Numerical modeling and experimental study of the influence of GDL properties on performance in a PEMFC

This work is to study the effect of properties of gas diffusion layer (GDL) on performance in a polymer electrolyte membrane fuel cell (PEMFC) by both numerical simulation and experiments. The 1-dimension numerical simulation using the mixture-phase model is developed to calculate polarization curve. We are able to estimate optimum GDL properties for cell performance from numerical simulation results. Various GDLs which have different properties are prepared to verify accuracy of the simulation results. The contact angle and gas permeability of GDLs are controlled by polytetrafluoroethylene (PTFE) content in micro-porous layers (MPLs). MPL slurry is prepared by homogeneous blending of carbon powder, PTFE suspension, isopropyl alcohol and glycerol. Then the slurry is coated on gas diffusion mediums (GDMs) surface with controlled thickness by blade coating method. Non-woven carbon papers which have different thicknesses of 200 μm and 380 μm are used as GDMs. The prepared GDLs are measured by surface morphology, contact angle, gas permeability and through-plane electrical resistance. Moreover, the GDLs are tested in a 25 cm² single cell at 70 °C in humidified H₂/air condition. The contact angle of GDL increases with increasing PTFE content in MPL. However, the gas permeability and through-plane electrical conductivity decrease with increasing PTFE content and thickness of GDM. These changes in properties of GDL greatly influence the cell performance. As a result, the best performance is obtained by GDL consists of 200 μm thick non-woven carbon paper as GDM and MPL contained 20 wt.% PTFE content.     

Preparation of microporous layer for proton exchange membrane fuel cell by using polyvinylpyrrolidone aqueous solution

A new method of preparing microporous layer (MPL) for proton exchange membrane fuel cell (PEMFC) was presented in this paper. Considering the bad dispersion of PTFE aqueous suspension in the carbon slurry based on ethanol, polyvinylpyrrolidone (PVP) aqueous solution was used to prepare carbon slurry for microporous layer. The prepared gas diffusion layers (GDLs) were characterized by scanning electron microscopy, contact angle system and pore size distribution analyzer. It was found that the GDL prepared with PVP aqueous solution had higher gas permeability, as well as more homogeneous hydrophobicity. Moreover, the prepared GDLs were used in the cathode of fuel cell and evaluated with fuel cell performance and EIS analysis, and the GDL prepared with PVP aqueous solution indicated better fuel cell performance and lower ohmic resistance and mass transfer resistance.     

Influence of properties of gas diffusion layers on the performance of polymer electrolyte-based unitized reversible fuel cells

Polymer electrolyte-based unitized reversible fuel cells (URFCs) combine the functionality of a fuel cell and an electrolyzer in a single device. In a URFC, titanium (Ti)-felt is used as a gas diffusion layer (GDL) of the oxygen electrode, whereas typical carbon paper is used as a GDL of the hydrogen electrode. Different samples of Ti-felt with different structural properties (porosity and fiber diameter) and PTFE content were prepared for use as GDLs of the oxygen electrode, and the relation between the properties of the GDL and the fuel cell performance was examined for both fuel cell and electrolysis operation modes. Experimental results showed that the cell with a Ti-felt GDL of 80 μm fiber diameter had the highest round-trip efficiency due to excellent fuel cell operation under relatively high-humidity conditions despite degradation in performance in the electrolysis mode.     

Application of hyperdispersant to the cathode diffusion layer for direct methanol fuel cell

In this study, Nafion ionomer, as a kind of hyperdispersant, was added to polytetrafluoroethylene (PTFE) water dispersion system to suppress the size of PTFE particles in the ink of microporous layer (MPL). The agglomeration behavior of PTFE in ethanol and MPL were investigated by laser diffraction, dynamic light scattering (DLS) and metallurgical microscopes. The electronic resistance, pore size distribution, gas permeability and surface hydrophobic/hydrophilic properties were also characterized for prepared gas diffusion layers (GDLs). It was shown that PTFE water dispersion system suffered flocculating when dispersed in ethanol and this agglomeration behavior was reduced by employing Nafion ionomer. With the increase in the Nafion ionomer adopted in the MPL, not only the decreased hydrophobic property was shown in the MPL, but the decreased PTFE particle size was also achieved, which results in improved crosslink of carbon and pores themselves as well as the volume loss of pores in micron scale. The increased gas permeability and electronic conductivity of the GDL made the one employing the PTFE dispersion system with 1% Nafion content own its advantages as the cathode diffusion layer for a direct methanol fuel cell (DMFC) under near-ambient conditions.     

Effects of gas diffusion layer structure on the open circuit voltage and hydrogen crossover of polymer electrolyte membrane fuel cells

The clamping pressure of polymer electrolyte membrane fuel cells for vehicle applications should be typically high enough to minimize contact resistance. However, an excessive compression pressure may cause a durability problem. In this study, the effects of gas diffusion layer (GDL) structure on the open circuit voltage (OCV) and hydrogen crossover have been closely examined. Results show that the performances of fuel cells with GDL-1 (a carbon fiber felt substrate with MPL having rough surface) and GDL-3 (a carbon fiber paper substrate with MPL having smooth surface) are higher than that with GDL-2 (a carbon fiber felt substrate with MPL having smooth surface) under low clamping torque conditions, whereas when clamping torque is high, the GDL-1 sample shows the largest decrease in cell performance. Hydrogen crossover for all GDL samples increases with the increase of clamping torque, especially the degree of increase of GDL-1 is much greater than that of the other two GDL samples. The OCV reduction of GDL-1 is much greater than that of GDL-2 and GDL-3. It is concluded that the GDL-3 is better than the other two GDLs in terms of fuel cell durability, because the GDL-3 shows the minimum OCV reduction.     

Effect of fiber orientation on Liquid–Gas flow in the gas diffusion layer of a polymer electrolyte membrane fuel cell

In this study, the lattice Boltzmann method was used to simulate the three-dimensional intrusion process of liquid water in the gas diffusion layer (GDL) of a polymer electrolyte membrane fuel cell (PEMFC). The GDL was reconstructed by the stochastic method and used to investigate fiber orientation's influence on liquid water transport in the GDL of a PEMFC. The fiber orientation can be described by the angle between a single fiber and the in-plane direction; three different samples were simulated for three different fiber orientation ranges. The simulated permeability correlated well with the anisotropic characteristics of reconstructed carbon papers. It was concluded that the fiber orientation had a significant effect on the liquid invasion pattern in the GDL by changing the pore shape and distribution of the GDL. The results indicated that the stochastically reconstructed GDL, taking into account the fiber orientation, better demonstrates the mass transport properties of the GDL.     

Effect of PTFE loading of gas diffusion layers on the performance of proton exchange membrane fuel cells running at high‐efficiency operating conditions

In this paper, the effects of microporous layer (MPL) addition and polytetrafluoroethylene (PTFE) loading of gas diffusion layers (GDLs) on the overall performance of the proton exchange membrane fuel cell have been investigated. The focus was on fuel cells that operate at relatively low current densities where the power demand is low, but the efficiency is of concern. The results show that, in the activation loss‐controlled region, the performance of the fuel cell operating with moderately PTFE‐treated carbon substrates is superior over that operating with coated GDLs. This is due to the addition of the MPL which lengthens the diffusion paths and significantly reduces the mass transport properties. Conversely, in the ohmic loss‐controlled region, the fuel cell with coated GDLs performs better than those with carbon substrates. This is explained by the enhanced contact of the GDL with the adjacent components after the MPL addition, which outweighs the negative effects associated with the activation loss‐controlled region. Also, it was found that the fuel cell performance becomes lower if the GDL is treated with a relatively high PTFE loading in either the carbon substrate (due to the decrease in the porosity of the GDL) or the MPL. Copyright © 2012 John Wiley & Sons, Ltd.     

Degradation of gas diffusion layers through repetitive freezing

This work investigates the degradation of an individual gas diffusion layer (GDL) by repeated freezing cycles. The pore size distribution, gas permeability, surface structure, and contact angle on the surface of the GDL were measured in four different types of GDL: SGL paper with a microporous layer (MPL); SGL paper with 5 wt% of polytetrafluoroethylene (PTFE) loading; Toray paper without PTFE loading; and Toray paper with 20 wt% of PTFE loading. After repeated freezing cycles, the porosity of the GDL without PTFE was reduced by 27.2% due to the volumetric expansion of the GDL. The peak of the log differential intrusion moved toward a smaller pore diameter slightly because of the repeated freezing process. The crack of the MPL increased in its width and length after repeated freezing cycles. The through-plane gas permeability of the GDL with the MPL doubled after repeated freezing cycles due to the growth of the crack in the MPL, but was very small for the GDLs with Toray paper. Besides, the GDLs with PTFE loading showed a relatively larger decrease in the contact angle on the surface than the GDL without PTFE loading due to the separation of PTFE from the carbon fiber during the repeated freezing process.     

Measurement of water transport rates across the gas diffusion layer in a proton exchange membrane fuel cell,and the influence of polytetrafluoroethylene content and micro-porous layer

Water management in a proton exchange membrane (PEM) fuel cell is one of the critical issues for improving fuel cell performance and durability, and water transport across the gas diffusion layer plays a key role in PEM fuel cell water management. In this work, we investigated the effects of polytetrafluoroethylene (PTFE) content and the application of a micro-porous layer (MPL) in the gas diffusion layer (GDL) on the water transport rate across the GDL. The results show that both PTFE and the MPL play a similar role of restraining water transport. The effects of different carbon loadings in the MPL on water transport were also investigated. The results demonstrate that the higher the carbon loading in the MPL, the more it reduces the water transport rate. Using the given cell hardware and components, the optimized operation conditions can be obtained based on a water balance analysis.     

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.     

Experimental characterization of in-plane permeability of gas diffusion layers

Recent studies indicate that PEM fuel cell performance may be strongly influenced by in-plane permeability of the gas diffusion layer (GDL). The current study employs a radial flow technique for obtaining in-plane permeability of GDLs, using either gas or liquid as the impregnating fluid. A model has been developed and experimentally verified to account for compressibility effects when permeability measurements are conducted using a gas. Permeability experiments are performed on samples of woven, non-woven, and carbon fiber-based GDL at various levels of compression using air as the impregnating fluid. Woven and non-woven samples are measured to have significantly higher in-plane permeability compared to carbon fiber paper at similar solid volume fractions.     

Impact of PTFE distribution on the removal of liquid water from a PEMFC electrode by lattice Boltzmann method

It is believed by many that polymer electrolyte membrane fuel cells (PEMFCs) will have a widespread application since they offer important features such as low operating temperature, high power density, and easy scale up. However, operation of PEMFCs is faced with some technical challenges including water management which may lead to flooding of the electrodes. Treatment of the gas diffusion layer (GDL) with a highly hydrophobic material such as PTFE is a common strategy for mitigating this issue. Several investigations have been done to clarify solely the effect of PTFE content. However, effects of PTFE distribution, which can be achieved through different treatment methods, has not been well studied yet. Lattice Boltzmann method (LBM) is one of the best choices for such numerical studies due to its capability of modeling multiphase flow in the complicated microstructure of a porous GDL considering its non-homogeneous and anisotropic transport properties. In the present study, droplet removal from four GDLs with different PTFE distributions through an interdigitated flow field is investigated using LBM. The results demonstrate that regardless of PTFE distribution, the interfacial forces between any untreated carbon fiber and a water droplet will strongly dominate over other forces and hence will prevent its removal. Therefore, it is concluded that an effective water management may be achieved by a suitable treatment method such that no carbon fiber inside the GDL remains uncoated.     

Effects of basic gas diffusion layer components on PEMFC performance with capillary pressure gradient

The gas diffusion layer (GDL) is composed of a substrate and a micro-porous layer (MPL), and is treated with polytetrafluoroethylene (PTFE) to promote water discharge. Additionally, the MPL mainly consists of carbon black and PTFE. In other words, the optimal design of these elements has a dominant effect on the polymer electrolyte membrane fuel cell (PEMFC) performance. For the GDL, it is crucial to prevent water flooding, and the water flux within the GDL is strongly affected by the capillary pressure gradient. In this study, the PEMFC performance was systematically investigated by varying the substrate PTFE content, MPL PTFE content, and MPL carbon loading per unit area. The effects of each experimental variable on the PEMFC performance and especially on the capillary pressure gradient were quantitatively analyzed when the GDLs were manufactured by the doctor blade manufacturing method. The experimental results indicated that as the PTFE content of the anode and cathode GDL increased, the PEMFC performance deteriorated due to the deformation of the porosity and tortuosity of the GDL. Additionally, the PEMFC performance improved as the MPL PTFE content of the cathode GDL increased at low relative humidity (RH), but the PEMFC performance tendency was reversed at high RH. Further, the MPL carbon loading of 2 mg/${\text{cm}}^2$ demonstrated the best performance, and the advantages and disadvantages of the MPL carbon loading were identified. In addition, the effects of each experimental variable on liquid water, water vapor, and gas permeability were investigated.     

Through-plane gas permeability of gas diffusion layers and microporous layer: Effects of carbon loading and sintering

Knowledge of the absolute permeability for the various porous layers is necessary to obtain accurate profiles for water saturation within the membrane electrode assembly (MEA) in a two-phase model of a polymer electrolyte membrane fuel cell (PEMFC). In this paper, the gas permeability of gas diffusion layers (GDLs) coated with microporous layers (MPLs) of various carbon loadings for two different carbon blacks have been experimentally measured. The permeability of the GDL was found to decrease by at least one order of magnitude after the MPL-coating. Also, the permeability of the MPLs was shown to be lower than that of the carbon substrate by 2–3 orders of magnitude. Further, it was found that the gas permeability of the MPLs changes significantly from one carbon loading to another despite the use of a single weight composition for all the MPLs coated, namely 20% PTFE and 80% carbon black. This signifies the possible inaccuracy in estimating the MPL permeability through employing the cross-section SEM images as they do not resolve the MPL penetration into the carbon substrate. Finally, the MPL sintering was found to slightly decrease the permeability of the GDL.     

Examination of the influence of PTFE coating on the properties of carbon paper in polymer electrolyte fuel cells

Polymer electrolyte fuel cells gain momentum due to the attainable high power densities and their relatively simple handling. Because their actual reactive catalytic layer is about < 10 μm, carbon papers are frequently used as additional backing in order to improve the gas distribution and water management in the fuel cell. To avoid flooding of the electrodes by the product water, the carbon paper is usually hydrophobed by partial coating with PTFE suspension. The influence of the PTFE coating and the following sintering time on through paper plane conductivity, gas permeability and paper hydrophobicity is analysed and discussed.     

Optimization of GDLs for high-performance PEMFC employing stainless steel bipolar plates

The effects of polytetraflouroethylene (PTFE) content in the gas diffusion layer (GDL) on the performance of PEMFCs with stainless-steel bipolar plates are studied under various operation conditions, including relative humidity, cell temperature, and gas pressure. The optimal PTFE content in the GDL strongly depends on the cell temperature and gas pressure. Under unpressurized conditions, the best cell performance was obtained by the GDL without PTFE, at a cell temperature of 65 °C and relative humidity (RH) of 100%. However, under the conditions of high cell temperature (80 °C), low RH (25%) and no applied gas pressure, which is more desirable for fuel cell vehicle (FCV) applications, the GDL with 30 wt.% PTFE shows the best performance. The GDL with 30 wt.% PTFE impedes the removal of produced water and increases the actual humidity within the membrane electrode assembly (MEA). A gas pressure of 1 bar in the cell using the GDL with 30 wt.% PTFE greatly improves the performance, especially at low RH, resulting in performance that exceeds that of the cell under no gas pressure and high RH of 100%.     

Investigation of sintered stainless steel fiber felt as gas diffusion layer in proton exchange membrane fuel cells

The feasibility of using sintered stainless steel fiber felt (SSSFF) as gas diffusion layer (GDL) in proton exchange membrane fuel cells (PEMFCs) is evaluated in this study. The SSSFF is coated with an amorphous carbon (a-C) film by closed field unbalanced magnetron sputter ion plating (CFUBMSIP) to enhance the corrosion resistance and reduce the contact resistance. The characteristics of treated SSSFF, including microscopic morphology, mechanical properties, electrical conductivity, electrochemical behavior and wettablity characterization, are systematically investigated and summarized according to the requirements of GDL in PEMFC. A membrane electrode assembly (MEA) with a-C coated SSSFF-15 GDL is fabricated and assembled with a-C coated stainless steel bipolar plates in a single cell. The initial peak power density of the single cell is 877.8 mW cm⁻² at a current density of 2324.9 mA cm⁻². Lifetime test of the single cell over 200 h indicates that the a-C coating protects the SSSFF-15 GDL from corrosion and decreases the performance degradation from 30.6% to 6.3%. The results show that the SSSFF GDL, enjoying higher compressive modulus and ductility, is a promising solution to improve fluid permeability of GDL under compression and PEMFC durability.     

Highly efficient single-layer gas diffusion layers for the proton exchange membrane fuel cell

In the present study, a series of highly efficient single-layer gas diffusion layers (SL-GDLs) was successfully prepared by the addition of a vapor grown carbon nanofiber (VGCF) in the carbon black/poly(tetrafluoroethylene) composite-based SL-GDL through a simple and inexpensive process. The scanning electron micrographs of the as-prepared VGCF-containing SL-GDLs (SL-GDL-CFs) showed that the GDLs had a microporous layer (MPL)-like structure, while the wire-like VGCFs were well dispersed and crossed among the carbon black particles in the SL-GDL matrix. Utilization of the SL-GDL-CFs for MEA fabrication was also done by direct coating with the catalyst layer. Due to the presence of VGCFs, the properties of the SL-GDL-CFs, including electronic resistivity, mechanical characteristic, gas permeability, and water repellency, varied with the VGCF content, with the overall effect beneficial to the performance of the proton exchange membrane fuel cell (PEMFC). The best performances obtained from the PEMFC with VGCFs at 15 wt.% was approximately 63% higher than those without VGCFs, and about 85% as efficient as ELAT GDL, a commercial dual-layer GDL, for both the H₂/O₂ and H₂/air systems.     

Characterization of transport properties in gas diffusion layers for proton exchange membrane fuel cells: 2. Absolute permeability

This is the second in a series of papers in which we present methods demonstrated in our group for the estimation of transport properties in gas diffusion layers (GDLs) for proton exchange membrane fuel cells (PEMFCs). Here we describe a method for determining separately the in-plane (x, y-directions) and through-plane (z-direction), viscous and inertial permeability coefficients of macro-porous substrates and micro-porous layers by controlling the direction of the gas flow through the porous sample. The method is applied initially to the macro-porous substrate of the GDL alone and subsequently to the macro-porous substrate with different micro-porous layers applied on it. The permeability coefficients of the micro-porous layer are calculated from the two measurements. The permeability coefficients are calculated from the Darcy–Forchheimer equation by application of the method of least squares. The method was applied to GDLs having different contents of polytetrafluoroethylene (PTFE) and carbon types. The samples with a higher PTFE content have in-plane and through-plane viscous permeability coefficients higher than those of the samples with lower PTFE content. The in-plane and through-plane viscous permeability coefficients also depend on the carbon type.     

Stochastic modeling and direct simulation of the diffusion media for polymer electrolyte fuel cells

This paper combines the stochastic-model-based reconstruction of the gas diffusion layer (GDL) of polymer electrolyte fuel cells (PEFCs) and direct simulation to investigate the pore-level transport within GDLs. The carbon-paper-based GDL is modeled as a stack of thin sections with each section described by planar two-dimensional random line tessellations which are further dilated to three dimensions. The reconstruction is based on given GDL data provided by scanning electron microscopy (SEM) images. With the constructed GDL, we further introduce the direct simulation of the coupled transport processes inside the GDL. The simulation considers the gas flow and species transport in the void space, electronic current conduction in the solid, and heat transfer in both phases. Results indicate a remarkable distinction in tortuosities of gas diffusion passage and solid matrix across the GDL with the former ～1.2 and the latter ～13.8. This difference arises from the synthetic microstructure of GDL, i.e. the lateral alignment nature of the thin carbon fiber, allowing the solid-phase transport to occur mostly in lateral direction. Extensive discussion on the tortuosity is also presented. The numerical tool can be applied to investigate the impact of the GDL microstructure on pore-level transport and scrutinize the macroscopic approach vastly adopted in current fuel cell modeling.