Predicting transport parameters in PEFC gas diffusion layers considering micro‐architectural variations using the Lattice Boltzmann method

A deep understanding of the behavior of microstructural parameters in proton exchange fuel cells (PEFCs) will help to reduce the material cost and to predict the performance of the device at cell scale. Changes in morphological configuration, that is, fiber diameter and fiber orientation, of the gas diffusion layers (GDLs) result in variations of fluid behavior throughout the layer, and therefore, the microstructural parameters are affected. The aim of this study is to analyze, for three selected fiber diameters and different percentage presence of inclined fibers, the behavior of the different microstructural parameters of the GDLs. This study is carried out over digitally created two‐dimensional GDL models, in which the fluid behavior is obtained by means of the lattice Boltzmann method. Once the fluid behavior is determined, the microstructural parameters, that is, the porosity, gas‐phase tortuosity, obstruction factor, through‐plane permeability, and inertial coefficient, are computed. Several relationships are found to predict the behavior of such parameters as function of the fiber diameter, presence of inclined rods, or porosity. The results presented in this work are compared and validated by previous theoretical and experimental studies found in the literature. Copyright © 2016 John Wiley & Sons, Ltd.     

In-plane and through-plane gas permeability of carbon fiber electrode backing layers

The absolute gas permeability of several common gas diffusion layer (GDL) materials for polymer electrolyte membrane fuel cells was measured. Measurements were made in three perpendicular directions to investigate anisotropic properties. Most materials were found to display higher in-plane permeability than through-plane permeability. The permeability in the two perpendicular in-plane directions was found to display significant anisotropy. Materials with the most highly aligned fibers showed the highest anisotropy and the permeability could differ by as much as a factor of 2. In-plane permeability was also measured as the GDL was compressed to different thicknesses. Typically, compression of a sample to half its initial thickness resulted in a decrease in permeability by an order of magnitude. Since the change in GDL thickness during compression can be converted to porosity, the relationship between measured permeability and porosity was compared to various models available in the literature, one of which allows the estimation of anisotropic tortuosity. The effect of inertia on fluid flow was also determined and found to vary inversely with permeability, in agreement with available correlations. The results of this work will be useful for 3D modeling studies where knowledge of permeability and effective diffusivity tensors is required.     

Gas diffusion through differently structured gas diffusion layers of PEM fuel cells

Proton exchange membrane fuel cell (PEMFC) gas diffusion layers (GDLs) play important parts in diffusing gas, discharging liquid water, and conducting electricity, etc. When liquid water is discharged through GDL to gas channel, there will be some pores of GDLs occupied by liquid water. In this study, based on a one-dimensional model, the distribution of liquid water phase saturation is analyzed for different GDL structures including GDL with uniform porosity, GDL with sudden change porosity (GDL with microporous layer (MPL)) and GDL with gradient porosity distribution. The effect on gas diffusion of the changes of porosity and liquid saturation due to water remaining in GDL pores is calculated. The conclusions are that for uniform porosity GDL, the gas diffusion increases with the increase of porosity and contact angle and increases with the decrease of the thickness of GDL; for GDL with MPL, the larger the MPL porosity and the thinner the MPL thickness are, the stronger the gas diffusion is; for gradient change porosity GDL with the same average equivalent porosity, the larger the porosity gradient is, the more easily the gas diffuses. The optimization for GDL gradient structure shows that the GDL with a linear porosity distribution of 0.4x+0.4$0.4x+0.4$ is the best of the computed cases.     

Numerical study on the compression effect of gas diffusion layer on PEMFC performance

A numerical method is developed to study the effect of the compression deformation of the gas diffusion layer (GDL) on the performance of the proton exchange membrane fuel cell (PEMFC). The GDL compression deformation, caused by the clamping force, plays an important role in controlling the performance of PEMFC since the compression deformation affects the contact resistance, the GDL porosity distribution, and the cross-section area of the gas channel. In the present paper, finite element method (FEM) is used to first analyze the ohmic contact resistance between the bipolar plate and the GDL, the GDL deformation, and the GDL porosity distribution. Then, finite volume method is used to analyze the transport of the reactants and products. We investigate the effects of the GDL compression deformation, the ohmic contact resistivity, the air relative humidity, and the thickness of the catalyst layer (CL) on the performance of the PEMFC. The numerical results show that the fuel cell performance decreases with increasing compression deformation if the contact resistance is negligible, but an optimal compression deformation exists if the contact resistance is considerable.     

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.     

A fractal permeability model for the gas diffusion layer of PEM fuel cells

In this paper a fractal permeability model for the gas diffusion layer (GDL) of PEM fuel cells (PEMFCs) is presented. The model accounts for the actual microstructures of the GDL in terms of two fractal dimensions, one relating the size of the capillary flow pathways to their population and the other describing the tortuosity of the capillary pathways. In addition, the gas molecule effect is considered by using the Adzumi equation. The fractal permeability model is found to be a function of the tortuosity fractal dimension, pore area fractal dimension, sizes of pore and the effective porosity of porous medium without any empirical constants. mercury-intrusion porosimetry was used to measure the microstructures of the GDL. Based on scanning electron microscope (SEM) images, two fractal dimensions are determined by the box-counting method. To verify the validity of the model, the predicted permeability data of the present fractal model were compared with the experimental data supplied by Toray Inc. It is found that the permeability prediction of the model was in accordance with experimental data. This verifies the validity of the present fractal permeability model for the GDL.     

Investigation of effects of non‐homogenous deformation of gas diffusion layer in a PEM fuel cell

Proton exchange membrane fuel cells have been promoted due to improved breakthrough and increased commercialization. The assembly pressure put on a single cell and a fuel cell stack has important influence on the geometric deformation of the gas diffusion layers (GDLs) resulting in a change in porosity, permeability, and the resistance for heat and charge transfer in proton exchange membrane fuel cells. In this paper, both the finite element method and the finite volume method are used, respectively, to predict the GDL deformation and associated effects on the geometric parameters, porosity, mass transport property, and the cell performance. It is found that based on the isotropic Young's modulus and the finite element method, the porosity and thickness under a certain assembly pressure are non‐homogeneous across the fuel cell in the in‐plane direction. The variations of the porosity change and compression ratio in the cross‐section plane are localized by three zones, that is, a linear porosity zone, a constant porosity zone, and a nonlinear porosity zone. The results showed that the GDL porosity and compression ratios maintain linear and nonlinear changes in the zone above the shoulders and the zone under the channel but close to the shoulder, respectively. However, a constant value is kept above the middle of the channel. The obtained non‐homogeneous porosity distribution is applied together with the deformed GDL for further computational fluid dynamics analysis, in which the finite volume method is implemented. The computational fluid dynamic results reveal that a higher assembly pressure decreases the porosity, GDL thickness, gas flow channel cross‐sectional areas, oxygen diffusion coefficient, oxygen concentration, and cell performance. The maximum oxygen mole fraction occurs where the maximum porosity exists. A sufficient GDL thickness is required to ensure transfer of fresh gas to the reaction sites far away from the channel. However, the reduction of porosity is a dominating factor that decreases the cell performance compared with the decreased gas channel flow area and GDL thickness in the assembly condition. Therefore, the assembly pressure should be balanced to consider both the cell performance and gas sealing security. Copyright © 2017 John Wiley & Sons, Ltd.     

Two-phase transport in the cathode gas diffusion layer of PEM fuel cell with a gradient in porosity

Two-phase transport in the cathode gas diffusion layer (GDL) of a proton exchange membrane fuel cell (PEMFC) is studied with a porosity gradient in the GDL. The porosity gradient is formed by adding micro-porous layers (MPL) with different carbon loadings on the catalyst layer side and on the flow field side. The multiphase mixture model is employed and a direct numerical procedure is used to analyze the profiles of liquid water saturation and oxygen concentration across the GDL as well as the resulting activation and concentration losses. The results show that a gradient in porosity will benefit the removal rate of liquid water and also enhance the transport of oxygen through the cathode GDL. The present study provides a theoretical support for the suggestion that a GDL with porosity gradient will improve the cell performance.     

Thermal management in PEMFCs: The respective effects of porous media in the gas flow channel

This study aims to evaluate the convective heat transfer enhancement of the proton exchange membrane fuel cells (PEMFC) numerically. As the higher heat transfer surfaces lead to higher heat transfer rates, a flat plate porous layer is utilized in the gas flow channel (GFC). This enhancement in heat transfer stems from the corresponding modification in the temperature and velocity profiles. The influencing parameters on these profiles are the thickness, permeability, and porosity of the GFC porous layer. After performing the simulations, the results indicate that convective heat transfer has a direct relationship with GFC porous layer's thickness and permeability. However, lower values of porosity lead to the higher Nusselt numbers. Previous investigations have also mentioned the positive impact of the microporous layer (MPL) on the water management of these fuel cells. Therefore, six different sizes of MPL and the gas diffusion layer (GDL) are utilized to evaluate their impacts on the thermal management. Results indicate that although these sizes have negligible effects on the heat transfer, Nu increases by enhancing the total size of MPL and GDL. The results also show that thicker MPLs lead to higher heat transfer rates. The evaluation of the friction factor also indicates the adverse effect of the GFC porous layer, although this undesirable effect is negligible. Finally, all the simulated values are utilized to train an artificial neural network (ANN) model with high precision. This ANN model can produce more data for sensitivity analysis and presenting respective 3D diagrams of the influencing parameters on heat transfer.     

Lattice Boltzmann simulations of anisotropic permeabilities in carbon paper gas diffusion layers

The multiple-relaxation-time (MRT) lattice Boltzmann method (LBM) with multi-reflection solid boundary conditions is used to study anisotropic permeabilities of a carbon paper gas diffusion layer (GDL) in a fuel cell. The carbon paper is reconstructed using the stochastic method, in which various porosities and microstructures are achieved to simulate different samples. The simulated permeability and tortuosity show anisotropic characteristics of the reconstructed carbon papers with in-plane permeability higher than through-plane, and in-plane tortuosity lower than through-plane. The calculated permeabilities are in good agreement with existing measurements. The relationship between the permeability and the porosity is fitted with empirical relations and some fitting constants are determined. Furthermore, the obtained relationship of tortuosity and porosity is used in a fractal model for permeabilities. The results indicate that the fractal model and the Kozeny–Carman equation provide similar predictions on the through-plane permeability of the carbon paper GDL.     

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.     

Parametric study of the porous cathode in the PEM fuel cell

The electrochemical behavior and the reactant transport in the porous gas diffusion layer (GDL) and catalyst layer (CL) are controlled by a large number of parameters such as porosity, permeability, conductivity, catalyst loading, and average pore size, etc. A three‐dimensional polymer electrolyte membrane fuel cell model is developed. The model accounts for the mass, fluid, and thermal transport processes as well as the electrochemical reaction. Using this model, the effects of the various porous electrode design parameters including porosity, solid electronic conductivity, and thermal conductivity of cathode GDL, and the catalyst loading, average pore size of cathode CL are investigated through parametric study. The model is shown to agree well with the experimental data of some porous electrode specifications. In addition, the model shows promise as a tool for optimizing the design of fuel cells. Copyright © 2008 John Wiley & Sons, Ltd.     

Diffusion parameter correlations for PEFC gas diffusion layers considering the presence of a water-droplet

A polymer electrolyte fuel cell (PEFC) produces electrical energy according to the electrochemical reactions carried out inside the cell. During the energy conversion, water molecules are also produced at the cathode side, which affects the gas diffusion layer (GDL) diffusion parameters. The generated water-drops from the reaction may give partial or total blockage of the reactant gases and also material oxidation. The mentioned phenomena influence the performance of the PEFCs. This paper aims to describe and quantify the impact on diffusion parameters of GDLs when the size of the formed water-drops inside the layer is varying. This study considers digitally generated GDLs, in which the porosity, gas-phase tortuosity and diffusibility are studied. The fluid flow behavior through the three-dimensional porous domain representing the GDL is obtained with the lattice Boltzmann method (LBM). Depending on the water-drop size, the impact of the mentioned parameters can be computed. For the current study a spherical water-drop whose radius varies between the 15 and 35% of the size of the domain was considered. The studied parameters showed a dependency of the water-drop radius, each changing independently and several correlations to predict the behavior of the mentioned diffusion transport parameters are proposed.     

Microstructure reconstruction and characterization of PEMFC electrodes

We reconstruct a proton exchange membrane fuel cell (PEMFC) catalyst layer (CL) and a non-woven carbon paper gas diffusion layer (GDL) by specially-designed stochastic methods. The reconstructed microstructures evidently distinguish all the participating components in the composite GDL/CL. Characterization analyses with respect to the reconstructed GDL/CL give important structural properties such as geometrical connectivity of an individual phase, pore size distribution, and volume-specific interfacial area. Self-developed Lattice Boltzmann (LB) models are established to calculate effective transport physical properties including effective thermal/electric conductivity and effective species diffusivity of the reconstructed GDL/CL, and permeability of the reconstructed GDL. Accordingly, we obtain tortuosity values for pore or solid phase in the reconstructed GDL/CL.     

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.     

Numerical study for in-plane gradient effects of cathode gas diffusion layer on PEMFC under low humidity condition

A numerical study about in-plane porosity and contact angle gradient effects of cathode gas diffusion layer (GDL) on polymer electrolyte membrane fuel cell (PEMFC) under low humidity condition below 50% relative humidity is performed in this work. Firstly, a numerical model for a fuel cell is developed, which considers mass transfer, electrochemical reaction, and water saturation in cathode GDL. For water saturation in cathode GDL, porosity and contact angle of GDL are also considered in developing the model. Secondly, current density distribution in PEMFC with uniform cathode GDL is scrutinized to design the gradient cathode GDL. Finally, current density distributions in PEMFC with gradient cathode GDL and uniform cathode GDL are compared. At the gas inlet side, the current density is higher in GDL with a gradient than GDL with high porosity and large contact angle. At the outlet side, the current density is higher in GDL with a gradient than GDL with low porosity and small contact angle. As a result, gradient cathode GDL increases the maximum power by 9% than GDL with low porosity and small contact angle. Moreover, gradient cathode GDL uniformizes the current density distribution by 4% than GDL with high porosity and large contact angle.     

Parameter sensitivity examination for a complete three-dimensional,two-phase,non-isothermal model of polymer electrolyte membrane fuel cell

Parameter sensitivity analysis is carried out for a complete three-dimensional, two-phase, non-isothermal model of polymer electrolyte membrane (PEM) fuel cell with a parallel flow field design. The model couples the two-phase flow of the multi-component reactants and liquid water, species transport, electrochemical reactions, proton and electron transport, and the electro-osmosis transport, back diffusion of water in the membrane, and energy transport. Twenty nine parameters, which are classified into the structural or transport parameters of porous layers (tortuosity, porosity, permeability, proton conductivity, electron conductivity, and thermal conductivity) as well as the electrochemical parameters (anodic and cathodic exchange current densities, anodic and cathodic transfer coefficients for anode and cathode reactions), are used to implement individual parameter investigation. The results show the parameters can be divided in to strongly sensitive, conditional sensitive and weak sensitive parameters according to its effect on the cell polarization curve. The optimization of parameters of cathode gas diffusion layer (GDL) and catalyst layer (CL) is more important to improve cell performance than that of anode GDL and CL because liquid water transport and removal affect significantly membrane hydration and reactant transport. Electrochemical parameters determine the activation potential and the slope of ohmic polarization hence these parameters can be used to fit experimental polarization curve more effectively than the other parameters.     

Feasibility of periodic surface models to develop gas diffusion layers: A gas permeability study

A geometric modeling scheme called periodic surface model (PS) is used to construct three dimensional (3D) models of a gas diffusion layer's (GDL) microstructure, which allows for rapid model construction and modification of representative volume elements (RVE) with embedded periodic boundary conditions. The reconstructed PS models are optimized with the help of the genetic algorithm embedded in MATLAB to generate models with refined mesh for computational fluid dynamics (CFD) analysis. The GDL geometry is built in ANSYS/ICEM CFD, automatically, using a customized code that couples MATLAB and ICEM. To verify the validity of the suggested modeling approach the microstructures of the GDLs with different porosity and fiber orientation are generated and the in-plane and through-plane permeability and tortuosity are calculated using ANSYS/FLUENT software. The numerically predicted values of in-plane and through-plane permeability are compared to experimental measurements. Using the genetic algorithm significantly decreases the fibers intersection volume in the RVE, especially as porosity decreases. It has been found that the tortuosity of the GDL is a function of the spatial orientation of the fibers in the RVE, when the fibers are at a small angle, the in-plane tortuosity can be higher than the through-plane tortuosity.     

Numerical study on permeability of gas diffusion layer with porosity gradient using lattice Boltzmann method

In this paper, the lattice Boltzmann method (LBM) has been employed to explore the permeability and internal fluid flow behavior of the gas diffusion layer (GDL). Three different non-uniform porosity distributions are designed as linear type, stepped type, and transitional type and compared with constant porosity samples. Results show that the linear porosity gradient distribution leads to higher permeability values compared with the other two types. For samples with total porosity of 0.65 and 0.75, optimal porosity gradient distributions bring about an enhancement of permeability have been found. The impact of porosity gradient distribution on the velocity field is presented. Dependencies of permeability with porosity and tortuosity are demonstrated through several fitted equations.     

Analysis of surface and interior degradation of gas diffusion layer with accelerated stress tests for polymer electrolyte membrane fuel cell

The effects of surface and interior degradation of the gas diffusion layer (GDL) on the performance and durability of polymer electrolyte membrane fuel cells (PEMFCs) have been investigated using three freeze-thaw accelerated stress tests (ASTs). Three ASTs (ex-situ, in-situ, and new methods) are designed from freezing ?30 °C to thawing 80 °C by immersing, supplying, and bubbling, respectively. The ex-situ method is designed for surface degradation of the GDL. Change of surface morphology from hydrophobic to hydrophilic by surface degradation of GDL causes low capillary pressure which decreased PEMFC performance. The in-situ method is designed for the interior degradation of the GDL. A decrease in the ratio of the porosity to tortuosity by interior degradation of the GDL deteriorates PEMFC performance. Moreover, the new method showed combined effects for both surface and interior degradation of the GDL. It was identified that the main factor that deteriorated the fuel cell performance was the increase in mass transport resistance by interior degradation of GDL. In conclusion, this study aims to investigate the causes of degraded GDL on the PEMFC performance into the surface and interior degradation and provide the design guideline of high-durability GDL for the PEMFC.