PEMFCs, once the droplet fills the channel corner, the successive droplets emerging from the GDL surface near the corner will merge with this water, and may eventually lead to channel flooding, depending on the airflow rate. Therefore, it is essential to avoid corner filling in the channel to prevent such degenerative effects. In our prior work, it was demonstrated that the material roughness also influences the contact angle measurements. To avoid discrepan- F489 Figure 3. Confocal Laser Scanning Microscope images of different GDL and channel wall materials. (a) MRC-105 (b) SGL-25BC (c) TGP-H-060 (d) Cu 110 (e) Graphite Composite (f) SS 2205MRC-105. cies due to the local surface roughness variation in our experiments, the channel walls were polished using an emery cloth. The surface roughness of the sidewall was measured using the Confocal Laser Scanning Microscope (CLSM), and the corresponding images of different channel walls and the GDL samples are shown in Figure 3. The surface roughness for different sidewall materials was confirmed to be less than 900 nm from the image slices and is summarized in Table III. Effect of channel wall material.— For these set of experiments, the base GDL material MRC-105 was used while the sidewall material was changed along with the channel open angle. Stainless steel (SS-2205) sidewall.— According to the theoretical prediction using the Concus-Finn condition, the transition angle for SS-2205 and MRC-105 was found to be 49◦ . Experimentally it was found that for 45◦ channel, the corner filling did not occur for any air velocity agreeing with the theoretical predictions. A recorded image sequence of the droplet growth and its interaction with the SS-2205 sidewall for an open angle of 45◦ and air velocity of 1.6 m/s is shown in Figure 4. The IDCA for the SS-2205 sidewall and the MRC-105 base measured from each frame of the video sequence was plotted against the Concus-Finn Limit (CFL) as shown in Figure 5a. According to the Concus-Finn condition, any point falling below the CFL line would lead to corner filling condition, and any point above would lead to no corner filling condition. The observed behavior can also be compared to the plot of the IDCA points that lie above the CFL line. Hence, the findings from our experiments regarding droplet filling agreed with the corresponding theoretical predictions. However for a 50◦ channel, contradictory results were obtained between the experimental observation and the theoretical predictions. For 50◦ channel, corner filling was observed only for the lower air velocities (0.2–0.6 m/s), and not for the higher air velocities (0.7–2.4 m/s). Image sequences of the droplet interacting with the 50◦ channel walls for an air velocity of 1.6 m/s are shown in Figure 6. It was also observed that the IDCA for lower air velocities fell below the CFL line satisfying the corner filling criterion (Figure 5b). In contrast, the IDCA for higher air velocities fell above the CFL line leading to non-corner filling behavior. From the experiments it was observed that the effect of air velocity was pronounced, and caused noticeable oscillations Table III. Surface Roughness Measured for the Different Sidewall Materials Used. Figure 2. Concus-Finn Condition a) Different contact angles made by the droplet with the base and the sidewall b) Plot representing the Concus-Finn condition when the droplet contacts the base and the sidewall. Material Surface Roughness (Ra) Copper (Cu-110) Graphite Composite Stainless Steel (SS-2205) Polycarbonate (Lexan) 554 nm 873 nm 558 nm 666 nm Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use F490 Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) Figure 4. Image sequence of the droplet interaction with the Stainless Steel (SS-2205) sidewall and MRC-105 base in the 45◦ open angle channel with 1.6 m/s air velocity inside the channel. The red circle in the image shows that the droplet does not fill the corner of the channel. in the droplet at higher velocities. These oscillations affected the transition between the channel filling and non-filling behaviors at the transition angles (disagreeing with the traditional Concus-Finn condition). Due to the oscillations in a droplet, the instantaneous contact angle the droplet makes with the sidewall may become larger than the equilibrium contact angle just prior to its contact with the sidewall. If the conditions are close to the Concus-Finn criterion, the higher contact angle experienced due to oscillation may cause the droplet to not fill the corner. Therefore, the use of dynamic contact angles is emphasized to predict the droplet behavior and thus the overall water coverage ratio on the GDL more accurately. Copper (Cu-110) sidewall.— A set of similar experiments were conducted with the Cu-110 sidewall. According to the theoretical prediction, the transition angle for Cu-110 and MRC-105 was 48◦ . The experimental results observed for Cu-110 for both the 45◦ and 50◦ channels were similar to those observed for SS-2205 sidewalls. Figure 5. Plot of instantaneous dynamic contact angle (IDCA) made by the droplet with the Stainless Steel (SS-2205) sidewall and the MRC-105 GDL base for (a) 45◦ open angle channel and (b) 50◦ open angle channel at different air velocities. Graphite composite sidewall.— The transition angle for the graphite sidewall according to the theoretical prediction was 52◦ . From the experimental results, it was found that for 45◦ and 50◦ open angle channels, the droplet did not fill the channel corners for any air velocities (0.2–2.4 m/s) and the results agreed with the IDCA plot (Figure 7) which showed no corner filling behavior for any air velocities. The three channel wall materials commonly considered for use in the automobile applications (stainless steel, copper, graphite) have been found to have varying effects on the droplet behavior depending upon the CAH value. The graphite composite, which has the largest CAH, behaved differently compared to the materials that have lower CAH values near the transition angle. It can be concluded that the CAH affects the droplet behavior in the gas channels. Materials that have larger CAH can accommodate a larger range of IDCA that the droplet makes with the wall and the GDL, facilitating later corner filling than that given by the Concus-Finn condition. Due to the oscillations in a droplet, the instantaneous contact angle the droplet makes with the sidewall may become larger than the equilibrium contact angle just prior to its contact with the sidewall. If the conditions are close to the Concus-Finn criterion, the higher contact angle experienced due to oscillation may cause the droplet to not fill the corner. On the other hand, materials having smaller CAH can only accommodate smaller oscillations in the droplets produced by the air flow without leading to corner filling of the channel. Figure 6. Image sequence of the droplet interaction with the Stainless Steel (SS-2205) sidewall and MRC-105 base in the 50◦ open angle channel with 1.6 m/s air velocity inside the channel. The red circle in the image shows that the droplet filled the corner of the channel. Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) F491 Figure 7. Plot of instantaneous dynamic contact angle made by the droplet with the graphite sidewall and the MRC-105 GDL base for (a) 45◦ open angle channel and (b) 50◦ open angle channel at different air velocities. Figure 8. Plot of instantaneous dynamic contact angle made by the droplet with the polycarbonate sidewall and the TGP-H-060 base for (a) 45◦ open angle channel and (b) 50◦ open angle channel at different air velocities. When using MRC-105 GDL with any of the tested channel materials, the droplet filling of the channel corners did not take place for open angles below 45◦ . The 50◦ open angle channel behaved as a transition between filling and non-filling conditions. The Concus-Finn condition (using static contact angles) could not accurately predict the corner filling behavior of the droplet near the transition angle. Hence, using IDCA information would be helpful in predicting the droplet behavior in the gas channel of PEMFC instead of static contact angle information. with the theoretical predictions for all air velocities. The IDCA plots for the 45◦ and the 50◦ open angle channels at 0.2 and 1.6 m/s air velocities are shown in Figure 8. Effect of GDL material.— There are different types of GDL materials that are used in the PEMFCs. The most commonly used are Toray, SGL and the MRC-105. To evaluate the effect of a GDL material on the droplet growth and removal, experiments were performed under similar conditions as mentioned earlier. In these experiments the channel wall material was kept constant (polycarbonate) while the GDL materials were changed along with the channel open angle. The GDL materials used for these experiments were TGP-H-060 and SGL-25BC with 6% PTFE. SGL-25BC and polycarbonate channel wall.— The transition angle for SGL-25BC and a polycarbonate sidewall was found to be 51◦ . Similar experimental results were observed for SGL-25BC in which the droplets did not fill the channel corners for the 45◦ and 50◦ channels for any air velocities. The image sequence of the droplet growth in the 50◦ open angle channel at 1.6 m/s air velocity is shown in Figure 9a. The plot comparing the IDCA for both SGL-25BC— polycarbonate and MRC-105-polycarbonate material pairs, observed in our previous study,28 at air velocities 0.2 and 1.6 m/s is shown in Figure 9b. It is observed from the plot that the IDCA point for the MRC-105-polycarbonate material pair covers larger range of contact angles compared to the SGL-25BC-polycarbonate material pair. This may also be one of the reasons why at lower air velocities, the MRC105 showed corner filling behavior. However the SGL-25BC did not show corner filling behavior in the 50◦ open angle channel. TGP-H-060 and polycarbonate channel wall.— For TGP-H-060 with 6% PTFE and a polycarbonate sidewall, the transition angle was found to be 50◦ according to the theoretical prediction using the Concus-Finn condition. The experimental results showed no corner filling for both 45◦ and 50◦ open angle channels. These results agreed Effect of used GDL material.— To understand the effect of GDL deterioration on the droplet dynamics inside the gas channel of PEMFCs, MRC-105 GDLs, which were previously run for 40 and 125 hours in an experiment performed by Lu et al.,22 were employed. Experiments were performed using these GDL samples with polycarbonate Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use F492 Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) Figure 9. (a) Image sequence of the droplet interaction with the polycarbonate sidewall and SGL-25BC base in the 50◦ open angle channel with 1.6 m/s air velocity. (b) Plot of instantaneous dynamic contact angle made by the droplet with the polycarbonate sidewall and the base MRC-105 and SGL-25BC GDL for 50◦ open angle channel at different air velocities. channel walls under similar test conditions. It was observed from these experiments that after 40 hours run time, the used GDL performed similarly to a fresh MRC-105 GDL. For 45◦ open angle channel, it did not show corner filling behavior for any air velocities introduced in the system. For 50◦ open angle channel, it showed corner filling behavior at lower air velocities (0.2–0.6 m/s), and no corner filling at higher air velocities (0.7–2.4 m/s). However, the GDL with 125 hours run time showed a different behavior. It was observed that the droplet filled the channel corners for both 45◦ and 50◦ open angle channels for all the air velocities. To further understand this behavior, the advancing and receding contact angles on the used GDL samples were measured and are shown in Table I. It was observed that 125 hours run time GDL had much lower advancing and receding contact angles compared to those for the fresh samples. However, samples with 40 hours run time did not show much difference from the fresh samples in terms of advancing and receding contact angles. This shows that the wettability of the GDL samples reduced with longer run time. The transition contact angle between corner filling and non-filling for both 40 and 125 hours run time samples with polycarbonate were measured. It was seen that the transition angles were 49◦ and 37◦ respectively as shown in Table II. This explains the discrepancy observed in the droplet dynamics for the 125 hours run time sample. To further validate these results, the IDCA for 50◦ open angle channel were plotted against the CFL for both 40 and 125 hour run time samples with polycarbonate sidewall, and are shown in Figure 10. Figure 10a shows that for the 40 hours run time sample, the droplet fills the channel corners at lower air velocities (0.2–0.6 m/s), and does not fill at higher air velocities (0.7–2.4 m/s). For the 125 hours run time sample, Figure 10b shows that for all air velocities, the IDCA point fell below the CFL line. This indicates that the droplet should fill the channel corners for all air velocities. This work indicates that the GDL material deteriorates or loses its wettability after longer run time which perhaps affects the corner filling behavior of the droplet and lead to larger accumulation of water inside the gas channel. Further study with a larger number of samples and different run times is warranted to explore this effect further. Pressure drop across the droplet.— Pressure drop across the droplet is one of the important parameters in understanding the dynamics of water removal. In PEMFCs, lower pressure drop in the system corresponds to a lesser amount of water hold up in the channel and thus, lower gas transport resistance. Therefore, lower pressure drop in the system would result in higher gas transport and thus increasing the efficiency of the PEMFC system. To measure the pressure drop across the droplet, a pressure sensor was connected to the channel using a pressure tap just before the droplet inlet location in the upstream of the channel. The peak pressure drop across the droplet in a channel for different channel wall materials and air velocities are plotted in Figure 11. The uncertainty in the peak pressure drop value was about 0.25%. For the 45◦ channel, Figure 11a showed that for different channel wall materials, the peak pressure drop across the droplet followed a similar trend. The pressure drop in the system would increase with an increase in the air velocity. This is mainly due to the blockage created by the droplet in the channel. Once the pressure inside the system reaches its maximum value, the droplet would be removed from the system due to the force exerted by the air flow on the droplet. However, at very high air velocities (1.8–2.4 m/s) the peak pressure drop value starts to decrease. At higher air velocity, the droplet starts to transition toward film flow regime instead of slug flow, as observed for lower air velocities in the system. Therefore, the force required to remove the droplet is lower for higher air velocities as compared to that required at lower air velocities. The different flow patterns observed in the 50◦ open angle channel is shown in Figure 12. It is seen from the figure that, at lower air velocities, the droplet grows and completely fills the channel cross section to form the slug flow. Once the pressure inside the channel overcomes the surface tension force with which the liquid is held in the channel, the liquid is removed from the channel. However, at higher air velocities, the force exerted by the air flow in the channel is much higher than the surface tension force exerted on the liquid. Hence, before the liquid completely blocks the channel and the pressure drop increases in the channel, the liquid is removed from the channel as a film flow. It was also observed that different channel materials showed significant differences in the peak pressure drop value in the 50◦ open angle channel. From Figure 11b, it was observed that Cu-110 and SS2205 produced a much higher pressure drop compared to the graphite composite channel wall at lower air velocities (0.2–1 m/s). This was mainly due to the channel corner filling observed for both Cu-110 and SS-2205 at lower air velocities. On the other hand, graphite Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) F493 Figure 10. Plot of instantaneous dynamic contact angle made by the droplet in a 50◦ open angle channel at different air velocities with the polycarbonate sidewall; (a) 40 hours run MRC-105 GDL; and (b) 125 hours run MRC-105 GDL. composite channel wall showed no corner filling at lower air velocities, resulting in a much lower pressure drop in the system. At medium air velocities (1.1–1.7 m/s) the channel wall materials showed a similar peak pressure drop in the system, which increased with an increase in the air velocity. This corresponded to the non-corner filling condition observed in the experiments. At higher air velocities (1.8–2.4 m/s), the peak pressure drop in the system starts to gradually decrease, since the droplet transitions to the film flow and produces a much lower blockage in the channel cross section compared to that at lower and medium velocities. The peak pressure drop measured for different GDL materials also followed a similar pattern, as observed for different channel wall materials and is plotted in Figure 13a. From the experiments it was observed that for both SGL-25BC and TGP-H-060, the droplet did not fill the channel corners in 45◦ , as well as 50◦ open angle channels for any air velocities. The peak pressure drop values measured for a given channel angle with different GDL materials also showed similar results. For both SGL-25BC and TGP-H-060, the peak pressure drop in a channel increased as the air velocity increased, for air velocities lower than 1.7 m/s. However, for higher air velocities (1.8–2.4 m/s) the peak pressure drop started to decrease. It was also interesting to note that the pressure drop values observed for different GDL types with polycarbonate sidewall were similar to those observed for MRC105 GDL and polycarbonate channels in our previous study.28 Hence, Figure 11. Plot of peak differential pressure drop across the droplet as a function of air velocity, for different channel wall material, (a) 45◦ open angle channel, and (b) 50◦ open angle channel. The uncertainty in the pressure drop was around 0.25%. this shows that different types of GDLs do not have any significant differences in the droplet-wall interactions. Peak pressure drop for used GDL materials differed significantly compared to those of the fresh GDL samples. Figure 13b shows the peak pressure drop measured for a 50◦ open angle polycarbonate channel with used GDL samples at different air velocities. From the plot it is observed that the peak pressure drops for the 40 hour run time sample at lower air velocities were higher compared to those at higher air velocities. This showed that the droplet fills the channel corners, forms a slug flow at lower air velocities, and results in a higher pressure drop. At higher air velocities, the droplet transition to film flow and does not fill the channel corners, leading to a lower pressure drop in the system. For the 125 hours run time sample, the droplets resulted in a slug flow for all air velocities. The peak pressure drop values for all air velocities were much higher compared to those for the 40 hour run time samples. This showed that after a longer run, the hydrophobicity of the GDL was reduced and lead to a slug flow, causing increased liquid stagnation in the channels and reduced area available on the GDL surface for gas transport. Downloaded on 2013-05-09 to IP 129.21.225.12 address. Redistribution subject to ECS license or copyright; see ecsdl.org/site/terms_use F494 Journal of The Electrochemical Society, 160 (6) F487-F495 (2013) Figure 12. Different flow patterns observed in the 50◦ open angle channel (a) Slug flow at lower air velocities (b) Film flow at higher air velocities. Conclusions In this work, ex-situ experiments were conducted to study the water droplet dynamics in a PEMFC gas channel with different channel sidewall angles, channel wall materials, and GDL materials under controlled air flow velocities between 0.2–2.4 m/s. High speed video images showing the droplet interaction with the channel walls were recorded. The pressure drop across the droplet was also recorded simultaneously. It was revealed through the recorded high-speed videos that the droplet dynamics at the channel corners are significantly affected by the channel open angles, air flow velocities and the channel materials. r Sidewall material: Characteristic behaviors of different channel materials differ considerably based on their material property. The CAH played a major role in determining the corner filling behavior for each type of channel. Materials such as graphite, which have larger CAH, showed no corner filling behavior for any air velocities at the transition angle. These materials can accommodate larger oscillations before the droplet starts to move on the wall surface to fill the channel corner. However, for materials having smaller CAH (copper, stainless steel and polycarbonate), corner filling occurred at lower air velocities. r Air flow rate: Air flow in the channel produced oscillations in the water droplet which determined the instantaneous contact angles the droplet made with the sidewall and the base GDL. In this case, the IDCA of the droplet determines the corner filling behavior. Also, at lower air velocities the droplet completely blocks the channel and forms a slug flow, whereas at higher air velocities the droplet transforms into a film flow. r GDL materials: For channel open angles near the transition point, SGL-25BC and TGP-H-060 showed no corner filling. However, Figure 13. Plot of peak differential pressure drop values across the droplet (a) For different GDL materials in 45◦ and 50◦ open angle channels as a function of air flow velocity (b) For used GDL materials in 50◦ open angle channels as a function of air flow velocity. The uncertainty in the pressure drop was around 0.25%. MRC-105 showed corner filling at lower air velocities. The CAH and oscillations in the water droplet determined the corner filling behavior for a given GDL and wall material. r Used GDL materials: Hydrophobicity of the GDL material reduces with a longer run time, and leads to larger accumulation of liquid water in the channel compared to that with fresh GDL samples. This would reduce the available area for gas transport on the GDL surface and increased gas transport resistance with longer run times. Further work in this area is warranted with a larger number of GDL samples. r Concus-Finn condition: The Concus-Finn condition using static contact angle predicted the corner filling behavior inaccurately in a dynamic condition. Instead, using IDCA in the Concus-Finn condition detected the corner filling more accurately, especially near the transition angle. 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