Water permeation through gas diffusion layers of proton exchange membrane fuel cells

Water transport through gas diffusion layer of proton exchange membrane fuels cells is investigated experimentally. A filtration cell is designed and the permeation threshold and the apparent water permeability of several carbon papers are investigated. Similar carbon paper with different thicknesses and different Teflon loadings are tested to study the effects of geometrical and surface properties on the water transport. Permeation threshold increases with both GDL thickness and Teflon loading. In addition, a hysteresis effect exists in GDLs and the permeation threshold reduces as the samples are retested. Moreover, several compressed GDLs are tested and the results show that compression does not affect the breakthrough pressure significantly. The measured values of apparent permeability indicate that the majority of pores in GDLs are not filled with water and the reactant access to the catalyst layer is not hindered.     

Effect of polytetrafluoroethylene-treatment and microporous layer-coating on the in-plane permeability of gas diffusion layers used in proton exchange membrane fuel cells

The in-plane permeability has been experimentally estimated for a number of carbon substrates and microporous layer (MPL)-coated gas diffusion layers (GDLs) as used in proton exchange membrane (PEM) fuel cells. The results show that the in-plane permeability of the tested carbon substrates decreases with increasing polytetrafluoroethylene (PTFE) loading and, in contrast, the greater is the PTFE loading in the MPL, the greater is the permeability. It has been shown that the in-plane permeability of the carbon substrates is reduced by an order of magnitude if they are coated with MPLs. Further, the permeability is different from one in-plane principal direction to another by a factor of about two. Finally, ignoring the inertial terms (for the reported flow rates) and the compressibility of the flowing air results in significant errors in the obtained values of the permeability.     

Pore network modeling of fibrous gas diffusion layers for polymer electrolyte membrane fuel cells

A pore network model of the gas diffusion layer (GDL) in a polymer electrolyte membrane fuel cell is developed and validated. The model idealizes the GDL as a regular cubic network of pore bodies and pore throats following respective size distributions. Geometric parameters of the pore network model are calibrated with respect to porosimetry and gas permeability measurements for two common GDL materials and the model is subsequently used to compute the pore-scale distribution of water and gas under drainage conditions using an invasion percolation algorithm. From this information, the relative permeability of water and gas and the effective gas diffusivity are computed as functions of water saturation using resistor-network theory. Comparison of the model predictions with those obtained from constitutive relationships commonly used in current PEMFC models indicates that the latter may significantly overestimate the gas phase transport properties. Alternative relationships are suggested that better match the pore network model results. The pore network model is also used to calculate the limiting current in a PEMFC under operating conditions for which transport through the GDL dominates mass transfer resistance. The results suggest that a dry GDL does not limit the performance of a PEMFC, but it may become a significant source of concentration polarization as the GDL becomes increasingly saturated with water.     

The impact of thermal conductivity and diffusion rates on water vapor transport through gas diffusion layers

Proper water management in a hydrogen-fueled polymer electrolyte membrane (PEM) fuel cell is critical for performance and durability. A mathematical model has been developed to elucidate the effect of thermal conductivity and water vapor diffusion coefficient in the gas diffusion layers (GDLs). The fraction of product water removed in the vapor phase through the GDL as a function of GDL properties/set of material and component parameters and operating conditions has been calculated. The current model enables identification of conditions wherein condensation occurs in each GDL component. The model predicts the temperature gradient across various components of a PEM fuel cell, providing insight into the overall mechanism of water transport in a given cell design. The water condensation conditions and transport mode in the GDL components depend on the combination of water vapor diffusion coefficients and thermal conductivities of the GDL components. Different types of GDLs and water transport scenarios are defined in this work, based on water condensation in the GDL and fraction of water that the GDL removes through the vapor phase, respectively.     

Water permeation analysis on gas diffusion layers of proton exchange membrane fuel cells for Teflon-coating annotation

This study presents an analysis of water permeation of a polytetrafluoroethylene (PTFE)-coated gas diffusion layer (GDL) to determine the influence of hydrophobic treatment on the GDL for diagnosis of water flooding. It is found that the behaviour of water drainage is controlled by the pore configuration instead of the hydrophobicity in GDL. Better water drainage is achieved by the action of the Teflon coating in modulating the GDL pore configuration to give both a larger average pore size and a wider distribution of pore size. The results show that water penetration through the GDL must overcome a threshold surface tension defined by the largest pore range. A 30 wt.% PTFE coating of a GDL is shown to generate a satisfactory pore configuration, explaining the improved cell polarization performance with a lower driven pressure (∼1.91 kPa) and a higher rate of water drainage.     

Microporous layer coated gas diffusion layers for enhanced performance of polymer electrolyte fuel cells

The influence of microporous layer (MPL) design parameters for gas diffusion layers (GDLs) on the performance of polymer electrolyte fuel cells (PEFCs) was clarified. Appropriate MPL design parameters vary depending on the humidification of the supplied gas. Under low humidification, decreasing both the MPL pore diameter and the content of polytetrafluoroethylene (PTFE) in the MPL is effective to prevent drying-up of the membrane electrode assembly (MEA) and enhance PEFC performance. Increasing the MPL thickness is also effective for maintaining the humidity of the MEA. However, when the MPL thickness becomes too large, oxygen transport to the electrode through the MPL is reduced, which lowers PEFC performance. Under high humidification, decreasing the MPL mean flow pore diameter to 3 μm is effective for the prevention of flooding and enhancement of PEFC performance. However, when the pore diameter becomes too small, the PEFC performance tends to decrease. Both reduction of the MPL thickness penetrated into the substrate and increase in the PTFE content to 20 mass% enhance the ability of the MPL to prevent flooding.     

Effect of polytetrafluoroethylene-treatment and microporous layer-coating on the electrical conductivity of gas diffusion layers used in proton exchange membrane fuel cells

The purpose of this study is to investigate the effect of ploytetrafluoroethylene (PTFE)-treatment and microporous layer (MPL)-coating on the electrical conductivity of gas diffusion layers (GDLs), as used in proton exchange membrane fuel cells (PEMFCs). The results show that, for PTFE-treated GDLs, the electrical conductivity in orthogonal in-plane directions is almost invariant with the PTFE loading. On the other hand, the in-plane conductivity of the MPL-coated GDL SGL 10BE (50% PTFE) was found to be higher than that of the counterpart SGL 10BC (25% PTFE) and this was explained by the presence of more conductive carbon particles in the MPL of SGL 10BE. Further, the conductivity of each GDL sample was measured in two perpendicular in-plane directions in order to investigate the in-plane anisotropy. The results show that the electrical conductivity of the GDL sample in one direction is different to that in the other direction by a factor of about two. The contact resistance, the main factor affecting the through-plane conductivity, of PTFE-treated GDLs shows a different trend to the corresponding in-plane conductivity, namely it increases as the PTFE loading increases. On the other hand, the contact resistance of the MPL-coated GDL SGL 10BE (50% PTFE) was found to be lower than that of the counterpart SGL 10BC (25% PTFE) and again this was explained by the presence of more conductive carbon particles in the MPL of SGL 10BE. Also, it was noted that the MPL coating appears to have a positive effect in reducing the contact resistance between the GDL and the bipolar plate. This is most likely due to the compressibility of the MPL layers that allows them to fill in the ‘gaps’ that exist in the surface of the bipolar plates and therefore establishes a good contact between the latter plates and the GDLs. Finally, good curve fitting of the contact resistance as a function of the clamping pressure has been achieved.     

Effect of liquid water on transport properties of the gas diffusion layer of polymer electrolyte membrane fuel cells

Water management in polymer electrolyte membrane (PEM) fuel cells is of importance due to its impact on the performance, durability and ultimately the cost of the cell. In the gas diffusion layer (GDL), liquid water has a direct effect on species and heat transport. The amount of liquid water in the GDL affects the relative permeability and capillary pressure, which govern the convective and diffusive transport of liquid water. Liquid water acts as a barrier to the diffusion of gases through the void region and facilitates in heat transfer. In this study, the full morphology model was used in order to investigate the effects of liquid water presence on the transport properties of the carbon paper GDL and examine the applicability of using various laws to estimate the transport properties in the presence of liquid water. The numerical results were compared against published experimental data. Further, the method of standard porosimetry was used to experimentally measure the effect of Teflon treatment on the capillary pressure of carbon paper. It was found that the addition of PTFE to the GDL results in the increase of capillary pressure; however, further increases to the PTFE loading did not result in additional changes to the capillary pressure.     

Utilization of 3D printed carbon gas diffusion layers in polymer electrolyte membrane fuel cells

3D printing and carbonisation is used to produce designed gas diffusion layer materials for polymer electrolyte membrane fuel cells (PEMFC). Using a desktop UV 3D printer, designed porous microstructures are printed with micro and macro-scale features. Successful improvement of the pyrolysis process maintains the structural accuracy during carbonisation, reducing the material to electrically conductive carbon. The size of the material allows for testing in a lab scale fuel cell with 1.5 × 1.5 cm electrode size, which shows lower but interesting electrochemical performance (power density of 205 mW cm^?2). Challenges associated with integration of a 3D printed structure into a membrane electrode assembly are highlighted, including the low open circuit voltage caused by large amounts of membrane deformation and subsequent hydrogen crossover. This study shows that it is possible to design and manufacture a gas diffusion layer for fuel cells. Numerical simulation on the new GDL structure shows that advective-diffusive transport of oxygen in the 3D printed design is superior to conventional carbon paper. This study serves as the first attempt to implement 3D printed microstructures as GDL into PEMFC.     

Porosity-graded micro-porous layers for polymer electrolyte membrane fuel cells

In this paper, the effect of porosity-graded micro-porous layer (GMPL) on the performance of polymer electrolyte membrane fuel cells (PEMFCs) was studied in detail. The GMPL was prepared by printing micro-porous layers (MPL) with different content of NH₄Cl pore-former and the porosity of the GMPL decreased from the inner layer of the MPLs at the membrane/MPL interface to the outer layer of the MPLs at the gas diffusion electrode/MPL interface. The morphology and porosity of the GMPLs were characterized and the performance of the cell with GMPLs was compared with those having conventional homogeneous MPLs. The result demonstrates that the fuel cells consisting of GMPL have better performance than those consisting of conventional homogeneous MPLs, especially at high current densities. Micro-porous layer with graded porosity is beneficial for the electrode process of fuel cell reaction probably by facilitating the liquid water transportation through large pores and gas diffusion via small pores in the GMPLs.     

Liquid water breakthrough pressure through gas diffusion layer of proton exchange membrane fuel cell

The dynamic behavior of liquid water transport through the gas diffusion layer (GDL) of the proton exchange membrane fuel cell is studied with an ex-situ approach. The liquid water breakthrough pressure is measured in the region between the capillary fingering and the stable displacement on the drainage phase diagram. The variables studied are GDL thickness, PTFE/Nafion content within the GDL, GDL compression, the inclusion of a micro-porous layer (MPL), and different water flow rates through the GDL. The liquid water breakthrough pressure is observed to increase with GDL thickness, GDL compression, and inclusion of the MPL. Furthermore, it has been observed that applying some amount of PTFE to an untreated GDL increases the breakthrough pressure but increasing the amount of PTFE content within the GDL shows minimal impact on the breakthrough pressure. For instance, the mean breakthrough pressures that have been measured for TGP-060 and for untreated (0 wt.% PTFE), 10 wt.% PTFE, and 27 wt.% PTFE were 3589 Pa, 5108 Pa, and 5284 Pa, respectively.     

In-plane gas permeability of proton exchange membrane fuel cell gas diffusion layers

A new analytical approach is proposed for evaluating the in-plane permeability of gas diffusion layers (GDLs) of proton exchange membrane fuel cells. In this approach, the microstructure of carbon papers is modeled as a combination of equally-sized, equally-spaced fibers parallel and perpendicular to the flow direction. The permeability of the carbon paper is then estimated by a blend of the permeability of the two groups. Several blending techniques are investigated to find an optimum blend through comparisons with experimental data for GDLs. The proposed model captures the trends of experimental data over the entire range of GDL porosity. In addition, a compact relationship is reported that predicts the in-plane permeability of GDL as a function of porosity and the fiber diameter. A blending technique is also successfully adopted to report a closed-form relationship for in-plane permeability of three-directional fibrous materials.     

Controlling gas diffusion layer oxidation by homogeneous hydrophobic coating for polymer electrolyte fuel cells

Reduced production costs and enhanced durability are necessary for practical application of polymer electrolyte fuel cells. There has been a great deal of concern about degradation of the gas diffusion layer located outside the membrane electrode assembly. However, very few studies have been carried out on the degradation process, and no suitable methods for improving the durability of the cell have been found.In this work, the influence on the cell performance and factors involved in the degradation of the gas diffusion layer has been clarified through power generation tests.Long-term power generation tests on single cells for 6000 h were carried out under high humidity conditions with homogeneous and inhomogeneous hydrophobic coating gas diffusion layers. The results showed that the increase in the diffusion overvoltage from the gas diffusion layer could be controlled by the use of a homogeneous coating. Post-analyses indicated that this occurred by controlling oxidation of the carbon fiber.     

Pore-network modeling of liquid water flow in gas diffusion layers of proton exchange membrane fuel cells

Fluid flow through the gas diffusion layer (GDL) of fuel cells is numerically studied using a pore network modeling approach. The model is developed based on an experimental visualization technique (fluorescence microscopy). The images obtained from this technique are analyzed to find patterns of flow inside the GDL samples with different hydrophobicity. Three different flow patterns are observed: initial invasion, progression, and pore-filling. The observation shows that liquid water flows into the majority of available pores on the boundary of the untreated GDL and several branches are segregated from the initial pathways. For the treated GDL, however, a handful of boundary pores are invaded and the original pathways extend toward the other side of the medium with minimum branching. The numerical model, developed based on an invasion percolation algorithm, is used to study the effects of GDL hydrophobicity and thickness on the flow configuration and breakthrough time as well as to determine the flow rate and saturation in different GDL samples. During the injection of water into the samples, it is numerically shown that the flow rates are monotonically decreasing for both treated and untreated samples. For the treated sample, however, the injection flow rate is constantly lower than that of the untreated sample, resulting in a lower overall water saturation at breakthrough. The numerical results also suggest that hydrophobic treatment of thick samples has minor effects on water management and overall performance. The developed model can be used to optimize the GDL properties for designing porous medium with effective transport characteristics.     

Effects of compression on mechanical integrity,gas permeability and thermal stability of gas diffusion layers with/without sealing gaskets

The compressibility, the gas permeability and the thermal stability of 4 commercially available uncoated GDLs (or carbon substrates) and MPL-coated GDLs are, with/without Teflon and silicone sealing gaskets, investigated before and after performing ex-situ compression tests mimicking the compressive stresses within the fuel cell. The results show that the gas permeability of the tested GDLs are impacted more with Teflon gaskets than with the silicone gaskets and this is due to the lower stiffness of the former gaskets. Likewise, the GDLs are more deformed with the Teflon gaskets than with silicone gaskets and this is due to the same reason mentioned above. The thermogravimetric analysis (TGA) data suggests that the bare carbon substrates, unlike the MPL-coated GDLs, lose up to 40% of the PTFE material after the compression test either with or without sealing gaskets.     

Transient,spatially resolved desaturation of gas diffusion layers measured via synchrotron visualization

The transient 3-D visualization of the desaturation process of flooded gas diffusion layers (GDLs) is presented for the first time. Desaturation rates and pathways are reported for two commercial GDL samples, one with a PTFE treatment and the other without. On-the-fly Synchrotron X-ray CT is performed while the GDL sample is subjected to a humidified or dry air flow stream to visualize the transient desaturation. The two humidification conditions assist in separating the convective and evaporative components of the desaturation process, showing a slight contribution from the convective effect, while the majority of the desaturation is due to evaporative removal. The convective removal is found to be insufficient to fully desaturate either GDL, with water remaining trapped underneath the channel rib with the more hydrophobic GDL and within the pore space in the more hydrophilic GDL. Stop-and-shoot Synchrotron X-ray computed tomography (CT) is then used in conjunction with program-assisted segmentation to determine initial saturation water volumes. These are then combined with the desaturation times found from the on-the-fly experiments to determine desaturation rates for both GDLs. The desaturation rate using dry air flow for the more hydrophobic GDL is found to be nearly four times faster than that of the more hydrophilic GDL. Results demonstrate that an evaporative contribution is necessary for either GDL sample to reach full desaturation.     

Pore structure and effective diffusion coefficient of catalyzed electrodes in polymer electrolyte membrane fuel cells

For polymer electrolyte membrane (PEM) fuel cells, the pore structure and small effective diffusion coefficient (EDC) of the catalyst layers have significant impact on the cell performance. In this study, both the pore structure and EDC of the catalyst layers are investigated experimentally; the pore structure of the catalyst layer is characterized by the method of standard porosimetry, and the EDC is measured by a modified Loschmidt cell for oxygen-nitrogen mixture through the catalyzed electrodes. It is found that Pt loading has a direct impact on the pore structure and consequently the EDC of the catalyzed electrodes. As the Pt loading is increased, the porosity and mean pore size of the catalyzed electrode decrease, and the EDC decreases accordingly, however, it is increased by 15–25% by increasing the temperature from 25 °C to 75 °C. The EDC of the catalyst layer is about 4.6 × 10^?7 m² s^?1 at 75 °C, compared with 25.0 × 10^?7 m² s^?1 for the uncatalyzed electrode at the same temperature.     

Effect of capillary pressure on liquid water removal in the cathode gas diffusion layer of a polymer electrolyte fuel cell

In order to investigate the effect of capillary pressure on the transport of liquid water in the cathode gas diffusion layer (GDL) of a polymer electrolyte fuel cell, a one-dimensional steady-state mathematical model was developed, including the effect of temperature on the capillary pressure. Numerical results indicate that the liquid water saturation significantly increases with increases in the operating temperature of the fuel cell. An elevated operating temperature has an undesirable influence on the removal of liquid water inside the GDL. A reported peculiar phenomenon in which the flooding of the fuel cell under a high operating temperature and an over-saturated environment is more serious in a GDL combined with a micro-porous layer (MPL) than in a GDL without an MPL [Lim and Wang, Electrochim. Acta 49 (2004), 4149–4156] is explained based on the present analysis.     

Study on water transport in hydrophilic gas diffusion layers for improving the flooding performance of polymer electrolyte fuel cells

For hydrogen-based polymer electrolyte fuel cells (PEFCs), water transport control in gas diffusion layers (GDLs) by wettability distribution is useful to suppress the flooding problem. In this study, the water transport of a novel GDL with hydrophilic-hydrophobic patterns was investigated. First, we clarified that the water motion in the hydrophilic GDL with microstructures could be reproduced by the enlarged scale model. The scale model experiment also showed that the same water behavior in hydrophilic GDL can be obtained from Capillary numbers (Ca) in a range of Ca ~ 10^?5 to 10^?3. As the computational load is inversely proportional to Ca, the computational load could be reduced by 1/100th by using Ca ~ 10^?3, which is 100 times higher than PEFC operation (Ca ~ 10^?5). Finally, the simulation with Ca ~ 10^?3 was performed, and we showed that the GDL with straight region of contact angle 50° minimized the water accumulation.