Nathan P. Siegel

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.

Single domain PEMFC model based on agglomerate catalyst geometry

Abstract A steady two-dimensional computational model for a proton exchange membrane (PEM) fuel cell is presented. The model accounts for species transport, electrochemical kinetics, energy transport, current distribution, and water uptake and release in the catalyst layer. 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. The model for the catalyst regions is based on an agglomerate geometry, which requires water species to exist in both dissolved and gaseous forms simultaneously. Data related to catalyst morphology, which was required by the model, was obtained via a microscopic analysis of a commercially available membrane electrode assembly (MEA). The coupled set of differential equations is solved with the commercial computational fluid dynamics (CFD) solver, CFDesign™, and is readily adaptable with respect to geometry and material property definitions. The results show that fuel cell performance is highly dependent on catalyst structure, specifically the relative volume fractions of gas pores and polymer membrane contained within the active region as well as the geometry of the individual agglomerates.

Solar Thermochemical Water-Splitting Ferrite-Cycle Heat Engines

Thermochemical cycles are a type of heat engine that utilize high-temperature heat to produce chemical work. Like their mechanical work producing counterparts, their efficiency depends on the operating temperature and on the irreversibility of their internal processes. With this in mind, we have invented innovative design concepts for two-step solar-driven thermochemical heat engines based on iron oxide and iron oxide mixed with other metal oxide (ferrites) working materials. The design concepts utilize two sets of moving beds of ferrite reactant materials in close proximity and moving in opposite directions to overcome a major impediment to achieving high efficiency-thermal recuperation between solids in efficient countercurrent arrangements. They also provide an inherent separation of the product hydrogen and oxygen and are an excellent match with a high-concentration solar flux. However, they also impose unique requirements on the ferrite reactants and materials of construction as well as an understanding of the chemical and cycle thermodynamics. In this paper, the counter-rotating-ring receiver/reactor/ recuperator solar thermochemical heat engine concept is introduced, and its basic operating principles are described. Preliminary thermal efficiency estimates are presented and discussed. Our results and development approach are also outlined.

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.

A New Reactor Concept for Efficient Solar-Thermochemical Fuel Production

We describe and analyze the efficiency of a new solar-thermochemical reactor concept, which employs a moving packed bed of reactive particles produce of H2 or CO from solar energy and H2O or CO2. The packed bed reactor incorporates several features essential to achieving high efficiency: spatial separation of pressures, temperature, and reaction products in the reactor; solid–solid sensible heat recovery between reaction steps; continuous on-sun operation; and direct solar illumination of the working material. Our efficiency analysis includes material thermodynamics and a detailed accounting of energy losses, and demonstrates that vacuum pumping, made possible by the innovative pressure separation approach in our reactor, has a decisive efficiency advantage over inert gas sweeping. We show that in a fully developed system, using CeO2 as a reactive material, the conversion efficiency of solar energy into H2 and CO at the design point can exceed 30%. The reactor operational flexibility makes it suitable for a wide range of operating conditions, allowing for high efficiency on an annual average basis. The mixture of H2 and CO, known as synthesis gas, is not only usable as a fuel but is also a universal starting point for the production of synthetic fuels compatible with the existing energy infrastructure. This would make it possible to replace petroleum derivatives used in transportation in the U.S., by using less than 0.7% of the U.S. land area, a roughly two orders of magnitude improvement over mature biofuel approaches. In addition, the packed bed reactor design is flexible and can be adapted to new, better performing reactive materials.

MOLTEN NITRATE SALT DEVELOPMENT FOR THERMAL ENERGY STORAGE IN PARABOLIC TROUGH SOLAR POWER SYSTEMS

Thermal energy storage can enhance the utility of parabolic trough solar power plants by providing the ability to match electrical output to peak demand periods. An important component of thermal energy storage system optimization is selecting the working fluid used as the storage media and/or heat transfer fluid. Large quantities of the working fluid are required for power plants at the scale of 100-MW, so maximizing heat transfer fluid performance while minimizing material cost is important. This paper reports recent developments of multi-component molten salt formulations consisting of common alkali nitrate and alkaline earth nitrate salts that have advantageous properties for applications as heat transfer fluids in parabolic trough systems. A primary disadvantage of molten salt heat transfer fluids is relatively high freeze-onset temperature compared to organic heat transfer oil. Experimental results are reported for formulations of inorganic molten salt mixtures that display freeze-onset temperatures below 100°C. In addition to phase-change behavior, several properties of these molten salts that significantly affect their suitability as thermal energy storage fluids were evaluated, including chemical stability and viscosity. These alternative molten salts have demonstrated chemical stability in the presence of air up to approximately 500°C in laboratory testing and display chemical equilibrium behavior similar to Solar Salt. The capability to operate at temperatures up to 500°C may allow an increase in maximum temperature operating capability vs. organic fluids in existing trough systems and will enable increased power cycle efficiency. Experimental measurements of viscosity were performed from near the freeze-onset temperature to about 200°C. Viscosities can exceed 100 cP at the lowest temperature but are less than 10 cP in the primary temperature range at which the mixtures would be used in a thermal energy storage system. Quantitative cost figures of constituent salts and blends are not currently available, although, these molten salt mixtures are expected to be inexpensive compared to synthetic organic heat transfer fluids. Experiments are in progress to confirm that the corrosion behavior of readily available alloys is satisfactory for long-term use.

Development and Evaluation of a Prototype Solid Particle Receiver: On-Sun Testing and Model Validation

A prototype direct absorption central receiver, called the solid particle receiver (SPR), was built and evaluated on-sun at power levels up to 2.5 MW th at Sandia National Laboratories in Albuquerque, NM. The SPR consists of a 6 m tall cavity through which spherical sintered bauxite particles are dropped and directly heated with concentrated solar energy. In principle, the particles can be efficiently heated to a temperature in excess of 900°C, well beyond the stability limit of existing nitrate salt formulations. The heated particles may then be stored in a way analogous to nitrate salt systems, enabling a dispatchable thermal input to power or fuel production cycles. The focus of this current effort was to provide an experimental basis for the validation of computational models that have been created to support improved designs and further development of the solid particle receiver. In this paper we present information on the design and construction of the solid particle receiver and discuss the development of a computational fluid dynamics model of the prototype. We also present experimental data and model comparisons for on-sun testing of the receiver over a range of input power levels from 1.58―2.51 MW th . Model validation is performed using a number of metrics including particle velocity, exit temperature, and receiver efficiency. In most cases, the difference between the model predictions and data is less than 10%.

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.

Computational Fluid Dynamics Modeling of Gas-Particle Flow Within a Solid-Particle Solar Receiver

A detailed three-dimensional computational fluid dynamics (CFD) analysis on gas-particle flow and heat transfer inside a solid-particle solar receiver, which utilizes free-falling particles for direct absorption of concentrated solar radiation, is presented. The two-way coupled Euler-Lagrange method is implemented and includes the exchange of heat and momentum between the gas phase and solid particles. A two-band discrete ordinate method is included to investigate radiation heat transfer within the particle cloud and between the cloud and the internal surfaces of the receiver. The direct illumination energy source that results from incident solar radiation was predicted by a solar load model using a solar ray-tracing algorithm. Two kinds of solid-particle receivers, each having a different exit condition for the solid particles, are modeled to evaluate the thermal performance of the receiver Parametric studies, where the particle size and mass flow rate are varied, are made to determine the optimal operating conditions. The results also include detailed information for the gas velocity, temperature, particle solid volume fraction, particle outlet temperature, and cavity efficiency.

Testing of a CR5 Solar Thermochemical Heat Engine Prototype

Sandia National Laboratories (SNL) is investigating thermochemical approaches for reenergizing CO2 and H2 O feed stocks for input to synthetic liquid hydrocarbon fuels production. Key to the approach is the Counter-Rotating-Ring Receiver/Reactor/Recuperator (CR5), a novel solar-driven thermochemical heat engine concept for high-temperature carbon dioxide and water splitting based on two-step, nonvolatile metal oxide thermochemical cycles. The CR5 integrates two reactors, recuperators, and solar receiver and intrinsically separates the product gases. The CR5 thermochemical heat engine concept and the underlying thermodynamics and kinetics have many uncertainties. While results from laboratory scale material tests are promising, they are different than what occurs in a CR5. To evaluate the potential of the CR5 we have designed and built a CR5 prototype. The overall objective of the SNL Sunshine to Petrol (S2P) project is to show a solar thermochemical pathway for the efficient production of liquid fuels from CO2 and H2 O feed stocks. To achieve the overall long-term goal of 10% efficient conversion of sunlight to petroleum, the thermochemical solar conversion of sunlight to CO needs to be 20% efficient. The short-term goal for the CR5 prototype is to demonstrate a solar to chemical conversion efficiency of at least 2%. In this paper, we present initial test results for the CR5 prototype in the 16 kWt National Solar Thermal Test Facility (NSTTF) solar furnace in Albuquerque, NM. Lessons learned from the initial tests and approaches for improving performance to achieve our goals are also presented.Copyright