Kriston P. Brooks

Systems Modeling of Chemical Hydride Hydrogen Storage Materials for Fuel Cell Applications

A fixed bed reactor was designed, modeled and simulated for hydrogen storage on-board the vehicle for PEM fuel cell applications. Ammonia Borane (AB) was selected by DOEs Hydrogen Storage Engineering Center of Excellence (HSECoE) as the initial chemical hydride of study because of its high hydrogen storage capacity (up to {approx}16% by weight for the release of {approx}2.5 molar equivalents of hydrogen gas) and its stability under typical ambient conditions. The design evaluated consisted of a tank with 8 thermally isolated sections in which H2 flows freely between sections to provide ballast. Heating elements are used to initiate reactions in each section when pressure drops below a specified level in the tank. Reactor models in Excel and COMSOL were developed to demonstrate the proof-of-concept, which was then used to develop systems models in Matlab/Simulink. Experiments and drive cycle simulations showed that the storage system meets thirteen 2010 DOE targets in entirety and the remaining four at greater than 60% of the target.

Compact Reverse Water-Gas-Shift Reactor for Extraterrestrial In Situ Resource Utilization

A compact reverse water-gas-shift reactor suitable for extraterrestrial use as part of the in situ propellant production system is reported. The reactor is less than 15 cm 3 in volume and weighs less than 50 g. With an Ru/ZrO 2 -CeO catalyst it produces over 150 g H 2 O/h operating at 800°C. This is near equilibrium conversion at about half-scale of a Mars sample-return mission. Even at these high processing rates, the pressure drop remains low (from 1.6 to 7.6 kPa).

Bench-Scale Enhanced Sludge Washing and Gravity Settling of Hanford Tank S-107 Sludge

This report summarizes the results of a bench-scale sludge pretreatment demonstration of the Hanford baseline flowsheet using liter-quantities of sludge from Hanford Site single-shell tank 241-C-106 (tank C-106). The leached and washed sludge from these tests provided Envelope D material for the contractors supporting Tank Waste Remediation System (TWRS) Privatization. Pretreatment of the sludge included enhanced sludge washing and gravity settling tests and providing scale-up data for both these unit operations. Initial and final solids as well as decanted supernatants from each step of the process were analyzed chemically and radiochemically. The results of this work were compared to those of Lumetta et al. (1996a) who performed a similar experiment with 15 grams of C-106, sludge. A summary of the results are shown in Table S.1. Of the major nonradioactive components, those that were significantly removed with enhanced sludge washing included aluminum (31%), chromium (49%), sodium (57%), and phosphorus (35%). Of the radioactive components, a significant amount of {sup 137}Cs (49%) were removed during the enhanced sludge wash. Only a very small fraction of the remaining radionuclides were removed, including {sup 90}Sr (0.4%) and TRU elements (1.5%). These results are consistent with those of the screening test. All of the supernatants (both individually and as a blend) removed from these washing steps, once vitrified as LLW glasses (at 20 wt% Na{sub 2}O), would be less than NRC Class C in TRU elements and less than NRC Class B in {sup 90}Sr.

Dynamic Modeling and Simulation Based Analysis of an Ammonia Borane (AB) Reactor System for Hydrogen Storage

Research on ammonia borane (AB, NH3BH3) has shown it to be a promising material for chemical hydrogen storage in PEM fuel cell applications. AB was selected by DOE’s Hydrogen Storage Engineering Center of Excellence (HSECoE) as the initial chemical hydride of study because of its high hydrogen storage capacity (up to 19.6% by weight for the release of three molar equivalents of hydrogen gas) and its stability under typical ambient conditions. A model of a bead reactor system which includes feed and product tanks, hot and cold augers, a ballast tank/reactor, a H2 burner and a radiator was developed to study AB system performance in an automotive application and estimate the energy, mass, and volume requirements for this off-board regenerable hydrogen storage material. Preliminary system simulation results for a start-up case and for a transient drive cycle indicate appropriate trends in the reactor system dynamics. A new controller was developed and validated in simulation for a couple of H2 demand cases.

Design and Development of a Low-Cost, High Temperature Silicon Carbide Micro-Channel Recuperator

Typically, ceramic micro-channel devices are used for high temperature heat exchangers, catalytic reactors, electronics cooling, and processing of corrosive streams where the thermomechanical benefits of ceramic materials are desired. These benefits include: high temperature mechanical and corrosion properties and tailorable material properties such as thermal expansion, electrical conductivity and thermal conductivity. In addition, by utilizing Laminated Object Manufacturing (LOM) methods, inexpensive ceramic materials can be layered, featured and laminated in the green state and co-sintered to form monolithic structures amenable to mass production. In cooperation with the DOE and Pacific Northwest National Labs, silicon carbide (SiC) based micro-channel recuperator concepts are being developed and tested. The performance benefits of a high temperature, micro-channel heat exchanger are realized from the improved thermal efficiency of the high temperature cycles and the improved effectiveness of micro-channels for heat transfer. In designing these structures, the heat and mass transfer within the micro-channels are being analyzed with heat transfer models, computational fluid dynamics models and validated with experimental results. As an example, a typical micro-turbine cycle was modified and modeled to incorporate this ceramic recuperator and it was found that the overall thermal efficiency of the micro-turbine could be improved from about 27% to over 40%. Process improvements require technical advantages and cost advantages. These LOM methodologies have been based on well-proven industry standard processes where labor, throughput and capital estimates have been tested. Following these cost models and validation at the prototype scale, cost estimates were obtained. For the micro-turbine example, cost estimates indicate that the high-temperature SiC recuperator would cost about

Chemical Hydrides for Hydrogen Storage in Fuel Cell Applications

200 per kWe. The development of these heat exchangers is multi-faceted and this paper focuses on the design optimization of a layered micro-channel heat exchanger, its performance testing, and fabrication development through LOM methodologies.Copyright

GRAVITY SETTLING OF HANFORD SINGLE-SHELL TANK SLUDGES

Due to its high hydrogen storage capacity (up to 19.6% by weight for the release of 2.5 molar equivalents of hydrogen gas) and its stability under typical ambient conditions, ammonia borane (AB) is a promising material for chemical hydrogen storage for fuel cell applications in transportation sector. Several systems models for chemical hydride materials such as solid AB, liquid AB and alane were developed and evaluated at PNNL to determine an optimal configuration that would meet the 2010 and future DOE targets for hydrogen storage. This paper presents an overview of those systems models and discusses the simulation results for various transient drive cycle scenarios.

Radiator Performance Enhancement using a LiBr-H 2 O Absorption Cooler and Microchannel Technology: A Portable Life Support System Example

ABSTRACT The U.S. Department of Energy plans to use gravity settling in million-gallon storage tanks while pretreating sludge on the Hanford site. To be considered viable in these large tanks, the supernatant must become clear, and the sludge must be concentrated in an acceptable time. These separations must occur over the wide range of conditions associated with sludge pretreatment. In the work reported here, gravity settling was studied with liter quantities of actual single-shell tank sludge from Hanford Tank 241-C-107. Because of limited sludge availability, an approach was developed using the results of these liter-scale tests to predict full-scale operation. Samples were centrifuged at various g-forces to simulate compaction with higher layers of sludge. A semi-empirical settling model was then developed incorporating both the liter-scale settling data and the centrifuge compression results to describe the sludge behavior in a million-gallon tank. The settling model predicted that the compacted slud...

Heat and Mass Transfer Design of a Silicon Carbide Micro-Channel Heat Exchanger

Portable life support systems must be capable of performing thermal management in a wide variety of environments. Heat-actuated heat pumps may provide this flexibility, if they can be made small enough. Microchannel technologies represent a proven approach for reducing system volume and mass. The potential impact of adding a LiBr-H2O absorption cooler to increase the radiator temperature was considered. This study showed that such a heat pump can lift the radiator temperature from 15°C to 60°C with a coefficient of performance of 0.65 and that the radiator area can be reduced by up to 60%.

Methanation of carbon dioxide by hydrogen reduction using the Sabatier process in microchannel reactors

Efficiency and emissions of advanced gas turbine power cycles can be improved by incorporating high-temperature ceramic heat exchangers. In cooperation with the DOE, a highly effective microchannel ceramic recuperator for a microturbine is under development. In this recuperator, the use of microchannel architecture will improve heat transfer and provide a more uniform temperature distribution. This will result in overall higher productivity per unit volume compared to conventional hardware. The use of ceramic for the recuperator will allow higher temperature operation than available in conventional microturbines. Based on a model for a typical microturbine, these changes may improve the overall system efficiency from about 27% to over 40%.Copyright