In situ investigation of water transport in an operating PEM fuel cell using neutron radiography: Part 1 – Experimental method and serpentine flow field results

Effective management of liquid water produced in the cathodic reaction of a polymer electrolyte membrane (PEM) fuel cell is essential to achieve high cell efficiency. Few experimental methods are available for in situ measurements of water transport within an operating cell. Neutron radiography is a useful tool to visualize water within a cell constructed of many common materials, including metals. The application of neutron radiography to measurements of water content within the flow field channels of an operating 50 cm² PEM fuel cell is described. Details of the experimental apparatus, image processing procedure and quantitative analysis are provided. It is demonstrated that water tends to accumulate in the 180° bends of the serpentine anode and cathode flow fields used in this study. Moreover, the effects of both the current density and cathode stoichiometric ratio on the quantity of accumulated water are discussed.     

Water management studies in PEM fuel cells,Part II: Ex situ investigation of flow maldistribution,pressure drop and two-phase flow pattern in gas channels

Two-phase flow of water and reactant gases in the gas distribution channels of proton exchange membrane fuel cells (PEMFCs) plays a critical role in proper water management. In this work, the two-phase flow in PEMFC cathode parallel channels is studied over a wide range of superficial air velocity (air stoichiometry) and superficial water velocity in a specially designed ex situ experimental setup, which enables the measurement of instantaneous flow rates in individual gas channels and simultaneous visualization of the water flow structure. It is found that the two-phase flow at low superficial air velocities (air stoichiometry below 5) is dominated by slugs or semi-slugs, leading to severe flow maldistribution and large fluctuations in the pressure drop. Slug residence time, measured from the video observation and the instantaneous flow rate data, is found to be a new parameter to describe the slug flow. At higher air velocities, a water film is formed on the channel walls if they are hydrophilic. The pressure drop for the film flow is characterized by smaller but frequent fluctuations, which are found to result from the water buildup at the channel-exit manifold interface. As the superficial air velocity increases further, mist flow is obtained where little water buildup is observed. The water buildup in the gas channels at the two-phase flow is well described by the two-phase friction multiplier, defined as the ratio of the two-phase pressure drop to the single gas phase pressure drop. It is found that the two-phase friction multiplier increases with increasing water flow rate. A flow pattern map is developed using superficial water and air velocities with clearly defined transition regions.     

Numerical study of water management in the air flow channel of a PEM fuel cell cathode

The water management in the air flow channel of a proton exchange membrane (PEM) fuel cell cathode is numerically investigated using the FLUENT software package. By enabling the volume of fraction (VOF) model, the air–water two-phase flow can be simulated under different operating conditions. The effects of channel surface hydrophilicity, channel geometry, and air inlet velocity on water behavior, water content inside the channel, and two-phase pressure drop are discussed in detail. The results of the quasi-steady-state simulations show that: (1) the hydrophilicity of reactant flow channel surface is critical for water management in order to facilitate water transport along channel surfaces or edges; (2) hydrophilic surfaces also increase pressure drop due to liquid water spreading; (3) a sharp corner channel design could benefit water management because it facilitates water accumulation and provides paths for water transport along channel surface opposite to gas diffusion layer; (4) the two-phase pressure drop inside the air flow channel increases almost linearly with increasing air inlet velocity.     

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.     

Laser perforated fuel cell diffusion media. Part I: Related changes in performance and water content

In this study, cathode-side, bi-layered diffusion media (DM) samples with micro-porous layer were perforated with 300 μm laser-cut holes (covering 15% of the surface area in a homogenous pattern) using a ytterbium fiber laser to investigate the effect of structural changes on the gas and water transport. Under reduced humidity conditions (50% inlet relative humidity on the anode and cathode), the perforated DM were observed to increase the potential by an average of 6% for current densities ranging from 0.2 to 1.4 A cm⁻². However, the perforated DM showed reduced performance for current densities greater than 1.4 A cm⁻² and at all currents under high-humidity conditions. Neutron radiography experiments were also performed to understand the changes in liquid water retention characteristics of DM due to the laser perforations. Significant water accumulation and water redistribution were observed in the perforated DM, which helps explain the observed performance behavior. The results indicate that the perforations act as water pooling and possible channeling locations, which significantly alter the water condensation, storage, and transport scheme within the fuel cell. These observations suggest that proper tailoring of fuel cell DM possesses significant potential to enable fuel cell operations with reduce liquid overhead and high performance.     

In situ investigation of water transport in an operating PEM fuel cell using neutron radiography: Part 2 – Transient water accumulation in an interdigitated cathode flow field

An interdigitated cathode flow field has been tested in situ with neutron radiography to measure the water transport through the porous gas diffusion layer in a PEM fuel cell. Constant current density to open circuit cycles were tested and the resulting liquid water accumulation and dissipation rates with in-plane water distributions are correlated to measured pressure differential between inlet and outlet gas streams. The effect of varying the reactant gas relative humidity on liquid water accumulation is also demonstrated. These results provide evidence that the reactant gas establishes a consistent in-plane transport path through the diffusion layer, leaving stagnant regions where liquid water accumulates. A simplified permeability model is presented and used to correlate the relative permeability to varying gas diffusion layer liquid water saturation levels.     

Water balance for the design of a PEM fuel cell system

The design of a proton exchange membrane (PEM) fuel cell system is important for the optimization of the function of supporting parameters in the fuel cell. The water balance in a PEM fuel cell is investigated based on the water transport phenomena. In this investigation, the diffusion of water from the cathode side to the anode side of the cell is observed to not occur at 20% relative humidity at the cathode (RHC) and 58% relative humidity at the anode (RHA). The minimum concentration of condensed water at the cathode side is observed at a cathode gas inlet relative humidity of 40% RHC–92% RHC and at temperatures between 343 K and 363 K. RHC operating conditions that are greater than 90% and at a temperature of 363 K increased the concentration of condensed water and occurred quickly, which result in a water balance that became difficult to control. On the anode side, the condensation of water is observed at operating temperatures of 353 K and 363 K.     

Liquid water distribution patterns featuring back-diffusion transport in a PEM fuel cell with neutron imaging

Back-diffusion in PEM fuel cells is the water transport mechanism contributing to balance the water content profile in the membrane (in the through-plane direction), transporting water molecules from the cathode electrode towards the anode side of the membrane. In this technical note, neutron radiographs are presented for a 50 cm² N-117 fuel cell with serpentine flow field, where the effect of the back diffusion transport mechanism is clearly identified, in the form of crossed patterns following the cross-flow layout of the flow field. The back diffusion water transport is evident despite the high thickness of the N-117 membrane.     

Numerical investigation of the impact of two-phase flow maldistribution on PEM fuel cell performance

Flow maldistribution usually happens in PEM fuel cells when using common inlet and exit headers to supply reactant gases to multiple channels. As a result, some channels are flooded with more water and have less air flow while other channels are filled with less water but have excessive air flow. To investigate the impact of two-phase flow maldistribution on PEM fuel cell performance, a Volume of Fluid (VOF) model coupled with a 1D MEA model was employed to simulate two parallel channels. The slug flow pattern is mainly observed in the flow channels under different flow maldistribution conditions, and it significantly increases the gas diffusion layer (GDL) surface water coverage over the whole range of simulated current densities, which directly leads to poor fuel cell performance. Therefore, it is recommended that liquid and gas flow maldistribution in parallel channels should be avoided if possible over the whole range of operation. Increasing the gas stoichiometric flow ratio is not an effective method to mitigate the gas flow maldistribution, but adding a gas inlet resistance to the flow channel is effective in mitigating maldistribution. With a carefully selected value of the flow resistance coefficient, both the fuel cell performance and the gas flow distribution can be significantly improved without causing too much extra pressure drop.     

A flow channel design procedure for PEM fuel cells with effective water removal

Proper water management in polymer electrolyte membrane (PEM) fuel cells is critical to achieve the potential of PEM fuel cells. Membrane electrolyte requires full hydration in order to function as proton conductor, often achieved by fully humidifying the anode and cathode reactant gas streams. On the other hand, water is also produced in the cell due to electrochemical reaction. The combined effect is that liquid water forms in the cell structure and water flooding deteriorates the cell performance significantly. In the present study, a design procedure has been developed for flow channels on bipolar plates that can effectively remove water from the PEM fuel cells. The main design philosophy is based on the determination of an appropriate pressure drop along the flow channel so that all the liquid water in the cell is evaporated and removed from, or carried out of, the cell by the gas stream in the flow channel. At the same time, the gas stream in the flow channel is maintained fully saturated in order to prevent membrane electrolyte dehydration. Sample flow channels have been designed, manufactured and tested for five different cell sizes of 50, 100, 200, 300 and 441 cm². Similar cell performance has been measured for these five significantly different cell sizes, indicating that scaling of the PEM fuel cells is possible if liquid water flooding or membrane dehydration can be avoided during the cell operation. It is observed that no liquid water flows out of the cell at the anode and cathode channel exits for the present designed cells during the performance tests, and virtually no liquid water content in the cell structure has been measured by the neutron imaging technique. These measurements indicate that the present design procedure can provide flow channels that can effectively remove water in the PEM fuel cell structure.     

Water management studies in PEM fuel cells,part III: Dynamic breakthrough and intermittent drainage characteristics from GDLs with and without MPLs

The transport of liquid water and gaseous reactants through a gas diffusion layer (GDL) is one of the most important water management issues in a proton exchange membrane fuel cell (PEMFC). In this work, the liquid water breakthrough dynamics, characterized by the capillary pressure and water saturation, across GDLs with and without a microporous layer (MPL) are studied in an ex-situ setup which closely simulates a real fuel cell configuration and operating conditions. The results reveal that recurrent breakthroughs are observed for all of the GDL samples tested, indicating the presence of an intermittent water drainage mechanism in the GDL. This is accounted for by the breakdown and redevelopment of the continuous water paths during water drainage as demonstrated by Haines jumps. For GDL samples without MPL, a dynamic change of breakthrough locations is observed, which originates from the rearrangement of the water configuration in the GDL following the drainage. For GDL samples with MPL, no dynamic change of breakthrough location can be found and the water saturation is significantly lower than the samples without MPL. These results suggest that the MPL not only limits the number of water entry locations into the GDL (such that the water saturation is drastically reduced), but also stabilizes the water paths (or morphology). The effect of MPL on the two-phase flow dynamics in gas channels is also studied with multi-channel flow experiments. The most important result is that GDL without MPL promotes film flow and shifts the slug-to-film flow transition to lower air flow rates, compared with the case of GDL with MPL. This is closely related to the larger number of water breakthrough locations through GDL without MPL, which promotes the formation of water film.     

A two-phase non-isothermal mixed-domain PEM fuel cell model and its application to two-dimensional simulations

In this paper, a two-phase non-isothermal PEM fuel cell model based on the previously developed mixed-domain PEM fuel cell model with a consistent treatment of water transport in MEA has been established using the traditional two-fluid method. This two-phase multi-dimensional PEM fuel cell model could fully incorporate both the anode and cathode sides, properly account for the various water phases, including water vapor, water in the membrane phase, and liquid water, and truly enable numerical investigations of water and thermal management issues with the existence of condensation/evaporation interfaces in a PEM fuel cell. This two-phase model has been applied in this paper in a two-dimensional configuration to determine the appropriate condensation and evaporation rate coefficients and conduct extensive numerical studies concerning the effects of the inlet humidity condition and temperature variation on liquid water distribution with or without a condensation/evaporation interface.     

Two-phase flow pressure drop hysteresis in an operating proton exchange membrane fuel cell

Two-phase flow pressure drop hysteresis was studied in an operating PEM fuel cell. The variables studied include air stoichiometry (1.5, 2, 3, 4), temperature (50, 75, 90 °C), and the inclusion of a microporous layer. The cathode channel pressure drops can differ in PEM fuel cells when the current density is increased along a path and then decreased along the same path (pressure drop hysteresis). Generally, the descending pressure drop is greater than the ascending pressure drop at low current densities (<200 mA cm⁻²), and the effect is worse at low stoichiometries and low temperatures. The results show that the hysteresis occurs with or without the inclusion of a microporous layer. Initial results show a modified Lockhart-Martinelli approach seems to be able to predict the two-phase flow pressure drop during the ascending path. The results compare well with photographs taken from the cathode flow field channel of a visualization cell.     

Combined neutron radiography and locally resolved current density measurements of operating PEM fuel cells

Neutron radiographic imaging is combined with locally resolved current density measurements to study the effects of local water content on the performance of the corresponding electrochemical active area in an operating PEM fuel cell. Liquid water agglomerates are detected, quantified and correlated with the activity of the respective area. At low currents, depletion of the reactant gas leads to a decreasing performance along the anodic flowfield channel. At high currents, an optimum humidification is reached in the central part of the fuel cell; close to the inlets respectively outlets, flooding and drying can be observed concurrently and cause a non-uniform current density distribution across the reactive area. The fast response of the local performance on water droplets migrating in the gas channel is tracked by short-term imaging taking place on a timescale of several seconds.     

Two-phase flow pressure drop hysteresis in parallel channels of a proton exchange membrane fuel cell

Two-phase flow pressure drop hysteresis was studied in a non-operational PEM fuel cell to understand the effect of stoichiometry, GDL characteristics, operating range, and initial conditions (dry vs. flooded) for flow conditions typical of an operating fuel cell. This hysteresis is noted when the air and water flow rates are increased and then decreased along the same path, exhibiting different pressure drops. When starting from dry conditions, the descending pressure drop tended to be higher than the ascending pressure drop at lower simulated current densities. The hysteresis effect was noted for stoichiometries of 1-4 and was eliminated at a stoichiometry of 5. It was found that the hysteresis was greater when water breakthrough occurred at higher simulated current densities, which is a function of GDL properties. The operating range had to reach a critical simulated current density (800 mA cm⁻² in this case) between the ascending and descending approach to create a pressure drop hysteresis zone. The descending step size does not change the size of the hysteresis effect, but a larger step size leads to lower fluctuations in the pressure drop signal. An initially flooded condition also showed hysteresis, but the ascending approach tended to have a higher pressure drop than the descending approach.     

Diagnostic tools in PEM fuel cell research: Part I Electrochemical techniques

To meet the power density, reliability, and cost requirements that will enable a widespread use of fuel cells, many research activities focus on an understanding of the thermodynamics as well as the fluid mechanical and electrochemical processes within a fuel cell. To date, a wide range of experimental diagnostics is imperative not only to help a fundamental understanding of fuel cell dynamics but also to provide benchmark-quality data for modeling research. This two-part paper reviews various tools for diagnosing polymer electrolyte membrane (PEM) fuel cells and stacks, and attempts to incorporate the most recent technical advances in PEM fuel cell diagnosis. In Part I, we review various electrochemical techniques and outline the principle, experimental implementation, and data processing of each technique. Capabilities and weaknesses of these techniques are also discussed. In Part II of the review we will cover physical/chemical methods.     

A generalized numerical model for liquid water in a proton exchange membrane fuel cell with interdigitated design

A new approach to numerical simulation of liquid water distribution in channels and porous media including gas diffusion layers (GDLs), catalyst layers, and the membrane of a proton exchange membrane fuel cell (PEMFC) was introduced in this study. The three-dimensional, PEMFC model with detailed thermo-electrochemistry, multi-species, and two-phase interactions. Explicit gas-liquid interface tracking was performed by using Computational Fluid Dynamics (CFD) software package FLUENT^® v6.2, with its User-Defined Functions (UDF) combined with volume-of-fluid (VOF) algorithm. The liquid water transport on a PEMFC with interdigitated design was investigated. The behavior of liquid water was understood by presenting the motion of liquid water droplet in the channels and the porous media at different time instants. The numerical results show that removal of liquid water strongly depends on the magnitude of the flow field. Due to the blockage of liquid water, the gas flow is unevenly distributed, the high pressure regions takes place at the locations where water liquid appears. In addition, mass transport of the species and the current density distribution is significantly degraded by the presence of liquid water.     

Numerical investigation of the impact of gas and cooling flow configurations on current and water distributions in a polymer membrane fuel cell through a pseudo-two-dimensional diphasic model

For optimal performances, proton exchange membrane fuel cells require fine water and thermal management. Accurate modelling of the physical phenomena occurring in the fuel cell is a key issue to improve fuel cell technology. Here, an analytic steady state diphasic 2D model of heat and mass transfer is presented. Through this model, the aim of this work is to study the influence of local events on the global performances of a fuel cell. A part of the complete model is a microscopic representation of the coupling between water transport and charge transfers in the electrodes. The thickness of the liquid layer around the reactive agglomerates is deduced from the saturation. The evolution of the quantity of water within the catalyst layer is monitored and its influence on the global performances of the cell is investigated. In gas diffusion layers (GDLs), liquid and vapour water transport through are computed regarding the temperature. The flow direction of cooling water modifies the current density distribution along the cell. The impact of the direction of air and hydrogen feeding channels are investigated. It can modify greatly the fuel cell mean current density and the net water transport coefficient. The counter-flow mode was preferable. Likewise, thanks to a better membrane hydration, it results in independent performances regarding the hydrogen inlet relative humidity or stoichiometry.     

Gravity effect on water discharged in PEM fuel cell cathode

Experimental purpose is to test gravity influence on water discharged in PEM fuel cell cathode. Through changing the way of placement of the cathode and anode, it takes adjusting the electronic load to test the output of voltage and current. Corresponding to the position of the cathode-upward and the anode-upward, different humidification condition, draws the polarization curve using the voltage and current density. According to the placing position of the cathode and anode, cell temperature, humidification temperature of the cathode and anode gas, 4 groups of experimental results are obtained. The experimental conclusion is: when a PEM fuel cell is placed anode-upward, gravity is advantageous to discharge the liquid water in PEM fuel cell cathode. On the contrary, gravity is disadvantageous to discharge the liquid water.     

Study on water transport in PEM of a direct methanol fuel cell

Water transport phenomenon in PEM and the mechanism of occurrence and development of a two-phase countercurrent flow with corresponding transport phenomenon in the PEM are analyzed. A one-dimensional steady state model of heat and mass transfer in porous media system with internal volumetric ohmic heating is developed and simulated numerically. The results show that two dimensionless parameters D and N, which reflect the liquid water flow rate and inner heat source in the PEM, respectively, are the most important factors for the water fraction and thermal balance in the PEM. The saturation profiles within the two-phase region at various operating modes are obtained. Smaller mass flow rate of liquid water and high current density are the major contributions to the membrane dehydration.