Ned Djilali

Three-dimensional computational analysis of transport phenomena in a PEM fuel cell

Abstract A comprehensive non-isothermal, three-dimensional computational model of a polymer electrolyte membrane (PEM) fuel cell has been developed. The model incorporates a complete cell with both the membrane-electrode-assembly (MEA) and the gas distribution flow channels. With the exception of phase change, the model accounts for all major transport phenomena. The model is implemented into a computational fluid dynamics code, and simulations are presented with an emphasis on the physical insight and fundamental understanding afforded by the detailed three-dimensional distributions of reactant concentrations, current densities, temperature and water fluxes. The results show that significant temperature gradients exist within the cell, with temperature differences of several degrees K within the MEA. The three-dimensional nature of the transport is particularly pronounced under the collector plates land area and has a major impact on the current distribution and predicted limiting current density.

An assessment of alkaline fuel cell technology

This paper provides a review of the state of the art of alkaline fuel cell (AFC) technology based on publications during the past twenty-4ve years. Although popular in the 1970s and 1980s, the AFC has fallen out of favour with the technical community in the light of the rapid development of Proton Exchange Membrane Fuel Cells (PEMFCs). AFCs have been shown to provide high power densities and achieve long lifetimes in certain applications, and appear to compete favourably with ambient air PEM fuel cells. In this report we examine the overall technology of AFCs, and review published claims about power density and lifetime performance. Issues surrounding the sensitivity of the AFC to CO2 in the oxidant stream are reviewed and potential solutions discussed. A rough cost comparison between ambient air AFCs and PEMFCs is presented. Overall, it appears the Alkaline Fuel Cell continues to have potential to succeed in certain market niche applications, but tends to lack the R& D support required to re4ne the technology into successful market o

A 3D, multiphase, multicomponent model of the cathode and anode of a PEM fuel cell

A computational fluid dynamics multiphase model of a proton-exchange membrane ~PEM! fuel cell is presented. The model accounts for three-dimensional transport processes including phase change and heat transfer, and includes the gas-diffusion layers ~GDL! and gas flow channels for both anode and cathode, as well as a cooling channel. Transport of liquid water inside the gas-diffusion layers is modeled using viscous forces and capillary pressure terms. The physics of phase change is accounted for by prescribing local evaporation as a function of the undersaturation and liquid water concentration. Simulations have been performed for fully humidified gases entering the cell. The results show that different competing mechanisms lead to phase change at both anode and cathode sides of the fuel cell. The predicted amount of liquid water depends strongly on the prescribed material properties, particularly the hydraulic permeability of the GDL. Analysis of the simulations at a current density of 1.2 A/cm 2 show that both condensation and evaporation take place within the cathode GDL, whereas condensation prevails throughout the anode, except near the inlet. The three-dimensional distribution of the reactants and products is evident, particularly under the land areas. For the conditions investigated in this paper, the liquid water saturation does not exceed 10% at either anode or cathode side, and increases nonlinearly with current density. The operation of proton-exchange membrane ~PEM! fuel cells depends not only on the effective distribution of air and hydrogen, but also on the maintenance of an adequate cell operating temperature and fully humidified conditions in the membrane. The fully humidified state of the membrane is crucial to ensuring good ionic conductivity and is achieved by judicious water management. Water content is determined by the balance between various water transport mechanisms and water production. The water transport mechanisms are electro-osmotic drag of water ~i.e., motion of water molecules attaching to protons migrating through the membrane from anode to cathode!; back diffusion from the cathode ~due to nonuniform concentration!; and diffusion and convection to/from the air and hydrogen gas streams. Water production depends on the electric current density and phase change. Without control, an imbalance between production and removal rates of water can occur. This can result in either dehydration of the membrane, or flooding of the electrodes, which are both detrimental to performance. A common water management technique relies on the humidification of the air and hydrogen gas streams. At higher current densities, the excess product water is removed by convection via the air stream, and the rate of removal is controlled by adjusting moisture content in concert with pressure drop and temperature in the flow channels. Thermal management is also required to remove the heat produced by the electrochemical reaction in order to prevent drying out of the membrane, which in turn can result not only in reduced performance but also in eventual rupture of the membrane. Thermal management, which is performed via forced convection cooling in larger stacks, is also essential for the control of the water evaporation or condensation rates. The operation of a fuel cell and the resulting water and heat distributions depend on numerous transport phenomena including charge-transport and multicomponent, multiphase flow, and heat transfer in porous media. The complexity and interaction of these processes and the difficulty in making detailed in situ measurements have prompted the development of a number of numerical models. The theoretical framework was laid out in early one-dimensional numerical models of the membrane-electrode. 1-3 A quasi-twodimensional model based on concentrated solution theory was also proposed by Newman and Fuller, 4 and a full two-dimensional model including flow channels but no electrodes was also presented by Nguyen and White. 5 This model was refined in a number of subsequent studies to account for the porous electrodes and interdigitated

Three-dimensional computational analysis of transport phenomena in a PEM fuel cell—a parametric study

This paper presents the results of a parametric study conducted with a previously described three-dimensional, non-isothermal model of a polymer electrolyte membrane (PEM) fuel cell. The effect of various operational parameters such as the temperature and pressure on the fuel cell performance was investigated in detail. It was found that in order to obtain physically realistic results experimental measurements of various modelling parameters were needed. The results show good qualitative agreement with experimental results published in the literature. In addition, geometrical and material parameters such as the gas diffusion electrode (GDE) thickness and porosity as well as the ratio between the channel width and the land area were investigated. The contact resistance inside the cell was found to play an important role for the evaluation of the impact of such parameters on the fuel cell performance. The results demonstrate the usefulness of this computational model as a design and optimization tool.

A microfluidic fuel cell with flow-through porous electrodes.

A microfluidic fuel cell architecture incorporating flow-through porous electrodes is demonstrated. The design is based on cross-flow of aqueous vanadium redox species through the electrodes into an orthogonally arranged co-laminar exit channel, where the waste solutions provide ionic charge transfer in a membraneless configuration. This flow-through architecture enables improved utilization of the three-dimensional active area inside the porous electrodes and provides enhanced rates of convective/diffusive transport without increasing the parasitic loss required to drive the flow. Prototype fuel cells are fabricated by rapid prototyping with total material cost estimated at 2 USD/unit. Improved performance as compared to previous microfluidic fuel cells is demonstrated, including power densities at room temperature up to 131 mW cm-2. In addition, high overall energy conversion efficiency is obtained through a combination of relatively high levels of fuel utilization and cell voltage. When operated at 1 microL min-1 flow rate, the fuel cell produced 20 mW cm-2 at 0.8 V combined with an active fuel utilization of 94%. Finally, we demonstrate in situ fuel and oxidant regeneration by running the flow-through architecture fuel cell in reverse.

A two-dimensional analysis of mass transport in proton exchange membrane fuel cells

A theoretical model is developed to simulate transport phenomena in a proton exchange membrane fuel cell (PEMFC). The primary focus of this paper is the modelling and assessment of two-dimensional effects neglected in previous studies. The work is motivated by the need to understand the transport processes in fuel cells in order to improve heat and water management, and to alleviate mass transport limitations. The model takes into account diffusion of the humidified fuel (H2, CO2 and H2O(v)) and oxidant gases (O2, N2 and H2O(v)) through the porous electrodes, and convective and electro-osmotic transport of liquid water in the electrodes and the membrane. The thermodynamic equilibrium potential is calculated using the Nernst equation, and reaction kinetics are determined using the Butler–Volmer equation. A finite volume procedure is developed to solve the system of differential equations. The model is validated against available experimental data, and numerical simulations are presented for various one- and two-dimensional isothermal cases. The results indicate that the cathode potential loss, associated with the slow O2 reaction rate, is dominant at all practical current densities. The simulations also show that two-dimensionality has a significant effect on water management and on some aspects of fuel cell performance. In particular, the anode and cathode water fluxes are found to vary considerably along the oxidant and fuel flow channels, and two new transitional water transport regimes are revealed by the two-dimensional simulations. The influences of flow configuration and electrode porosity on predicted cell performance are also discussed.

Hydrogen Peroxide as an Oxidant for Microfluidic Fuel Cells

We demonstrate a microfluidic fuel cell incorporating hydrogen peroxide oxidant. Hydrogen peroxide (H 2 O 2 ) is available at high concentrations, is highly soluble and exhibits a high standard reduction potential. It also enables fuel cell operation where natural convection of air is limited or anaerobic conditions prevail, as in submersible and space applications. As fuel cell performance critically depends on both electrode and channel architecture, several different prototype cells are developed and results are compared. High-surface area electrodeposited platinum and palladium electrodes are evaluated both ex situ and in situ for the combination of direct H 2 O 2 reduction and oxygen reduction via the decomposition reaction. Oxygen gas bubbles produced at the fuel cell cathode introduce an unsteady two-phase flow component that, if not controlled, can perturb the co-laminar flow interface and reduce fuel cell performance. A grooved channel design is developed here that restricts gas bubble growth and transport to the vicinity of the cathodic active sites, enhancing the rate of oxygen reduction, and limiting crossover effects. The proof-of-concept microfluidic fuel cell produced power densities up to 30 mW cm -2 and a maximum current density of 150 mA cm -2 , when operated on 2 M H 2 O 2 oxidant together with formic acid-based fuel at room temperature.

Transport Phenomena in Polymer Electrolyte Membranes

This paper presents a critical examination and analysis of classical and recently proposed models for transport phenomena in polymer electrolyte membranes. Key experimental observations related to membrane conductivity, membrane hydration, and sorption isotherms are first reviewed. Proton transport mechanisms in bulk water, and the influence of the membrane phase on these mechanisms, are examined. Finally, various formulations and underlying assumptions to account for macroscopic transport are reviewed, and an analysis of the binary friction model (BFM) and dusty fluid model (DFM) is performed to resolve an outstanding formulation issue. It is shown that the BFM provides a physically consistent modeling framework and implicitly accounts for viscous transport (i.e., Schloegl equation), whereas the dusty fluid model erroneously accounts twice for viscous transport. In Part II we apply the BFM framework to develop a general transport model for perfluorosulfonic acid membranes.

Pore Scale Simulation of Transport and Electrochemical Reactions in Reconstructed PEMFC Catalyst Layers

A mesoscale simulation is developed to simulate transport and electrochemistry in a small section of a proton exchange membrane fuel cell (PEMFC) cathode catalyst layer. Oxygen, proton, and electron transport are considered in the model. Many simulations are run with a wide variety of different parameters on stochastically reconstructed microstructures with a resolution of 2 nm. Knudsen diffusion plays an important role in limiting the transport of oxygen through the catalyst layer. Using larger carbon spheres in the catalyst layer increases the effective diffusivity of oxygen through the catalyst layer. The effective proton conductivity increases when larger spheres are used, a normal distribution of spheres is used, or a higher overlap tolerance is used. Increasing the overlap tolerance or overlap probability results in an increase in the effective electron conductivity. When electrochemical reactions are considered in a part of the catalyst layer that is close to the gas diffusion layer, the critical parameter that determines oxygen consumption is the carbon sphere radius. Oxygen consumption at a given carbon volume fraction is larger in microstructures containing spheres with smaller radii, because there is more surface area available for electrochemical reactions.

Lab-on-chip methodologies for the study of transport in porous media: energy applications

We present a lab-on-chip approach to the study of multiphase transport in porous media. The applicability of microfluidics to biological and chemical analysis has motivated much development in lab-on-chip methodologies. Several of these methodologies are also well suited to the study of transport in porous media. We demonstrate the application of rapid prototyping of microfluidic networks with approximately 5000 channels, controllable wettability, and fluorescence-based analysis to the study of multiphase transport phenomena in porous media. The method is applied to measure the influence of wettability relative to network regularity, and to differentiate initial percolation patterns from active flow paths. Transport phenomena in porous media are of critical importance to many fields and particularly in many energy-related applications including liquid water transport in fuel cells, oil recovery, and CO(2) sequestration.