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Failure Analysis of Mark 1A Lithium/Iron Sulfide Battery

Description: The Mark 1A lithium/iron sulfide electric-vehicle battery, which consisted of two 20-kW-hr modules containing 60 cells each, was fabricated by Eagle-Picher Industries, Inc. and delivered to ANL for testing in May 1979. During startup heating prior to electrical testing, a short circuit developed in one of the modules, which resulted in a progressive failure of the cells. The other module, which was alongside and connected in series, was unaffected by the failure. The initial indication of difficulty was a small drop in the voltage of several cells, followed by short circuits in the balance of the cells and localized temperatures above 1000 C. A team consisting of ANL and Eagle-Picher personnel conducted a detailed failure analysis as the failed module was disassembled. The other module was also examined for purposes of comparison. The general conclusion was that the short circuit was initiated by electrolyte leakage and resulting corrosion in the nearby region which formed metallic bridges between cells and the cell ray, or arcing between cells and the cell tray through the butt joints in the electrical insulation. The above two mechanisms were also believed to be responsible for the failure propagation.
Date: October 1980
Creator: Kolba, V. M.; Battles, J. E.; Geller, J. D. & Gentry, K.
Partner: UNT Libraries Government Documents Department

Post-Test Examinations of Li-Al/FeSx Secondary Cells

Description: Post-test examinations were conducted to determine failure mechanisms, electrode morphologies, and in-cell corrosion of cell components, and to recommend appropriate design changes for improved cell performance and reliability. The reactive electrode materials required the design and construction of a special metallographic glovebox facility. Combinations of macro- and microscopic examinations determined that electrical short circuits were the predominant causes of cell failure. The major short circuit mechanism was extrusion of active material from one electrode and its subsequent contact with the opposing electrode (opposite polarity). Other mechanisms for short circuits included metallic deposits across separators, metallic deposits across the feed-through insulator (electrolyte leakage and corrosion), equipment malfunctions, cell assembly difficulties, etc. Post-test examinations confirmed that the short circuits were of mechanical origin; appropriate design changes were, therefore, recommended. Extensive microscopic examinations were conducted on both negative and positive electrodes to determine the morphology. Agglomeration of Li-Al was observed in the negative electrodes of most multi-plate cells. Examinations showed that the sulfides in the positive electrode remained as discrete particles in an electrolyte matrix. Also discussed are the results of post-test examinations to determine the following: lithium gradients in the negative electrodes, electrode expansion, materials distribution, copper deposition within electrode separators of FeS cells, Li2S deposits within electrode separators of FeS3 cells, and the in-cell corrosion of current collector materials in positive and negative electrodes.
Date: December 1980
Creator: Battles, J. E.; Mrazek, F. C. & Otto, N. C.
Partner: UNT Libraries Government Documents Department

Investigation of primary Li-Si/FeS/sub 2/ cells

Description: The factors that limit the performance of thermally activated Li-Si/FeS/sub 2/ batteries were defined through the use of electrochemical characterization tests and post-test examinations. For the characterization tests, 82 individual cells were instrumented with multiple voltage sensors and discharged under isothermal and isobaric conditions. The voltage data for the sensors were recorded to determine the ohmic and electrochemical impedances of each cell component at different levels of discharge. The data analysis completed to date has demonstrated that this approach can successfully differentiate the influence of various operating parameters (e.g., temperature, current density), electrode structures (e.g., FeS/sub 2/ particle size), and additives on cell capacity, specific energy, and power capability. Thirty cells selected from these tests and additional tests at SNL were examined using optical and scanning electron microscopy, energy dispersive spectroscopy, and X-ray diffraction. These analyses documented microstructural and compositional changes in the active materials and electrolyte. In general, the electrochemical impedance of the FeS/sub 2/ electrode limited cell performance. Several methods (including use of fine FeS/sub 2/ particle size, graphite additions, and higher operating temperatures) produced measurable reductions in this impedance and yielded significant improvements in specific energy and power. Additions of KCl to the negative electrode extended the low-temperature capacity of this electrode by counterbalancing gradients in electrolyte composition that develop during discharge.
Date: April 1, 1987
Creator: Redey, L.; Smaga, J.A.; Battles, J.E. & Guidotti, R.
Partner: UNT Libraries Government Documents Department

Pyrometallurgical processing of Integral Fast Reactor metal fuels

Description: The pyrometallurgical process for recycling spent metal fuels from the Integral Fast Reactor is now in an advanced state of development. This process involves electrorefining spent fuel with a cadmium anode, solid and liquid cathodes, and a molten salt electrolyte (LiCl-KCl) at 500{degrees}C. The initial process feasibility and flowsheet verification studies have been conducted in a laboratory-scale electrorefiner. Based on these studies, a dual cathode approach has been adopted, where uranium is recovered on a solid cathode mandrel and uranium-plutonium is recovered in a liquid cadmium cathode. Consolidation and purification (salt and cadmium removal) of uranium and uranium-plutonium products from the electrorefiner have been successful. The process is being developed with the aid of an engineering-scale electrorefiner, which has been successfully operated for more than three years. In this electrorefiner, uranium has been electrotransported from the cadmium anode to a solid cathode in 10 kg quantities. Also, anodic dissolution of 10 kg batches of chopped, simulated fuel (U--10% Zr) has been demonstrated. Development of the liquid cadmium cathode for recovering uranium-plutonium is under way.
Date: January 1, 1991
Creator: Battles, J.E.; Miller, W.E. & Gay, E.C.
Partner: UNT Libraries Government Documents Department

Actinide consumption: Nuclear resource conservation without breeding

Description: A new approach to the nuclear power issue based on a metallic fast reactor fuel and pyrometallurgical processing of spent fuel is showing great potential and is approaching a critical demonstration phase. If successful, this approach will complement and validate the LWR reactor systems and the attendant infrastructure (including repository development) and will alleviate the dominant concerns over the acceptability of nuclear power. The Integral Fast Reactor (IFR) concept is a metal-fueled, sodium-cooled pool-type fast reactor supported by a pyrometallurgical reprocessing system. The concept of a sodium cooled fast reactor is broadly demonstrated by the EBR-II and FFTF in the US; DFR and PFR in the UK; Phenix and SuperPhenix in France; BOR-60, BN-350, BN-600 in the USSR; and JOYO in Japan. The metallic fuel is an evolution from early EBR-II fuels. This fuel, a ternary U-Pu-Zr alloy, has been demonstrated to be highly reliable and fault tolerant even at very high burnup (160-180,000 MWd/MT). The fuel, coupled with the pool type reactor configuration, has been shown to have outstanding safety characteristics: even with all active safety systems disabled, such a reactor can survive a loss of coolant flow, a loss of heat sink, or other major accidents. Design studies based on a small modular approach show not only its impressive safety characteristics, but are projected to be economically competitive. The program to explore the feasibility of actinide recovery from spent LWR fuel is in its initial phase, but it is expected that technical feasibility could be demonstrated by about 1995; DOE has not yet committed funds to achieve this objective. 27 refs.
Date: January 1, 1991
Creator: Hannum, W.H.; Battles, J.E.; Johnson, T.R. & McPheeters, C.C.
Partner: UNT Libraries Government Documents Department

Magnesium transport extraction of transuranium elements from LWR fuel

Description: This report discusses a process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl{sub 2} and a U-Fe alloy containing not less than about 84% by weight uranium at a temperature in the range of from about 800{degrees}C to about 850{degrees}C to produce additional uranium metal which dissolves in the U-Fe alloy raising the uranium concentration and having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein. The CaCl{sub 2} having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO{sub 2}. The Ca metal and CaCl{sub 2} is recycled to reduce additional oxide fuel. The U-Fe alloy having transuranium actinide metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with Mg metal which takes up the actinide and rare earth fission product metals. The U-Fe alloy retains the noble metal fission products and is stored while the Mg is distilled and recycled leaving the transuranium actinide and rare earth fission products isolated.
Date: December 31, 1991
Creator: Ackerman, J.P.; Battles, J.E.; Johnson, T.R.; Miller, W.E. & Pierce, R.D.
Partner: UNT Libraries Government Documents Department

Uranium chloride extraction of transuranium elements from LWR fuel

Description: A process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels containing rare earth and noble metal fission products as well as other fission products is disclosed. The oxide fuel is reduced with Ca metal in the presence of Ca chloride and a U-Fe alloy which is liquid at about 800{degrees}C to dissolve uranium metal and the noble metal fission product metals and transuranium actinide metals and rare earth fission product metals leaving Ca chloride having CaO and fission products of alkali metals and the alkali earth metals and iodine dissolved therein. The Ca chloride and CaO and the fission products contained therein are separated from the U-Fe alloy and the metal values dissolved therein. The U-Fe alloy having dissolved therein reduced metals from the spent nuclear fuel is contacted with a mixture of one or more alkali metal or alkaline earth metal halides selected from the class consisting of alkali metal or alkaline earth metal and Fe or U halide or a combination thereof to transfer transuranium actinide metals and rare earth metals to the halide salt leaving the uranium and some noble metal fission products in the U-Fe alloy and thereafter separating the halide salt and the transuranium metals dissolved therein from the U-Fe alloy and the metals dissolved therein.
Date: December 31, 1991
Creator: Miller, W.E.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R. & Pierce, R.D.
Partner: UNT Libraries Government Documents Department

Investigation of Primary Li-Si/FeS2 Cells

Description: The factors that limit the performance of thermally activated Li-Si/FeS2 batteries were defined through the use of electrochemical characterization tests and post-test examinations. For the characterization tests, 82 individual cells were instrumented with multiple voltage sensors and discharged under isothermal and isobaric conditions. The voltage data for the sensors were recorded to determine the ohmic and electrochemical impedances of each cell component at different levels of discharge. The data analysis completed to date has demonstrated that this approach can successfully differentiate the influence of various operating parameters (e.g., temperature, current density), electrode structures (e.g., FeS2 particle size), and additives on cell capacity, specific energy, and power capability. Thirty cells selected from these tests and additional tests at SNL were examined using optical and scanning electron microscopy, energy dispersive spectroscopy, and X-ray diffraction. These analyses documented microstructural and compositional changes in the active materials and electrolyte. In general, the electrochemical impedance of the FeS2 electrode limited cell performance. Several methods (including use of fine FeS2 particle size, graphite additions, and higher operating temperatures) produced measurable reductions in this impedance and yielded significant improvements in specific energy and power. Additions of KCl to the negative electrode extended the low-temperature capacity of this electrode by counterbalancing gradients in electrolyte composition that develop during discharge.
Date: April 1987
Creator: Redey, L.; Smaga, J. A.; Battles, J. E. & Guidotti, Ronald
Partner: UNT Libraries Government Documents Department

Salt transport extraction of transuranium elements from LWR fuel

Description: This report discusses a process of separating transuranium actinide values from uranium values present in spent nuclear oxide fuels which contain rare earth and noble metal fission products. The oxide fuel is reduced with Ca metal in the presence of CaCl{sub 2} and a Cu-Mg alloy containing not less than about 25% by weight Mg at a temperature in the range of from about 750{degrees}C to about 850{degrees}C to precipitate uranium metal and some of the noble metal fission products leaving the Cu-Mg alloy having transuranium actinide metals and rare earth fission product metals and some of the noble metal fission products dissolved therein. The CaCl{sub 2} having Cao and fission products of alkali metals and the alkali earth metals and iodine dissolved therein is separated and electrolytically treated with a carbon electrode to reduce the CaO to Ca metal while converting the carbon electrode to CO and CO{sub 2}. The Ca metal and CaCl{sub 2} is recycled to reduce additional oxide fuel. The Cu-Mg alloy having transuranium metals and rare earth fission product metals and the noble metal fission products dissolved therein is contacted with a transport salt including Mg C1{sub 2} to transfer Mg values from the transport salt to the Cu-Mg alloy .hile transuranium actinide and rare earth fission product metals transfer from the Cu-Mg alloy to the transport salt. Then the transport salt is mixed with a Mg-Zn alloy to transfer Mg values from the alloy to the transport salt while the transuranium actinide and rare earth fission product values dissolved in the salt are reduced and transferred to the Mg-Zn alloy.
Date: December 31, 1991
Creator: Pierce, R.D.; Ackerman, J.P.; Battles, J.E.; Johnson, T.R. & Miller, W.E.
Partner: UNT Libraries Government Documents Department

IFR fuel cycle--pyroprocess development

Description: The Integral Fast Reactor (IFR) fuel cycle is based on the use of a metallic fuel alloy, with nominal composition U-2OPu-lOZr. In its present state of development, this fuel system offers excellent high-burnup capabilities. Test fuel has been carried to burnups in excess of 20 atom % in EBR-II irradiations, and to peak burnups over 15 atom % in FFTF. The metallic fuel possesses physical characteristics, in particular very high thermal conductivity, that facilitate a high degree of passive inherent safety in the IFR design. The fuel has been shown to provide very large margins to failure in overpower transient events. Rapid overpower transient tests carried out in the TREAT reactor have shown the capability to withstand up to 400% overpower conditions before failing. An operational transient test conducted in EBR-II at a power ramp rate of 0.1% per second reached its termination point of 130% of normal power without any fuel failures. The IFR metallic fuel also exhibits superior compatibility with the liquid sodium coolant. Equally as important as the performance advantages offered by the use of metallic fuel is the fact that this fuel system permits the use of an innovative reprocessing method, known as pyroprocessing,'' featuring fused-salt electrorefining of the spent fuel. Development of the IFR pyroprocess has been underway at the Argonne National Laboratory for over five years, and great progress has been made toward establishing a commercially-viable process. Pyroprocessing offers a simple, compact means for closure of the fuel cycle, with anticipated significant savings in fuel cycle costs.
Date: January 1, 1992
Creator: Laidler, J.J.; Miller, W.E.; Johnson, T.R.; Ackerman, J.P. & Battles, J.E.
Partner: UNT Libraries Government Documents Department

Lithium/Iron Sulfide Batteries for Electric-Vehicle Propulsion and Other Applications Progress Report for October 1979-March 1980

Description: This report covers the research and development activities of the program at Argonne National Laboratory (ANL) on lithium/iron sulfide batteries during the period October 1979-March 1980.
Date: August 1980
Creator: Barney, Duane L.; Steunenberg, R. K.; Chilenskas, A. A.; Gay, E. C.; Battles, J. E.; Miller, W. E. et al.
Partner: UNT Libraries Government Documents Department

Lithium/Iron Sulfide Batteries for Electric-Vehicle Propulsion and Other Applications Progress Report for October 1980-September 1981

Description: This report covers the research, development, and management activities of the programs involving high-performance lithium-aluminum/iron sulfide batteries at Argonne National Laboratory (ANL) and at contractors' laboratories during the period October 1980 through September 1981. These batteries, which are being developed for electric-vehicle propulsion and stationary energy-storage applications, consist of vertically oriented prismatic cells with one or more inner positive electrodes of FeS or FeS2, facing negative electrodes of lithium-aluminum, and molten LiCl-KC1 electrolyte.
Date: February 1982
Creator: Barney, Duane L.; Steunenberg, R. K.; Chilenskas, A. A.; Gay, E. C.; Battles, J. E.; Hudson, R. et al.
Partner: UNT Libraries Government Documents Department

Chemical Technology Division Annual Technical Report: 1991

Description: Annual report of the Argonne National Laboratory Chemical Technology Division (CMT) discussing the group's activities during 1991. These included electrochemical technology; fossil fuel research; hazardous waste research; nuclear waste programs; separation science and technology; integral fast reactor pyrochemical processes; actinite recovery; applied physical chemistry; basic chemistry research; analytical chemistry; research and development; and computer applications.
Date: March 1992
Creator: Argonne National Laboratory. Chemical Technology Division.
Partner: UNT Libraries Government Documents Department

Chemical Technology Division Annual Technical Report: 1992

Description: Annual report of the Argonne National Laboratory Chemical Technology Division (CMT) discussing the group's activities during 1992. These included electrochemical technology; fossil fuel research; hazardous waste research; nuclear waste programs; separation science and technology; integral fast reactor pyrochemical processes; actinide recovery; applied physical chemistry; basic chemistry research; analytical chemistry; applied research and development; and computer applications.
Date: June 1993
Creator: Argonne National Laboratory. Chemical Technology Division.
Partner: UNT Libraries Government Documents Department

Chemical Technology Division Annual Technical Report: 1993

Description: Annual report of the Argonne National Laboratory Chemical Technology Division (CMT) discussing the group's activities during 1992. These included electrochemical technology; fossil fuel research; hazardous waste research; nuclear waste programs; separation science and technology; integral fast reactor pyrochemical processes; actinide recovery; applied physical chemistry; basic chemistry research; and analytical chemistry.
Date: April 1994
Creator: Battles, J. E.; Myles, K. M.; Laidler, J. J. & Green, D. W.
Partner: UNT Libraries Government Documents Department

Electromagnetic continuous casting project: Final report

Description: This report describes the work on development of an electromagnetic casting process for steel, which was carried out at Argonne National Laboratory between January 1985 and December 1987. This effort was concerned principally with analysis and design work on magnet technology, liquid metal feed system, coolant system, and sensors and process controllers. Experimentation primarily involved (1) electromagnetic studies to determine the conditions and controlling parameters for stable levitation and (2) feed-system studies to establish important parameters that control and influence fluid flow from the liquid metal source to the caster. 73 refs., 91 figs., 11 tabs.
Date: October 1, 1988
Creator: Battles, J.E.; Rote, D.M.; Misra, B.; Praeg, W.F.; Hull, J.R.; Turner, L.R. et al.
Partner: UNT Libraries Government Documents Department

Development of high-specific-energy batteries for electric vehicles. Progress report, February 1973--July 1973

Description: A high-specific-energy lithium/sulfur battery having the performance characteristics required for powering pollutionfree automobiles is described. The cells currently under development have negative electrodes of molten lithium and positive electrodes of sulfur (plus an additive to reduce the sulfur vapor pressure) separated by a molten lithium halide-containing electrolyte. The operating temperature of the cells is about 400 deg C. The performance goals for a single cell include a capacity density of 0.4 A-hr/cm/sup 2/ at a current density of 0.1 A/cm/sup 2/, a peak power density of 1-2 W/cm/sup 2/, and a minimum cycle life of 1000 cycles. Cells with positive electrodes consisting of sulfurarsenic-carbon mixtures in graphite housings have achieved short-time peak power densities and capacity densities that meet or exceed the goals for a single cell. A capacity density of 0.1 A-hr/cm/sup 2/ has been sustained at a discharge current density of 0.1 A/cm/sup 2/l (1-V cutoff) for more than 500 hr and 100 cycles. Improvement in cell design is needed, however, to achieve higher sulfur utilization and longer cell lifetimes. (auth)
Date: December 1, 1973
Creator: Nelson, P.A.; Gay, E.C.; Steunenberg, R.K.; Battles, J.E.; Schertz, W.W.; Vissers, D.R. et al.
Partner: UNT Libraries Government Documents Department

IFR fuel cycle

Description: The next major milestone of the IFR program is engineering-scale demonstration of the pyroprocess fuel cycle. The EBR-II Fuel Cycle Facility has just entered a startup phase, which includes completion of facility modifications and installation and cold checkout of process equipment. This paper reviews the development of the electrorefining pyroprocess, the design and construction of the facility for the hot demonstration, the design and fabrication of the equipment, and the schedule and initial plan for its operation.
Date: January 1, 1992
Creator: Battles, J.E.; Miller, W.E. (Argonne National Lab., IL (United States)); Lineberry, M.J. & Phipps, R.D. (Argonne National Lab., Idaho Falls, ID (United States))
Partner: UNT Libraries Government Documents Department