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O'Brien, J E

Publications and source records attributed to O'Brien, J E.

RECENT ADVANCES IN HIGH TEMPERATURE ELECTROLYSIS AT IDAHO NATIONAL LABORATORY: SINGLE CELL TESTS

An experimental investigation on the performance and durability of single solid oxide electrolysis cells (SOECs) is under way at the Idaho National Laboratory. In order to understand and mitigate the degradation issues in high temperature electrolysis, single SOECs with different configurations from several manufacturers have been evaluated for initial performance and long-term durability. A new test apparatus has been developed for single cell and small stack tests from different vendors. Single cells from Ceramatec Inc. show improved durability compared to our previous stack tests. Single cells from Materials and Systems Research Inc. (MSRI) demonstrate low degradation both in fuel cell and electrolysis modes. Single cells from Saint Gobain Advanced Materials (St. Gobain) show stable performance in fuel cell mode, but rapid degradation in the electrolysis mode. Electrolyte-electrode delamination is found to have significant impact on degradation in some cases. Enhanced bonding between electrolyte and electrode and modification of the microstructure help to mitigate degradation. Polarization scans and AC impedance measurements are performed during the tests to characterize the cell performance and degradation.

08 HYDROGEN↗

RECENT ADVANCES IN HIGH TEMPERATURE ELECTROLYSIS AT IDAHO NATIONAL LABORATORY: STACK TESTS

High temperature steam electrolysis is a promising technology for efficient sustainable large-scale hydrogen production. Solid oxide electrolysis cells (SOECs) are able to utilize high temperature heat and electric power from advanced high-temperature nuclear reactors or renewable sources to generate carbon-free hydrogen at large scale. However, long term durability of SOECs needs to be improved significantly before commercialization of this technology. A degradation rate of 1%/khr or lower is proposed as a threshold value for commercialization of this technology. Solid oxide electrolysis stack tests have been conducted at Idaho National Laboratory to demonstrate recent improvements in long-term durability of SOECs. Electrolytesupported and electrode-supported SOEC stacks were provided by Ceramatec Inc., Materials and Systems Research Inc. (MSRI), and Saint Gobain Advanced Materials (St. Gobain), respectively for these tests. Long-term durability tests were generally operated for a duration of 1000 hours or more. Stack tests based on technology developed at Ceramatec and MSRI have shown significant improvement in durability in the electrolysis mode. Long-term degradation rates of 3.2%/khr and 4.6%/khr were observed for MSRI and Ceramatec stacks, respectively. One recent Ceramatec stack even showed negative degradation (performance improvement) over 1900 hours of operation. A three-cell short stack provided by St. Gobain, however, showed rapid degradation in the electrolysis mode. Improvements on electrode materials, interconnect coatings, and electrolyteelectrode interface microstructures contribute to better durability of SOEC stacks.

08 HYDROGEN↗

Pressurized Testing of Solid Oxide Electrolysis Stacks with Advanced Electrode-Supported Cells

A new facility has been developed at the Idaho National Laboratory for pressurized testing of solid oxide electrolysis stacks. Pressurized operation is envisioned for large-scale hydrogen production plants, yielding higher overall efficiencies when the hydrogen product is to be delivered at elevated pressure for tank storage or pipelines. Pressurized operation also supports higher mass flow rates of the process gases with smaller components. The test stand can accommodate cell dimensions up to 8.5 cm x 8.5 cm and stacks of up to 25 cells. The pressure boundary for these tests is a water-cooled spool-piece pressure vessel designed for operation up to 5 MPa. The stack is internally manifolded and operates in cross-flow with an inverted-U flow pattern. Feed-throughs for gas inlets/outlets, power, and instrumentation are all located in the bottom flange. The entire spool piece, with the exception of the bottom flange, can be lifted to allow access to the internal furnace and test fixture. Lifting is accomplished with a motorized threaded drive mechanism attached to a rigid structural frame. Stack mechanical compression is accomplished using springs that are located inside of the pressure boundary, but outside of the hot zone. Initial stack heatup and performance characterization occurs at ambient pressure followed by lowering and sealing of the pressure vessel and subsequent pressurization. Pressure equalization between the anode and cathode sides of the cells and the stack surroundings is ensured by combining all of the process gases downstream of the stack. Steady pressure is maintained by means of a backpressure regulator and a digital pressure controller. A full description of the pressurized test apparatus is provided in this paper.

08 HYDROGEN↗

4 kW Test of Solid Oxide Electrolysis Stacks with Advanced Electrode-Supported Cells

A new test stand has been developed at the Idaho National Laboratory for multi-kW testing of solid oxide electrolysis stacks. This test stand will initially be operated at the 4 KW scale. The 4 kW tests will include two 60-cell stacks operating in parallel in a single hot zone. The stacks are internally manifolded with an inverted-U flow pattern and an active area of 100 cm2 per cell. Process gases to and from the two stacks are distributed from common inlet/outlet tubing using a custom base manifold unit that also serves as the bottom current collector plate. The solid oxide cells incorporate a negative-electrode-supported multi-layer design with nickel-zirconia cermet negative electrodes, thin-film yttria-stabilized zirconia electrolytes, and multi-layer lanthanum ferrite-based positive electrodes. Treated metallic interconnects with integral flow channels separate the cells and electrode gases. Sealing is accomplished with compliant mica-glass seals. A spring-loaded test fixture is used for mechanical stack compression. Due to the power level and the large number of cells in the hot zone, process gas flow rates are high and heat recuperation is required to preheat the cold inlet gases upstream of the furnace. Heat recuperation is achieved by means of two inconel tube-in-tube counter-flow heat exchangers. A current density of 0.3 A/cm2 will be used for these tests, resulting in a hydrogen production rate of 25 NL/min. Inlet steam flow rates will be set to achieve a steam utilization value of 50%. The 4 kW test will be performed for a minimum duration of 1000 hours in order to document the long-term durability of the stacks. Details of the test apparatus and initial results will be provided.

08 HYDROGEN↗

Similarity and generalized analysis of efficiencies of thermal energy storage systems

This paper examined the features of three typical thermal storage systems including: (1) direct storage of heat transfer fluid in containers, (2) storage of thermal energy in a packed bed of solid filler material, with energy being carried in/out by a flowing heat transfer fluid which directly contacts the packed bed, and (3) a system in which heat transfer fluid flows through tubes that are imbedded into a thermal storage material which may be solid, liquid, or a mixture of the two. The similarity of the three types of thermal storage systems was discussed, and generalized energy storage governing equations were introduced in both dimensional and dimensionless forms. The temperatures of the heat transfer fluid during energy charge and discharge processes and the overall energy storage efficiencies were studied through solution of the energy storage governing equations. Finally, provided in the paper are a series of generalized charts bearing curves for energy storage effectiveness against four dimensionless parameters grouped up from many of the thermal storage system properties including dimensions, fluid and thermal storage material properties, as well as the operational conditions including mass flow rate of the fluid, and the ratio of energy charge and discharge time periods. Engineers can conveniently look up the charts to design and calibrate the size of thermal storage tanks and operational conditions without doing complicated individual modeling and computations. It is expected that the charts will serve as standard tools for thermal storage system design and calibration.

25 ENERGY STORAGE↗

DEGRADATION ISSUES IN SOLID OXIDE CELLS DURING HIGH TEMPERATURE ELECTROLYSIS

Idaho National Laboratory (INL) is performing high-temperature electrolysis research to generate hydrogen using solid oxide electrolysis cells (SOECs). The project goals are to address the technical and degradation issues associated with the SOECs. This paper provides a summary of various ongoing INL and INL sponsored activities aimed at addressing SOEC degradation. These activities include stack testing, post-test examination, degradation modeling, and a list of issues that need to be addressed in future. Major degradation issues relating to solid oxide fuel cells (SOFC) are relatively better understood than those for SOECs. Some of the degradation mechanisms in SOFCs include contact problems between adjacent cell components, microstructural deterioration (coarsening) of the porous electrodes, and blocking of the reaction sites within the electrodes. Contact problems include delamination of an electrode from the electrolyte, growth of a poorly (electronically) conducting oxide layer between the metallic interconnect plates and the electrodes, and lack of contact between the interconnect and the electrode. INL's test results on high temperature electrolysis (HTE) using solid oxide cells do not provide a clear evidence whether different events lead to similar or drastically different electrochemical degradation mechanisms. Post-test examination of the solid oxide electrolysis cells showed that the hydrogen electrode and interconnect get partially oxidized and become non-conductive. This is most likely caused by the hydrogen stream composition and flow rate during cool down. The oxygen electrode side of the stacks seemed to be responsible for the observed degradation due to large areas of electrode delamination. Based on the oxygen electrode appearance, the degradation of these stacks was largely controlled by the oxygen electrode delamination rate. University of Utah (Virkar) has developed a SOEC model based on concepts in local thermodynamic equilibrium in systems otherwise in global thermodynamic non-equilibrium. This model is under continued development. It shows that electronic conduction through the electrolyte, however small, must be taken into account for determining local oxygen chemical potential, within the electrolyte. The chemical potential within the electrolyte may lie out of bounds in relation to values at the electrodes in the electrolyzer mode. Under certain conditions, high pressures can develop in the electrolyte just under the oxygen electrode (anode)/electrolyte interface, leading to electrode delamination. This theory is being further refined and tested by introducing some electronic conduction in the electrolyte.

08 HYDROGEN↗