Simulation of species transport and water management in PEM fuel cells

A single phase computational fuel cells model is presented to elucidate three-dimensional interactions between mass transport and electrochemical kinetics in proton exchange membrane (PEM) fuel cells with straight gas channels. The governing differential equations are solved over a single computational domain, which consists of a gas channel, gas diffusion layer, and catalyst layer for both the anode and cathode sides of the cell as well as the solid polymer membrane. Emphasis is placed on obtaining a basic understanding of how three-dimensional flow and transport phenomena in the air cathode impact the electrochemical process in the flow field. The complete cell model has been validated against experimentally measured polarization curve, showing good accuracy in reproducing cell performance over moderate current density interval. Fully three-dimensional results of the flow structure and species profiles are presented for cathode flow field. The effects of pressure on oxygen transport and water removal are illustrated through main axis of the flow structure. The model results indicate that oxygen concentration in reaction sites is significantly affected by pressure increase which leads to rising fuel cells power.     

A two-phase flow and transport model for the cathode of PEM fuel cells

A unified two-phase flow mixture model has been developed to describe the flow and transport in the cathode for PEM fuel cells. The boundary condition at the gas diffuser/catalyst layer interface couples the flow, transport, electrical potential and current density in the anode, cathode catalyst layer and membrane. Fuel cell performance predicted by this model is compared with experimental results and reasonable agreements are achieved. Typical two-phase flow distributions in the cathode gas diffuser and gas channel are presented. The main parameters influencing water transport across the membrane are also discussed. By studying the influences of water and thermal management on two-phase flow, it is found that two-phase flow characteristics in the cathode depend on the current density, operating temperature, and cathode and anode humidification temperatures.     

An analytical study of the PEM fuel cell with axial convection in the gas channel

A quasi two-dimensional mathematical model for a polymer electrolyte membrane (PEM) fuel cell is developed with consideration of axial convection in the gas channel and analytical solutions are obtained. A half-cell model which contains the cathode gas channel, gas diffuser, catalyst layer, and the membrane is investigated. To account for the effect of gas velocity in the gas channel, axial convection is included in the oxygen transport equation of the gas channel. Expressions for the oxygen mass fraction distribution in the gas channel, gas diffuser, and catalyst layer, and the current density and the membrane phase potential in the catalyst layer and membrane are derived. The solutions are presented in the form of infinite series. The polarization curve is also expressed as a function of the surface overpotential. Due to the advantage of the closed-form solutions this model can be easily employed as a diagnostic tool for PEM fuel cell simulations.     

A two-phase flow and transport model for PEM fuel cells

A two-phase flow and multi-component mathematical model with a complete set of governing equations valid in different components of a PEM fuel cell is developed. The model couples the flows, species, electrical potential, and current density distributions in the cathode and anode fluid channels, gas diffusers, catalyst layers and membrane, respectively. The modeling results of typical concentration distributions are presented. The coupling of oxygen concentration, current density, overpotential and potential are shown in the membrane electrode assembly (MEA). The model predicted fuel cell polarization curves for different cathode pressures compared well with our experimental data.     

Electrochemical reaction and performance of proton exchange membrane fuel cells with a novel cathode flow channel shape

This study focuses on the investigation of the electrochemical reaction along a novel cathode flow channel of PEM fuel cells with various shoulder/channel (S/C) ratios at the outlet port. A three-dimensional mathematical model, considering conservation principles of mass, momentum, species and electric current is employed. Local variations of important model variables such as reactant concentration and local current density are presented by contour plots to elucidate the effects of channel geometry on transport process, catalyst reaction and cell performance. The potential fields of solid and membrane phases are also resolved in the cell domain and the driving force of the electrochemical reactions – the catalyst activation overpotential – is harnessed in modeling. Numerical calculations reveal the influence of the cathode channel configuration on the local distributions of various model variables. The results also show the dependence between optimal channel configuration and cell operating condition. At a medium reaction rate, the reaction sites underneath the shoulder region generate more current than the channel region. Therefore, a convergent channel configuration with a larger S/C ratio at the outlet port develops more current because such a design facilitates the electron transport and enhances local activation overpotential. However, as the cell voltage decreases and the reaction rate increases, such configuration loses its merit gradually as the requirement for a higher reactant concentration is more important and the reaction sites underneath the channel region have a higher reaction rate. Consequently, the divergent channel configuration with a lower S/C ratio of 0.67 performs better at a cell voltage of 0.22 V.     

PEMFC电极孔隙率的优化研究

对质子交换膜燃料电池单体建立了三维稳态电化学模型,考察了气体扩散层孔隙率对电池性能的影响,验证了扩散层孔隙率及层厚的变化反映从气体通道到扩散层和催化剂层的反应气体扩散量,进而影响电化学反应的活跃程度;以膜与阴极催化剂层界面处获得的最大电压为目标函数,采用鲍威尔搜索法对气体扩散层孔隙率进行数值优化,得到了扩散层孔隙率和层厚的最优值。通过优化前后氧气浓度和电流密度的对比显示,这些参数可以显著改善电极的传质性能,使燃料电池获得最佳性能。     

A hybrid model of cathode of PEM fuel cell using the interdigitated gas distributor

A two-dimensional (2D), single- and two-phase, hybrid multi-component transport model is developed for the cathode of PEM fuel cell using interdigitated gas distributor. The continuity equation and Darcy's law are used to describe the flow of the reactant gas and production water. The production water is treated as vapor when the current density is small, and as two-phase while the current density is greater than the critical current density. The advection–diffusion equations are utilized to study species transport of multi-component mixture gas. The Butler–Volmer equation is prescribed for the domain in the catalyst layer. The predicted results of the hybrid model agree well with the available experimental data. The model is used to investigate the effects of operating conditions and the cathode structure parameters on the performance of the PEM fuel cell. It is observed that liquid water appears originally in the cathodic catalyst layer over outlet channel under intermediate current and tends to be distributed uniformly by the capillary force with the increase of the current. It is found that reduction of the width of outlet channel can enhance the performance of PEM fuel cell via the increase of the current density over this region, which has, seemingly, not been discussed in previous literatures.     

An inverse geometry design problem for optimization of single serpentine flow field of PEM fuel cell

The cathode flow-field design of a proton exchange membrane fuel cell (PEMFC) determines its reactant transport rates to the catalyst layer and removal rates of liquid water from the cell. This study optimizes the cathode flow field for a single serpentine PEM fuel cell with 5 channels using the heights of channels 2–5 as search parameters. This work describes an optimization approach that integrates the simplified conjugated-gradient scheme and a three-dimensional, two-phase, non-isothermal fuel cell model. The proposed optimal serpentine design, which is composed of three tapered channels (channels 2–4) and a final diverging channel (channel 5), increases cell output power by 11.9% over that of a cell with straight channels. These tapered channels enhance main channel flow and sub-rib convection, both increasing the local oxygen transport rate and, hence, local electrical current density. A diverging, final channel is preferred, conversely, to minimize reactant leakage to the outlet. The proposed combined approach is effective in optimizing the cathode flow-field design for a single serpentine PEMFC. The role of sub-rib convection on cell performance is demonstrated.     

A three-dimensional agglomerate model for the cathode catalyst layer of PEM fuel cells

In this work, a three-dimensional, steady-state, multi-agglomerate model of cathode catalyst layer in polymer electrolyte membrane (PEM) fuel cells has been developed to assess the activation polarization and the current densities in the cathode catalyst layer. A finite element technique is used for the numerical solution to the model developed. The cathode activation overpotentials, and the membrane and solid phase current densities are calculated for different operating conditions. Three different configurations of agglomerate arrangements are considered, an in-line and two staggered arrangements. All the three arrangements are simulated for typical operating conditions inside the PEM fuel cell in order to investigate the oxygen transport process through the cathode catalyst layer, and its impact on the activation polarization. A comprehensive validation with the well-established two-dimensional “axi-symmetric model” has been performed to validate the three-dimensional numerical model results. Present results show a lowest activation overpotential when the agglomerate arrangement is in-line. For more realistic scenarios, staggered arrangements, the activation overpotentials are higher due to the slower oxygen transport and lesser passage or void region available around the individual agglomerate. The present study elucidates that the cathode overpotential reduction is possible through the changing of agglomerate arrangements. Hence, the approaches to cathode overpotential reduction through the optimization of agglomerate arrangement will be helpful for the next generation fuel cell design.     

Computational model of a PEM fuel cell with serpentine gas flow channels

A three-dimensional computational fluid dynamics model of a PEM fuel cell with serpentine flow field channels is presented in this paper. This comprehensive model accounts for the major transport phenomena in a PEM fuel cell: convective and diffusive heat and mass transfer, electrode kinetics, and potential fields. A unique feature of the model is the implementation of a voltage-to-current (VTC) algorithm that solves for the potential fields and allows for the computation of the local activation overpotential. The coupling of the local activation overpotential distribution and reactant concentration makes it possible to predict the local current density distribution more accurately. The simulation results reveal current distribution patterns that are significantly different from those obtained in studies assuming constant surface overpotential. Whereas the predicted distributions at high load show current density maxima under the gas channel area, low load simulations exhibit local current maxima under the collector plate land areas.     

Modeling the Influence of GDL and flow-field plate parameters on the reaction distribution in the PEMFC cathode catalyst layer

In this paper, a two-dimensional cross-the-channel model was applied to investigate the influence of gas diffusion layer (GDL) property and flow-field geometry on the local reaction rate in the PEMFC cathode catalyst layer. The model predictions show that the rate of consumption of oxygen or current density under the land area may differ considerably from that under the channel. Simulation results indicate that for a fixed channel width, increasing the channel-to-land width ratio results in improved water transport and positively impacts the overall reaction rates at high overpotential. However, too high ratio may retard electron transport and thus lead to worse cathode performance. Numerical simulation results revealed that GDL electrical conductivity and thickness have a strong influence on how the chemical species and electrons are transported to the active catalyst sites. Depending on the electrical conductivity of GDL, the region of higher reaction rate may occur either under the land or under the channel. Consideration of orthotropic electrical conductivity of GDL affects the simulation results significantly highlighting the need to improve our understanding of GDL transport coefficients. Simulation of GDL compression effects showed that the total current density is not affected significantly but current density distribution is. The extent of reactant bypass through the GDL from one channel to the other depends on the GDL permeability and results in a significant enhancement in reaction rates.     

Performance prediction of proton exchange membrane fuel cells using a three-dimensional model

In this study a steady-state three-dimensional computational fluid dynamics (CFD) model of a proton exchange membrane fuel cell is developed and presented for a single cell. A complete set of conservation equations of mass, momentum, species, energy transport, and charge is considered with proper account of electrochemical kinetics based on Butler–Volmer equation. The catalyst layer structure is considered to be agglomerate. This model enables us to investigate the flow field, current distribution, and cell voltage over the fuel cell which includes the anode and cathode collector plates, gas channels, catalyst layers, gas diffusion layers, and the membrane. The numerical solution is based on a finite-volume method in a single solution domain. In this investigation a CFD code was used as the core solver for the transport equations, while mathematical models for the main physical and electrochemical phenomena were devised into the solver using user-developed subroutines. Three-dimensional results of the flow structure, species concentrations and current distribution are presented for bipolar plates with square cross section of straight flow channels. A polarization curve is obtained for the fuel cell under consideration. A comparison between the polarization curves obtained from the current study and the corresponding available experimental data is presented and a reasonable agreement is obtained. Such CFD model can be used as a tool in the development and optimization of PEM fuel cells.     

A mathematical model for simulating methanol permeation and the mixed potential effect in a direct methanol fuel cell

A mathematical model for simulating methanol permeation and the pertinent mixed potential effect in a direct methanol fuel cell (DMFC) is presented. In this model a DMFC is divided into seven compartments namely the anodic flow channel, the anodic diffusion layer, the anodic catalyst layer, the proton exchange membrane (PEM), the cathodic catalyst layer, the cathodic diffusion layer and the cathodic flow channel. All compartments are considered to have finite thickness, and within every one of them a set of governing equations are given to stipulate methanol transport and oxygen transport. For the flow channels, fluid dynamics, which could substantially lower the local methanol concentration within catalyst layers is taken into account. With the knowledge of local concentrations of the species, the electrochemical reaction rates within both catalyst layers can be quantified by a kinetic Tafel expression. For the anodic catalyst layer the local external current generated by methanol oxidation is computed; for the cathodic catalyst layer, in addition to the local external current generated by oxygen reduction, the local internal current as a result of methanol permeation is also computed. With the information of the local internal current, the mixed potential effect, which is responsible for adversely lowering the cell voltage can be analyzed.     

叉指型PEMFC阴极内的两相流动模拟

对叉指型质子交换膜燃料电池(PEMFC)阴极提出一个二维两相的多组分流体输运模型,应用连续性方程和Darcy定律以及组分扩散方程描述了反应气体和生成水的流动和传质。利用Leverett函数关联毛细压力与水饱和度,采用半经验关系式给出了气液在多孔层的相对渗透率。本模型预测的叉指型PEMFC性能曲线与文献中实验结果符合较好。研究发现,液态水在阴极内由催化层向出口流动是气体流动的剪切力和毛细驱动力共同作用的结果,液态水流速比气体流速小3个数量级或更多,液态水在电极上的分布比较均匀。     

Along‐channel flooding prediction of polymer electrolyte membrane fuel cells

Non‐uniform current distribution in polymer electrolyte membrane (PEM) fuel cells results in local over‐heating, accelerated ageing, and lower power output than expected. This issue is quite critical when a fuel cell experiences water flooding. In this study, the performance of a PEM fuel cell is investigated under cathode flooding conditions. A two‐dimensional approach is proposed for a single PEM fuel cell based on conservation laws and electrochemical equations to provide useful insight into water transport mechanisms and their effect on the cell performance. The model results show that inlet stoichiometry and humidification, and cell operating pressure are important factors affecting cell performance and two‐phase transport characteristics. Numerical simulations have revealed that the liquid saturation in the cathode gas distribution layer (GDL) could be as high as 20%. The presence of liquid water in the GDL decreases oxygen transport and surface coverage of active catalyst, which in turn degrades the cell performance. The thermodynamic quality in the cathode flow channel is found to be greater than 99.7%, indicating that liquid water in the cathode gas channel exists in very small amounts and does not interfere with the gas phase transport. A detailed analysis of the operating conditions shows that cell performance should be optimized based on the maximum average current density achieved and the magnitude of its dispersion from its mean value. Copyright © 2010 John Wiley & Sons, Ltd.     

Transport phenomena within the porous cathode for a proton exchange membrane fuel cell

A two-phase, one-dimensional steady model is developed to analyze the coupled phenomena of cathode flooding and mass-transport limiting for the porous cathode electrode of a proton exchange membrane fuel cell. In the model, the catalyst layer is treated not as an interface between the membrane and gas diffusion layer, but as a separate computational domain with finite thickness and pseudo-homogenous structure. Furthermore, the liquid water transport across the porous electrode is driven by the capillary force based on Darcy's law. And the gas transport is driven by the concentration gradient based on Fick's law. Additionally, through Tafel kinetics, the transport processes of gas and liquid water are coupled. From the numerical results, it is found that although the catalyst layer is thin, it is very crucial to better understand and more correctly predict the concurrent phenomena inside the electrode, particularly, the flooding phenomena. More importantly, the saturation jump at the interface of the gas diffusion layer and catalyst layers is captured, when the continuity of the capillary pressure is imposed on the interface. Elsewise, the results show further that the flooding phenomenon in the CL is much more serious than that in the GDL, which has a significant influence on the mass transport of the reactants. Moreover, the saturation level inside the cathode is determined, to a great extent, by the surface overpotential, the absolute permeability of the porous electrode, and the boundary value of saturation at the gas diffusion layer-gas channel interface. In order to prevent effectively flooding, it should remove firstly the liquid water accumulating inside the CL and keep the boundary value of liquid saturation as low as possible.     

Effects of flow distributor geometry and diffusion layer porosity on reactant gas transport and performance of proton exchange membrane fuel cells

A study has been conducted on the effects of flow distributor and diffusion layer geometries and morphologies on the transport phenomena of reactant gas from flow channels to gas diffuser, and on the performance of a proton exchange membrane fuel cell. The emphasis of the analysis is placed on the effects of the cross-section of the channel of the anode flow distributor and the porosity of the gas-diffusion layer. By applying a two-dimensional mass transport model, the effects of the channel width fraction, λ=ℓ_c/ℓ_b, the channel number, N, the porosity of the diffuser layer, ε, and the surface overpotential of the catalyst layer, η, on the resultant current density are investigated. The cell performance is evaluated by the predicted voltage–current density curves. It is disclosed that an increase in either λ, N or ε may lead to a better cell performance. At relatively low overpotential, better uniformity in current density distribution along the width of the cell (x-direction) can be attained. Based on the present results, a correlation of overpotentials is proposed, namely, η_cr=0.165λ^0.0935N^0.2033ε^0.0856, which may serve as a guideline to justify the validity of a simplified one-dimensional model.     

Numerical studies of liquid water behaviors in PEM fuel cell cathode considering transport across different porous layers

In this paper, a two-phase two-dimensional PEM fuel cell model, which is capable of handling liquid water transport across different porous materials, is employed for parametric studies of liquid water transport and distribution in the cathode of a PEM fuel cell. Attention is paid particularly to the coupled effects of two-phase flow and heat transfer phenomena. The effects of key operation parameters, including the outside cell boundary temperature, the cathode gas humidification condition, and the cell operation current, on the liquid water behaviors and cell performance have been examined in detail. Numerical results elucidate that increasing the fuel cell temperature would not only enhance liquid water evaporation and thus decrease the liquid saturation inside the PEM fuel cell cathode, but also change the location where liquid water is condensed or evaporated. At a cell boundary temperature of 80 °C, liquid water inside the catalyst layer and gas diffusion media under the current-collecting land would flow laterally towards the gas channel and become evaporated along an interface separating the land and channel. As the cell boundary temperature increases, the maximum current density inside the membrane would shift laterally towards the current-collecting land, a phenomenon dictated by membrane hydration. Increasing the gas humidification condition in the cathode gas channel and/or increasing the operating current of the fuel cell could offset the temperature effect on liquid water transport and distribution.     

Numerical investigation of transport component design effect on a proton exchange membrane fuel cell

A numerical investigation of the transport phenomena and performance of a proton exchange membrane fuel cell (PEMFC) with various design parameters of the transport component is presented. A three-dimensional fuel cell model, incorporating conservations of species, momentum, as well as current transport, is used. The Bulter–Volmer equation that describes the electrochemical reaction in the catalyst layer is introduced; the activation overpotential connects the solid phase potential field to that of the electrolyte phase. Through cell performance simulation with various channel aspect ratios and gas diffusion layer (GDL) thicknesses, a slender channel is found suitable for cells operating at moderate reaction rate, and a flat channel produces more current at low cell voltage. Plots of transverse oxygen concentration and phase potential variation indicate that these oppositely affect the local current density pattern. The relative strengths of these two factors depend on the transport component position and geometry, as well as on the cell operating conditions. Consequently, the curves of cell output current density demonstrate that the optimal GDL thickness increases as the cell voltage decreases. However, at the lowest considered cell voltage of 0.14 V, optimal thickness decreases as that of a thick GDL. The oxygen deficiency caused by long traveling length and clogging effect of liquid water reverses this relationship.     

Simultaneous measurement of current and temperature distributions in a proton exchange membrane fuel cell

Using a specially designed current distribution measurement gasket in anode and thin thermocouples between the catalyst layer and gas diffusion layer (GDL) in cathode, in-plane current and temperature distributions in a proton exchange membrane fuel cell (PEMFC) have been simultaneously measured. Such simultaneous measurements are realized in a commercially available experimental PEMFC. Experiments have been conducted under different air flow rates, different hydrogen flow rates and different operating voltages, and measurement results show that there is a very good correlation between local temperature rise and local current density. Such correlations can be explained and agree well with basic thermodynamic analysis. Measurement results also show that significant difference exists between the temperatures at cathode catalyst layer/GDL interface and that in the center of cathode endplate, which is often taken as the cell operating temperature. Compared with separate measurement of local current density or temperature, simultaneous measurements of both can reveal additional information on reaction irreversibility and various transport phenomena in fuel cells.