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NSWCDD/TR-92/146

SAFT AMERICA LITHIUM SULFUR DIOXIDE BATTERY(P/N 38303301) FOR FLYRT APPLICATION:PERFORMANCE DISCHARGE TEST REPORT

BY J. A. BANNER P. B. DAVIS E. R. PEED C. S. WINCHESTER

RESEARCH AND TECHNOLOGY DEPARTMENT

AUGUST1991

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Approved for public release; distribution is unlimited.

~aS NAVAL SURFACE WARFARE CENTERDAHLGREN DIVISION .WHITE OAK DETACHMENT

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NSWCDDITR-92/146

SAFT AMERICA LITHIUM SULFUR DIOXIDE BATTERY(P/N 38303301) FOR FLYRT APPLICATION:PERFORMANCE DISCHARGE TEST REPORT

BY J. A. BANNER P. B. DAVIS E. R. PEED C. S. WINCHESTER

RESEARCH AND TECHNOLOGY DEPARTMENT

AUGUST 1991

Approved for public release; distribution is unlimited

NAVAL SURFACE WARFARE CENTERDAHLGREN DIVISION * WHITE OAK DETACHMENT

Silver Spring, Maryland 20903-5000

NSWCDD/TR-92/146

FOREWORD

The Battery Technology Group of the Electrochemistry Branch (Code R33) ofthe Naval Surface Warfare Center, White Oak Detachment, was tasked by theCountermeasures Group of the Naval Research Laboratory to execute a series ofperformance discharge tests on a lithium/sulfur dioxide (Li/SO2 ) battery. The batterywas designed and assembled by SAFT America (P/N 38303301) for use in the FlyingRadar Target (FLYRT) Demonstration Program. The preliminary battery tests weredesigned to determine the ability of the battery to fulfill the electrical requirementsof the FLYRT payload package. These requirements include a power requirement ofa nominal 600 watts for 10 to 12 minutes and a loaded voltage within the range of 66to 100 volts. This report details the tests performed, the results generated, and theconclusions and recommendations based on these results.

Approved by:

CARL E. MUELLER, HeadMaterials Division

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ABSTRACT

The Battery Technology Group of the Electrochemistry Branch (Code R33) ofthe Naval Surface Warfare Center, White Oak Detachment, was tasked by theCountermeasures Group of the Naval Research Laboratory to execute a series ofperformance discharge tests on a Li/SO 2 battery. The battery was designed andassembled by SAFT America (P/N 38303301) to be used for the Flying Radar Target(FLYRT) Demonstration Program. The preliminary battery tests included dischargetests designed to determine the ability of the SAFT America battery to deliver anominal 600 watts for 10 to 12 minutes within the voltage range of 66 to 100 volts.The battery was tested insulated in some cases to determine the effects of anadiabatic environment on its performance. The battery exceeded the goals set forpower and lifetime in all tests. However, events consistently occurred at the end ofbattery life that raised safety concerns with the present battery design. Data werealso analyzed for voltage delay characterization; no serious voltage delay problemswere evident.

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CONTENTS

Page

INTRO YDUCTIONRIPTIO ...... .................................................... 1

BATTERY DESCRIPTION .......................................................... 1

TEST O N E S. CRI...O ............................................................ 3TEST DESCRIPTION ......... ................................................... 3TEST RESU LTS .. ......... ...................................................... 3

TES T Tw o ............................................................. 6TEST I)ESCRIPTION ......... ................................................... 6

TEST RESU LTS........... ...................................................... 6

TESTTIIREESCRIPT IO ........................................................... 9TEST I)ESCRIPTION .............. .............................................. 9TEST RESU LTS. ........... ...................................................... 9

T E ST ESOU R ............................................................ 9TEST DESCRIPTION ......... ................................................... 9TEST RESULTS............................................................ 12

VOLTAGE DELAY ISSUES .......................................................... 12BAC KG RO U N D ................................................................. 12VOLTAGE DELAY IN PRELIMINARY TESTING .................................. 15

CONCLUSIONS AND RECOMMENDATIONS ........................................ 15

D IST R IB U T IO N .................................................................... (1)

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ILLUSTRATIONS

Fizure Page

1 SCHEMATIC OF li/SO2 BATTERY ..................................... 2

2 TEST CIRCUIT FOR 6-AMPERE CONSTANT CURRENT I)ISCIIARGE

(T EST # 1) ........................................................ 4

3 CONSTANT CURRENT I)ISCliARGE AT 6 AMPS ........................ 5

4 TEST CIRCUIT FOR 8-AMPERE CONSTANT CURRENT I)ISCHIARGE(TrEST # 2) ........................................................ 7

5 CONSTANT CURRENT DISCllARGE AT 8 AMPS ........................ 8

6 TEST CIRCUIT FOR 5.5-AMPERE RESISTIVE DISCHARGE (TEST #3) . 1.. 0

7 RESISTIVE I)ISCIlARGE AT 5.5 AMPS ................................. 11

8 TEST CIRCUIT FOR 8.75-AMPERE RESISTIVE DISCIIARGE(T EST # 4) ........................................................ 1 3

9 RESISTIVE I)ISCIIARGE AT 8.75 AMPS ................................ 14

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INTRODUCTION

The Electrochemistry Branch (Code R33) of the Naval Surface Warfare Center,White Oak Detachment (NSWCWODET), was tasked by the Naval ResearchLaboratory (NRL) to conduct battery performance discharge tests on four specializedlithium/sulfur dioxide (Li/SO2) battery packs designed and assembled by SAFTAmerica, Inc. The performance requirement for this battery is a nominal 600-wattdischarge for 10 to 12 minutes within the voltage range of 66 to 100 volts.

BATTERY DESCRIPTION

The battery (P/N 38303301) contains 33 nominal "1.25C" size SAFT AmericaLi/SO 2 cells (P/N L030SH) connected in series to produce an open circuit voltage of99 volts. The cells are arranged in four columns of eight cells each, with the thirty-third cell placed perpendicularly on one end (see Figure 1). Each string of eight cellsis independently packaged in a shrink wrap tube. The four 8-cell subassemblies areheld in place by lines of hot melt glue between adjacent cell columns and a covering ofshrink wrap around the entire battery. Each cell has a coined metal vent on thebottom of the cell can. The cells were less than 2 years old.

The battery contains three safety devices, an electrical fuse, a thermal fuse anda diode. The diode is located in the positive lead of the battery, and the two fuses arelocated in the negative lead. The batteries tested were assembled by SAFT Americaat their Valdese, North Carolina, plant.

It is anticipated that the thermal environment which the battery willexperience in the Flying Radar Target (FLYRT) vehicle will be extreme. The designconstraints of the payload and the vehicle indicate that the battery will discharge inan adiabatic manner. Additionally, because of nearby high thermal rejectionelectronics, the battery will be a potential heat sink for the thermal environment ofthe payload. To simulate this scenario, some of the discharge tests were performed onbatteries wrapped in insulation.

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NSWCDDfTR-92/146

end cell

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FIGURE 1. SCIhEMATIC OF Li/SO2 BATTERY

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TEST ONE

TEST DESCRIPTION

The first test was a constant current discharge at 6 amperes. The test wasperformed at room temperature and the battery was not insulated. The temperatureof the battery was monitored using five K-type thermocouples taped on the battery.The test circuit is illustrated in Figure 2. The performance goal for the battery at a6-ampere discharge rate was 10 to 12 minutes above 66 volts. The test was continuedinto voltage reversal to evaluate safety performance issues.

TEST RESULTS

The battery met the performance goal of 12 minutes and continued dischargingbenignly for an additional 28 minutes before ventings began. The discharge curve forthis test is presented in Figure 3. The battery delivered a nominal 530 watts for atotal of 40 minutes, with an average voltage of about 86 volts. At the end of thedischarge, some of the cells were entering voltage reversal. The battery sustainedvoltage reversal for approximately 1 minute before cell venting began.

The initial event consisted of several benign, muted ventings in which cellsreleased pressure through their vents with a popping sound. The gases escapedthrough the battery shrink wrap with little or no physical damage. Within5 minutes, however, a cell near the end of the battery (where the thirty-third cell islocated) vented violently, accompanied by a lithium fire which transitioned into acarbonaceous fire. The carbonaceous fire was identified by the coloration of the flameand is attributed to consumption of the acetonitrile electrolyte. The shrink wrap wasburned away exposing some of the cells. The ventings and fires spread to adjacentcells, and over the period of approximately 1 hour, all of the cells vented and burned.Some cells were physically separated from the battery pack by the force of theventings.

Inspection after the fire showed that six or seven cells had been detached fromthe battery. All of the cells had vented and were severely corroded. Some cellsappeared to have vented through the glass to metal seal, however, most vented fromthe coined vent. The postmortem analysis revealed that the cell closest to the outputleads did not vent. This cell possessed an open circuit voltage (OCV) of 2.92 volts atthe time of the postmortem analysis.

Although this summary indicates that the battery reached end of life in aspectacular fashion, it should be reiterated that the battery discharged safely forthree times the desired life, and did not fail violently until several cells were forcedinto voltage reversal.

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TEST TWO

TEST DESCRIPTION

The second test was a constant current discharge at 8 amperes. This test wasalso performed at room temperature, however the battery was insulated with twolayers (each layer was approximately 1 inch thick) of Fiberfrax" insulation securedby fiberglass tape. The battery was insulated to simulate an adiaba-c dischargecondition. Six K-type thermocouples were taped onto the surface of the battery(underneath the insulation) to monitor the temperature of the battery during thetest. The test circuit is illustrated in Figure 4. Because the battery performed sosuccessfully during the 6-ampere test, the performance goal chosen for the constantcurrent discharge at 8 amperes was also 10 to 12 minutes.

TEST RESULTS

The discharge curve for this test is presented in Figure 5. Although thedischarge curve shows a voltage drop initially, the battery delivered about 660 wattsover a lifetime of 20 minutes at an average voltage of 82.5 volts. Thus, the batterymet and exceeded all of its performance requirements in this test.

The first event was a muted, benign vent which occurred 18 minutes into thedischarge. The electrical load was disconnected at this time, but because of the heatheld in by the insulation, the battery went into thermal runaway, venting violently2 minutes later and burning for over 45 minutes. The ventings were accomparied bylithium and carbonaceous fire-. As in the first test, the fire began at the end of thebattery by the thirty-third cell and propagated to the other end.

The FiberfraxTM insulation did not burn, so the cells were held in theirconfiguration by the two layers of insulation and the fiberglass tape. Thepostmortem analysis revealed that all the cells were severely damaged, with mostventing through the vent, but with some venting through the glass to metal seal. Atleast two cells vented through holes in the cell case as well as through the vent area.However, the cell cases did not fragment. The nickel tabs and connectors werecorroded by the sulfur dioxide and the intense heat of the fire.

From this test, it is possible to conclude that although the battery could performfor the required life of 12 minutes at a rate of 8 amperes under adiabatic conditions,the potential for thermal runaway resulting in extensive battery ventingaccompanied by fire is increased under these circumstances.

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TEST THREE

TEST DESCRIPTION

During the initial setup for this test, it was discovered that the battery pack asreceived had one or more vented or leaky cells. This was determined because a strongsmell of SO2 was detected upon opening the sealed, transparent bag which held thebattery. A closer inspection of the battery was made in an effort to determine whichcell or cells had leaked. The gray shrink wrap was removed, but the cells could not beexposed further without the risk of short circuiting them. From what was visible, itwas not possible to locate the faulty cell(s). There was also no more evidence of SO2 ,either visual or olfactory.

Based on the supposition that a leaky cell represented a cell with decreasedcapacity, it was decided that the battery should be discharged resistively at a lowrate. This allowed the faulty cell(s) to be forced into reversal and subsequent failureby the balance of cells in the battery assembly. This was accomplished by subjectingthe battery to a resistive discharge at 5.5 amperes. The battery temperature wasmonitored using six K-type thermocouples taped to individual cells. The test circuitis illustrated in Figure 6.

TEST RESULTS

The discharge curve for this test is presented in Figure 7. The test was endedafter an apparent single venting occurred 35 minutes into the discharge. The batterydelivered about 481 watts during this time, with an average voltage of about87.5 volts.

A postmortem analysis of the battery was performed to determine if the safetydevices functioned. Initial inspection of the battery pack revealed that the positivelead was severed into two pieces at thepoint where the diode was located. Upondisassembling the pack, a single vented cell was located directly beneath the pointwhere the positive lead was severed. Neither the electrical fuse nor the thermal fuseappeared to have functioned. It appears that the cell which had leaked SO2 hadsuffered a capacity loss and was forced into reversal by the stronger cells in the series.It subsequently vented directly onto the positive lead, severing it and ending thedischarge.

TEST FOUR

TEST DESCRIPTION

The final test was a resistive discharge at 8.75 amperes. The test wasperformed at room temperature and the battery was insulated in one layer ofFiberfrax ' to simulate the adiabatic nature of the application. Battery temperature

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during the test was monitored using six K-type thermocouples taped to the surface ofthe battery (underneath the insulation). The test circuit is illustrated in Figure 8.The goal of this test was to determine if an event or venting would occur at the end ofbattery life without the cells being pushed into voltage reversal by either a powersource in the circuit or the presence of a weak cell.

TEST RESULTS

The discharge curve for this test is presented in Figure 9. The batterydischarged successfully for 22 minutes. The voltage curve is relatively flat, and thebattery delivered about 721 watts at an average of approximately 82.5 volts in22 minutes. This performance exceeds all of the requirements for the application. Asbefore, the insulation allowed sufficient thermal buildup so that cells ventedviolently near end of life, causing both lithium and carbonaceous fires. These fireswere similar to the results in the second test. The condition of the cells after the fireburned out was also similar to the postmortem results of test two. Most cells ventedthrough the coined metal vent, but a few vented violently through the glass to metalseal and two through the cell case. All of the cells were severely corroded.

From the results of this test, it was concluded that discharging this battery toend of life in an adiabatic environment will lead to a failure involving violent ventingand fires. However, the battery is able to safely perform for the required lifetime of10 to 12 minutes and deliver more than the required 600 watts during that time.

VOLTAGE DELAY ISSUES

BACKGROUND

Voltage delay is a passivation layer phenomenon associated with most activebatteries, particularly those batteries subjected to long-term storage or highextremes of temperature and specifically to those exposed to the combination of bothconditions. The phenomenon is associated with the formation of anodic films.Voltage delay is manifested by a high a pparent cell resistance which decreases thecell voltage to lower than expected levels upon load application and maintains thepolarized condition for several seconds to several hours before voltage recoveryoccurs.

Voltage delay in lithium anode/sulfur dioxide cathode batteries is associatedwith the formation of a layer of tightly packed lithium dithionite (Li2S 2 0 4 ) crystalson the lithium anode surface. This layer is a by-product of SO2 reaction with thelithium metal anode. The rate of film formation and its characteristic density andthickness are increased by extreme (> 40°C) temperature. This passivation layerserves a beneficial purpose in that it is the primary mechanism that allows theLi/SO 2 chemistry to withstand prolonged storage at elevated temperatures withoutextreme loss of capacity. However, significant voltage delays may be expected if thefilm becomes too thick.

Breakup of the film, sufficient to allow substantial current flow (>0.1 mA/cm 2 )with low polarization, can be caused by either impact shock (external mechanical

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disruption of the film layer) or by electrochemical discharge of the anode through themicropores of the film. Sustaining a moderate discharge load on a battery/cell willcause breakup of the passivation layer. 'Vake-up" loadings, typically using a "slow-blo" fuse in a low resistance (short) circuit have often been effective in the breakup ofthe passivation layer allowing immediate discharge above minimum voltages.

VOLTAGE DELAY IN PRELIMINARY TESTING

The four battery packs (consisting of 33 Li/SO 2 cells in series) were dischargedby turning on the load abruptly, without precursor loading or "wake-up" loadingbeing applied to the battery packs. Minimal voltage delay was observed on the fourbattery pack tests, and in all cases, battery voltage did not drop below the specifiedminimum voltage for the application (66 VDC). For three of the tests, cell/batteryrecovery took less than 1 minute to reach stable voltage plateaus.

However, as depicted in the accompanying voltage-time traces for the batterytests, the voltage required several minutes to stabilize in the second test (seeFigure 5). This voltage curve exhibits an anomalous double-dip followed byrecovery. The battery discharged in this test required slightly more than 2 minutesto attain stable discharge voltage. This double-dip behavior may be associated withthe overall lower performance from the 8.0 ampere discharge test than that observedfrom the 8.75 ampere discharge test (test four - see Figure 9). The voltage dipbehavior may be indicative of a weak cell in the series string or of improperly storedcells.

Discharge testing was conducted at ambient temperatures (250C) underdifferent current drain rates (5.5 to 8.5 amperes) with reasonably fresh (< 2-year old)cells that had presumably not been exposed to abusively high temperature storage. Iftesting had been conducted with cells under cold, preconditioning extremes (-40°C to00C), with old cells and/or with cells that had undergone long-term high temperaturestorage, the voltage delay could have been severe, perhaps dropping to less than0.1 VDC/cell (< 3.0 VDC/battery) until the passivation layer breakup occurred.

CONCLUSIONS AND RECOMMENDATIONS

The four tests performed on the 33-cell Li/SO 2 battery designed and assembledby SAFT America for NRL reveal that the battery can meet the performancedischarge criteria set forth by NRL for their FLYRT application. However, theviolent behavior of this battery at end of life raises clear safety concerns. The resultsfrom the fourth test show that voltage reversal of the whole battery pack at end of lifeis not necessary to induce violent venting and fire. Heat buildup is sufficient to causesafety hazards and limit performance. It is also obvious that the safety devices asthey exist in the present design are insufficient, and that some design changes will benecessary to improve battery safety.

Based upon the voltage delay behavior of the four preliminary tests performed,moderate to warm precondition temperature should have little impact on theperformance of the batteries, providing that future payload batteries use fresh cells of

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known storage history. Cold preconditioning of the batteries, as may be expectedunder demonstration flights scenarios, may cause excessive voltage delay.

Self-heating of the cell stack under adiabatic discharge load conditions will aidin alleviating the cold condition effects on battery performance, after the batteryrecovers from the voltage delay. Alternatively, usage of a wake-up pulse applicationto the battery stack would be considered to assure rapid start-up of the battery pack.Electrical wiring schemes for applying the wake-up current pulse should be externalto the safety devices in the battery circuit.

Performance of the battery pack in an adiabatic environment might not bepossible if the pack is preconditioned above 60°C. Above 600C, the temperatureincrease of the battery pack would be sufficient to cause the thermal fuse to function.Should the fuse fail to operate, as experienced during this test program, the batterywould cease performance as the cells went into thermal runaway.

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EIECTRONICS SYSTEM DIVISIONATTrN A P KARPINSKY 1 PO BOX 750WI IITTAKER TECIIN ICAL PROI)UCTS FISI hERS NY 1445392 MECIIANIC STREEITPAWCATUCK CT 02891 ATTN J CAPUTO

LORAL DEFENSE SYSTEMSATTN BATTEIRY SAILES IN VISION 1 1210 MASSILLON ROADPANASONIC INDUSTRIAL CO AKRON Ol 44315-000111O BOX 1511SECAUCUS NJ 07094 ATTN M WALSH

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ATTN N ISAACSATTN A IIIMY I CATALYST RESEARCIIWESTINGHOUSE ELECTRIC CORP 38 LOVETON CIRCLE1310 BEULAII ROAD SPARKS MD 21152PITTSBURGlH PA 15235

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NSWCDDfTR-92/146

I)ISTI'iBUTION (CONT.)

Copies

ATTN R ST'ANIEWICZ 1G CIIAGNON 1

SAFI' AMERICA107 BEAVER COURTCOCKEYSVILLE MD 21030

ATTN N SIIUSTrER IWESTINGHlOUSEELECThIrCAI. POWER SYSTEMS476 CENTER STREETCIHARDON O!l 44024

INTERNAL DISTRIBUTION:E231 2E232 3E342 (GIDEP) 1E!35 1R30 I1133 11133 (STAFF) 27!{33 (BANNER) 30R33 (PEED) 11133 (WEST-FREEMAN) I

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Form ApprovedREPORT DOCUMENTATION PAGE OMB No. 0704-0188

'ubhii reporting buraen for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions. searching existing datasourc es. gathering and maintaining the data needed, and completing and reviewing the collection of information. Send comments regarding this burden esti mate or any otheraspect of this collection of information, including suggestions for reducing this burden, to Washington Headquarters Services, Directorate for Information Operations andReports. 1215 Jefferson Davis Highway. Suite 1204. Arlington. VA 22202-4302. and to the Office of Management and Budget. Paperwork Reduction Project (0704-0188).Washington, DC 20503

1. AGENCY USE ONLY (Leave blank) 2. REPORT DATE 3. REPORT TYPE AND DATES COVERED

August 1991 August 1991 to March 1992

4. TITLE AND SUBTITLE 5. FUNDING NUMBERSSAFT America Lithium Sulfur Dioxide Battery (PIN 38303301) for FLYRT Application-Performance Discharge Test Report

6. AUTHOR(S)

J. A. Banner, P. B. Davis, E. R. Peed, and C. S. Winchester

7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) 8. PERFORMING ORGANIZATIONREPORT NUMBER

Naval Surface Warfare Center (Code R33)10901 New IHampshire Avenue NSWCDDfTR-92/146Silver Spring, MD 20903-5000

9. SPONSORING/MONITORING AGENCY NAME(S) AND ADDRESS(ES) 10. SPONSORING/MONITORINGAGENCY REPORT NUMBER

11. SUPPLEMENTARY NOTES

12a. DISTRIBUTION/AVAILABILITY STATEMENT 12b. DISTRIBUTION CODE

Approved for public release; distribution is unlimited.

13. ABSTRACT (Maximum 200 words)

The Battery Technology Group of the Electrochemistry Branch (Code R33) of the Naval SurfaceWarfare Center, White Oak Detachment, was tasked by the Countermeasures Group of the NavalResearch Laboratory to execute a series of performance discharge tests on a Li/SO2 battery. The batterywas designed and assembled by SAFT America (P/N 38303301) to be used for the Flying Radar Target(FLYRT) Demonstration Program. The preliminary battery tests included discharge tests designed todetermine the ability of the SAFT America battery to deliver a nominal 600 watts for 10 to 12 minuteswithin the voltage range of 66 to 100 volts. The battery was tested insulated in some cases to determinethe effects of an adiabatic environment on its performance. The battery exceeded the goals set for powerand lifetime in all tests. However, events consistently occurred at the end of battery life that raised safetyconcerns with the present battery design. Data were also analyzed for voltage delay characterization; noserious voltage delay problems were evident.

14. SUBJECT TERMS 15. NUMBER OF PAGESLithium Battery 30Flying Radar Target (FLYRT) 16. PRICE CODELithium Sulfur Dioxide Chemistry

17. SECURITY CLASSIFICATION 18. SECURITY CLASSIFICATION 19. SECURITY CLASSIFICATION 20. LIMITATION OF

OF REPORT OF THIS PAGE OF ABSTRACT ABSTRACT

UNCLASSIFIED UNCLASSIFIED UNCLASSIFIED SAR4SN 7540-01-280-5500 Standard Form 298 (Rev. 2-89'

Prescribed by ANSI Std Z39-16298-102