Daniel S. Hussey

In Situ High-Resolution Neutron Radiography of Cross-Sectional Liquid Water Profiles in Proton Exchange Membrane Fuel Cells

High-resolution neutron radiography was used to image an operating proton exchange membrane fuel cell in situ. The cross-sectional liquid water profile of the cell was quantified as a function of cell temperature, current density, and anode and cathode gas feed flow rates. Detailed information was obtained on the cross-sectional water content in the membrane electrode assembly and the gas flow channels. At low current densities, liquid water tended to remain on the cathode side of the cell. Significant liquid water in the anode gas flow channel was observed when the heat and water production of the cell were moderate, where both water diffusion from the cathode and thermal gradients play a significant role in determining the water balance of the cell. Within the membrane electrode assembly itself, the cathode side was moderately more hydrated than the anode side of the assembly from 0.1 to 1.25 A cm -2 . The total liquid water content of the membrane electrode assembly was fairly stable between current densities of 0.25 and 1.25 A cm -2 , even though the water in the gas flow channels changed drastically over this current density range. At 60°C, the water content in the center of the gas diffusion layer was depleted compared to the membrane or gas flow channel interfaces. This phenomenon was not observed at 80°C where evaporative water removal is prevalent.

Real-Time Imaging of Liquid Water in an Operating Proton Exchange Membrane Fuel Cell

Neutron imaging experiments were carried out to measure the water content of an operating proton exchange membrane fuel cell (PEMFC) under varying conditions of current density and temperature. It was found that the water content of the PEMFC is strongly coupled to the current density and temperature of the cell. These measurements indicate that changes in water content lag changes in current density by at least 100 s, both when the current density was increased and decreased. Less liquid water was measured in the cells when operating at 80°C than at 40°C. At 60°C cell temperature, a peak in water content was observed around 650 mA/cm 2 and the water content was found to decrease with increasing current density. This is explained in the context of cell heating by performing a simple thermal analysis of an operating PEMFC so as to yield quantitative information on the waste heat and its effects on the liquid water contained in the cell.

Measurement of Liquid Water Accumulation in a PEMFC with Dead-Ended Anode

2active area, Nafion 111-IP membrane, and carbon cloth gas diffusion layer. Even though dry hydrogen is supplied to the anode via pressure regulation, accumulation of liquid water in the anode gas distribution channels was observed in most tested conditions. Moreover, the accumulation of liquid water in the anode channels is followed by a significant voltage drop. Anode purges and cathode surges are also used as a diagnostic tool for differentiating between anode and cathode water flooding. The rate of accumulation of liquid water, and its impact on the rate of cell voltage drop is shown for a range of temperature, current density, cathode inlet RH, and air stoichiometric conditions. Operating the fuel cell under dead-ended anode conditions offers the opportunity to observe water dynamics and measured cell voltage during large and repeatable transients.

Understanding Liquid Water Distribution and Removal Phenomena in an Operating PEMFC via Neutron Radiography

A proton exchange membrane fuel cell (PEMFC) was imaged using neutron radiography under pseudo steady-state operating conditions to determine the total liquid water content of the cell and the liquid water content distribution across the active cell area as a function of cell temperature, current density, and cathode air flow rate. A simple cathode-based model was formulated to rationalize the observed dry inlet regions which were most strongly influenced by temperature and current density. Between temperatures of 40 and 80°C and current densities of 0.5 and 1.5 A cm -2 , the outlet gas temperature was measured to be 1-5°C greater than the cell bulk temperature. This small temperature difference was enough to account for drying of 20-40% of the cell area, depending on the bulk cell temperature. For the cell construction used in this work, the temperature and cathode stoichiometric flow had a marginal effect on the polarization curve performance but had a large effect on the liquid water content and distribution within the cell.

Neutron Imaging of Lithium Concentration in LFP Pouch Cell Battery

This paper shows how neutron radiography can be used for in situ quantification of the lithium concentration across battery electrodes, a critical physical system state. The change in lithium concentration between the charged and discharged states of the battery causes a change in number of detected neutrons after passing through the battery. Electrode swelling is also observed during battery charging. The experimental setup and the observations from testing a pouch cell with LFP cathode and graphite anode are reported here. The bulk Li concentration across the electrode and folds of the pouch cell is quantified at various states of charge. To interpret the measurements, the optics of the neutron beam (geometric unsharpness) and detector resolution are considered in order to quantify the lithium concentration from the images due to the thinness of the electrode layers. The experimental methodology provides a basis for comprehensive in situ metrology of bulk lithium concentration.

Quantification of Temperature Driven Flow in a Polymer Electrolyte Fuel Cell Using High-Resolution Neutron Radiography

In this study, the effect of a controlled temperature gradient on water transport across a single fuel cell was quantitatively investigated using high-resolution neutron imaging. The direction of liquid water transport under isothermal and non-isothermal conditions was observed in both hydrophilic and hydrophobic diffusion media (DM). The change in distribution of liquid saturation with time revealed two different mechanisms of water transport; capillary driven flow and phase-change induced (PCI) flow, in which a water vapor concentration gradient is created by condensation at a colder location. This concentration gradient drives diffusion flow toward the colder location. A maximum liquid saturation plateau of ca. 30% was shown for all conditions tested, indicating a critical transition between pendular and funicular modes of liquid water storage was captured. Based on this, it is suggested that PCI-flow may be the main mode of liquid transport below this critical transition threshold, above which, capillary flow dominates. As expected, both average cell temperature and the magnitude of temperature gradient were shown to significantly affect the rate of condensation within the DM. Experimental results were compared with water saturation distribution model predictions from literature and show reasonable qualitative agreement. Finally, it was concluded that current available models significantly over predict vapor phase diffusive transport in saturated fuel cell media using a Bruggeman type model.

Imaging of Water Profiles in PEM Fuel Cells Using Neutron Radiography: Effect of Operating Conditions and GDL Composition

The performance of polymer electrolyte membrane (PEM) fuel cells as a function of cathode inlet relative humidity (RH) and gas diffusion layer (GDL) properties has been characterized. The performance of 50 cm2 fuel cells at high current densities was a strong function of the polytetrafluoroethylene (PTFE) content in the cathode GDL microporous layer (MPL). The voltage at a current density of 1.4 A cm-2 decreased at all inlet RHs as the PTFE content in the cathode MPL increased from 5 % by weight to 23 % by weight. This was associated with a corresponding increase in the mass transport resistance as measured by AC impedance. The low frequency resistance also increased with increasing cathode inlet RH. These results were validated by high-resolution neutron radiography on specially designed 2.25 cm2 cells that showed increased water content in the GDLs at high inlet RHs and high microporous layer PTFE content. High-resolution neutron imaging also revealed higher water concentrations at the outlets, cathode GDL, anode flow channel, and MEA/GDL above the land when compared to the inlets, anode GDL, cathode flow channel, and MEA/GDL above the channel respectively.

Consideration of the Role of Micro-Porous Layer on Liquid Water Distribution in Polymer Electrolyte Fuel Cells

Evidence of a region of gradual property change between the micro-porous layer and the macroporous layer of bilayer diffusion media is presented, and a mathematical model describing the effects of this gradual interfacial region is developed. The model results in a continuous liquid water saturation distribution across the diffusion media compared to the sharp discontinuity in the liquid phase saturation predicted by the earlier sudden interface models. High-resolution neutron radiography is used to measure the water content profile across the diffusion media, and the results are compared with the model predictions. The effect of the geometric blur, and uncertainty in-neutron radiography, is accounted for by applying the effects of geometric blur to model results. When the blur is considered, the neutron radiography results are found to be very similar to model predictions.

Measurement of Water Content in Polymer Electrolyte Membranes Using High Resolution Neutron Imaging

Sufficient water content within a polymer electrolyte membrane (PEM) is necessary for adequate ionic conductivity. Membrane hydration is therefore a fundamental requirement for fuel cell operation. The hydration state of the membrane affects the water transport within, as both the diffusion coefficient and electro-osmotic drag depend on the water content. Membranes water uptake is conventionally measured ex situ by weighing free-swelling samples equilibrated at controlled water activity. In the present study, water profiles in Nafion{reg_sign} membranes were measured using the high-resolution neutron imaging. The state-of-the-art, 10 {micro}m resolution neutron detector is capable of resolving water distributions across N1120, N1110 and N117 membranes. It provides a means to measure the water uptake and transport properties of fuel cell membranes in situ.

Observations of Transient Flooding in a Proton Exchange Membrane Fuel Cell Using Time-Resolved Neutron Radiography

The generation and transport of water in both liquid and gas phases during device operation are important areas to understand both steady state and transient performance of proton exchange membrane fuel cells. Localized concentrations of liquid water within the cell can cause flooding, which leads to decreases in cell performance, fuel starvation, degradation, or, in extreme cases, collapse of cell output. A variety of experimental and simulation techniques have been used to elucidate flooding events; yet, a comprehensive understanding of what leads to flooding and the specific details of how flooding affects fuel cell performance, especially during transient operation, have not been completely developed. The work reported here couples direct observations of liquid water flooding, primarily in the gas flow channel, with measurements of cell performance, outlet temperature, and outlet dew point during a step change in current density. Liquid water buildup and water slug dynamics were monitored with the temperature and electrical performance of the cell in real time. The size of the water slugs was connected to the cell performance to illustrate how the liquid water influences cell operation and how the conditions of the cathode gas flow control the liquid water content of the cell.