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.     

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.     

Effect of weave tightness and structure on the in-plane and through-plane air permeability of woven carbon fibers for gas diffusion layers

In this study, woven gas diffusion layers (GDLs) with varying weave type and tightness are investigated. Plain and twill weave patterns were manufactured in-house. The in-plane and through-plane air permeability of the woven samples were tested, and mercury intrusion porosimetry (MIP) tests were performed to study the pore structure. It was found that the twill weave has a higher permeability than the plain weave, which is consistent with literature. Like non-woven carbon papers, woven GDLs have higher in-plane permeability than through-plane permeability; however it has been shown that it is possible to manufacture a GDL with higher through-plane permeability than in-plane permeability. It was also concluded that the percentage of macropores in the weave is the driving factor in determining the through-plane air permeability. This work lays the groundwork for future studies to attempt to characterize the relationship between the weave structure and the air permeability in woven GDLs.     

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.     

Analytic determination of the effective thermal conductivity of PEM fuel cell gas diffusion layers

Accurate information on the temperature field and associated heat transfer rates are particularly important in devising appropriate heat and water management strategies in proton exchange membrane (PEM) fuel cells. An important parameter in fuel cell performance analysis is the effective thermal conductivity of the gas diffusion layer (GDL). Estimation of the effective thermal conductivity is complicated because of the random nature of the GDL micro structure. In the present study, a compact analytical model for evaluating the effective thermal conductivity of fibrous GDLs is developed. The model accounts for conduction in both the solid fibrous matrix and in the gas phase; the spreading resistance associated with the contact area between overlapping fibers; gas rarefaction effects in microgaps; and salient geometric and mechanical features including fiber orientation and compressive forces due to cell/stack clamping. The model predictions are in good agreement with existing experimental data over a wide range of porosities. Parametric studies are performed using the proposed model to investigate the effect of bipolar plate pressure, aspect ratio, fiber diameter, fiber angle, and operating temperature.     

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.     

Modeling of composite fibrous porous diffusion media

To engineer the desired properties of fibrous porous media, a parametric modeling approach is needed to support the rational design of the materials before the fabrication. In this study, we propose a methodology that enables the accurate representation of three-dimensional (3D) microstructures of fibrous porous media and prediction of their transport properties. Toray TGP-H-060 gas diffusion layer (GDL) is selected as an example to demonstrate the feasibility of the suggested design methodology. The detailed microstructure of the GDL with the inclusion of locally distributed binder is constructed using an extended periodic surface (PS) modeling technique. A 3D morphological approach is taken to create the binder distribution within the fibrous microstructure. Transport properties including permeability, relative diffusivity, and tortuosity and local structure characteristics of the generated microstructure, under different binder loading are calculated. It is shown that the detailed model of the fiber-binder composite has a strong influence on the predicted properties.     

Evaluating breakthrough pressure in gas diffusion layers of proton exchange membrane fuel cells

This paper studied the breakthrough pressure for liquid water to penetrate the gas diffusion layer （GDL） of a pro- ton exchange membrane fuel cell （PEMFC）. An ex-situ testing was conducted on a transparent test cell to visu- alize the water droplet formation and detachment on the surface of different types of GDLs through a CCD cam- era. The breakthrough pressure, at which the liquid water penetrates the GDL and starts to form a droplet, was measured. The breakthrough pressure was found to be different for the GDLs with different porosities and thick- nesses. The equilibrium pressure, which is defined as the minimum pressure required maintaining a constant flow through the GDL, was also recorded. The equilibrium pressure was found to be much lower than the breakthrough pressure for the same type of GDL. A pore network model was modified to further study the relationship between the breakthrough pressure and the GDL properties and thicknesses. The breakthrough pressure increases for the thick GDL with smaller micro-pore size.     

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.     

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.     

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.     

Comparing through-plane diffusibility correlations in PEFC gas diffusion layers using the lattice Boltzmann method

One of the key elements in a polymer electrolyte fuel cell (PEFC) is the gas diffusion layer (GDL). The GDL offers mechanical support to the cell and provides the medium for diffusing the reactant gases from the flow plates to the electrolyte enabling the electrochemical reactions, and therefore the energy conversion. At the same time, it has the task of transporting the electrons from the active sites, near to the electrolyte, towards the flow plates.Describing the fluid flow and mass transport phenomena through the GDLs is not an easy task not only because of their complex geometries, but also because of these phenomena occur at microscale levels. Most of the PEFC models at cell scale make assumptions about certain microscale transport parameters, assumptions that can make a model less close to the reality. The purpose of this study is to analyze five different proposed correlations to estimate the through-plane (TP) diffusibility of digitally created GDLs and using lattice Boltzmann (LB) models. The correlations are ranked depending on their precision, accuracy and symmetry. The results show that the best estimation is given when the porosity and gas-phase tortuosity are taken into account in the correlation.     

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.     

Experimental investigation of current distributions in a direct methanol fuel cell with various gas diffusion layers and Nafion membranes

The influences of the gas diffusion layer (GDL) properties on the current distributions of a direct methanol fuel cell are investigated. Cathode GDLs with different hydrophobicity/hydrophilicity, air permeability, microporous layer (MPL), thickness, and texture properties are examined. Among the GDLs examined, a thin hydrophobic GDL with an MPL has the most homogeneous current distribution, which is primarily ascribed to the better water management capabilities of the cathode GDL properties. The differences in the current distribution among the different GDLs are more apparent when the air flow rate and loaded current are lower. The effect of the membrane thickness on the current distributions is also investigated. Among the membranes examined, Nafion^® 112 has different current distributions from the others, whereas there is no noticeable difference between the current distributions with Nafion^® 115 and Nafion^® 117. The current distribution with Nafion^® 112 is most affected by the enhanced methanol crossover and the high mixed potential.     

Carbon black / PTFE composite hydrophobic gas diffusion layers for a water-absorbing porous electrolyte electrolysis cell

The characteristics of a water-absorbing porous electrolyte electrolysis cell, in which pressurized water is injected directly into the electrolyte layer, are investigated. High water support force is required for the gas diffusion layer (GDL) in this novel cell design, and therefore here we report a new type of hydrophobic GDL comprising an acetylene black (AB) and poly(tetrafluoroethylene) (PTFE) composite film. The method of preparation of the AB/PTFE slurry, film formation methods, and the AB/PTFE weight ratio were investigated and optimized. The ball-milling and transfer method were suitable for preparing uniform AB/PTFE slurry and successfully covering AB/PTFE film without any cracks on micro-porous layer coated carbon paper, respectively. An investigation about different PTFE weight ratios against AB from 0.1 to 6 showed a serious trade-off character between electrical resistance R, gas permeability V′, and water support force P_lim. The 1/2.5 of AB/PTFE weight ratio was most optimal, which showed to have most equivalent R (2.5 Ω cm^?2), V′(136 mL atm^?1 cm^?2 min^?1), and P_lim (0.25 MPa). We also confirmed that fabricated GDL with optimal condition was worked as the blocking layer against water injected through electrolyte layer and pressurized by nitrogen gas, and as gas-permeation layer for generated hydrogen gas in water electrolysis test.     

Effects of porosity gradient in gas diffusion layers on performance of proton exchange membrane fuel cells

A three-dimensional, two-phase, non-isothermal model has been developed to explore the interaction between heat and water transport in proton exchange membrane fuel cells (PEMFCs). Water condensate produced from the electrochemical reaction may accumulate in the open pores of the gas diffusion layer (GDL) and retard the oxygen transport to the catalyst sites. This study predicts the enhancement of the water transport for linear porosity gradient in the cathode GDL of a PEMFC. An optimal porosity distribution was found based on a parametric study. Results show that a optimal linear porosity gradient with ?₁ = 0.7 and ?₂ = 0.3 for the parallel and z-serpentine channel design leads to a maximum increase in the limiting current density from 10,696 Am⁻² to 13,136 Am⁻² and 14,053 Am⁻² to 16,616 Am⁻² at 0.49 V, respectively. On the other hand, the oxygen usage also increases from 36% to 46% for the parallel channel design and from 55% to 67% for the z-serpentine channel design. The formation of a porosity gradient in the GDL enhances the capillary diffusivity, increases the electrical conductivity, and hence, benefits the oxygen transport throughout the GDL. The present study provides a theoretical support for existing reports that a GDL with a gradient porosity improves cell performance.     

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.     

Scale effect and two-phase flow in a thin hydrophobic porous layer. Application to water transport in gas diffusion layers of proton exchange membrane fuel cells

Pore network simulations are performed to study water transport in gas diffusion layers (GDLs) of polymer electrolyte membrane fuel cells (PEMFCs). The transport and equilibrium properties are shown to be scale dependent in a thin system like a GDL. A distinguishing feature of such a thin system is the lack of length scale separation between the system size and the size of the representative elementary volume (REV) over which are supposed to be defined the macroscopic properties within the framework of the continuum approach to porous media. Owing to the lack of length scale separation, two-phase flow traditional continuum models are expected to offer poor predictions of water distribution in a GDL. This is illustrated through comparisons with results from the pore network model. The influence of inlet boundary conditions on invasion patterns is studied and shown to affect greatly the saturation profiles. The effects of GDL differential compression and partial coverage of outlet surface are also investigated.     

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.     

Development of simulated gas diffusion layer of polymer electrolyte fuel cells and evaluation of its structure

In polymer electrolyte fuel cell (PEFC), it is important to understand the behavior of liquid water in gas diffusion layer (GDL) which is one of the constructional elements so as to improve the output performance and the durability. As this behavior of liquid water is attributed to not only the hydrophilicity but also inhomogeneous structure, it is needed to examine in consideration of an actual GDL structure. In this study, as the basic examination of two-phase flow analysis in an actual GDL, a simulated GDL was made by numerical analysis considering the fiber placement. Furthermore, the prediction methods for pore size distribution, permeability and tortuosity of this simulated GDL were developed with the numerical analysis. These parameters of flow and mass transfer were compared with other studies, and the validity of this simulated GDL was confirmed. In addition, effective diffusion coefficient was calculated from tortuosity in simulated GDL, and PEFC output performance was evaluated by a simple model. Moreover, the optimal GDL was examined in consideration of the effect of porosity and fiber diameter at the fiber level.