Characterization of Spent Fuel Approved Testing Material--ATM-104

416 Pages·2005·32.24 MB·English

|
zl 0i_ PNL-5109-104
UC-802
III I I I IIII rl I II I
MC:C:
Materials Characterization Center
Characterization of
Spent Fuel Approved
Testing Material--ATM-104
I
December 1991
=
Prepared for the U.S. Department of Energy
under Contract DE-AC06-76RLO 1830
Pacific Northwest Laboratory
Operated for the U.S. Department of Energy
by Battelle Memorial Institute
Z
_ 0
J
0
=
DISCLAIMER
This report was prepared asan account of work sponsored by an agency of the
United StatesGovernment. Neither the United StatesGovernmenl nor any agency
thereof, nor Battelle Memorial Institute, nor any of their employees, makes any
warranty, expressedorimplied, orassumesanylegal liability orresponsibility for
theaccuracy, completeness, orusefulnessofanyinformation, apparatus, product,
orprocessdisclosed,orrepresentsthatitsusewould notinfringe privately owned
rights. Reference herein toany specific commercial product, process, orservice b/
lradename, trademark, manufacturer, orotherwise does notnecessarily constitute
or imply its endorsement, recommendation, or favoring by the United States
Government orany agency thereof, or Battelle Memorial Institute. The views and
opinions ofauthors expressed herein do not necessarily stateor reflect those of the
United StatesGovernment orany agency thereof.
PACIFIC NORTHWEST LABORATORY
opera ted by
BATTELLE MEMORIAL INSTITUTE
for tile
UNITED STATES DEPARTMENT OF ENERGY
under Contract DE.ACO6.,76RLO 1830
PrintedintheUnitedStatesofAmerica
AvailabletoDOEandDOEcontractorsfrom the
OfficeofScientificandTechnicalInformation, P.O.Box62,OakRidge,TN 37831;
pricesavailablefrom(615) 576-8401.FTS626-8401.
AvailabletothepublicfromtheNationalTechnicalInformationService,
U.S.DepartmentofCommerce,52U5PortRoyalRd.,Springfield,VA22161.
PNL--5109-104
DE92 0066 36
CHARACTERIZATIONOF SPENTFUEL
APPROVEDTESTING MATERIAL--ATM-lO4
R. J. Guenther
D. E. Blahnik
U. P. Jenquin
J. E. Mendel
L. E. Thomas
C. K. Thornhill
December 1991
Prepared for
the U.S. Department of Energy
under Contract DE-ACO6-76RLO 1830
Pacific Northwest Laboratory
Richland, Washington 99352
...... -........ '........... _LZ',"_I'STUIqL._!'v'ITT'L'i"_
ABSTRACT
The characterizationdata obtainedto date are describedfor Approved
TestingMaterial104 (ATM-lO4),which is spentfuel fromAssemblyD047 of the
CalvertCliffsNuclearPowerPlant (UnitI), a pressurized-waterreactor.
This reportis one in a seriesbeingpreparedby the MaterialsCharacterlza-
tion Center at PacificNorthwestLaboratory(PNL)on spentfuelATMs. The
ATMs are receivingextensiveexaminationsto providea sourceof well-
characterizedspent fuel for testingin the U.S. Departmentof EnergyOffice
of CivilianRadioactiveWasteManagement(OCRWM)Program. ATM-lO4consistsof
128 full-lengthirradiatedfuel rodswith rod-averageburnupsof about
42 MWd/kgMand expectedfissiongas releaseof aboutI%.
A varietyof analyseswere performedto investigatecladdingcharac-
teristics,radionuclideinventory,and redistributionof fissionproducts.
Characterizationdata includeI) fabricatedfuel design,irradiationhistory,
and subsequentstorageand handlinghistory;2) isotopicgamma scans;
3) fissiongas analyses;4) ceramographyof the fuel and metallographyof the
cladding;5) specialfuel studiesinvolvinganalyticaltransmissionelectron
microscopy(AEM)and electronprobemicroanalyses(EPMA);6) calculated
nuclideinventoriesand radioactivitiesin the fuel and cladding;and
7) radiochemicalanalysesof the fuel and cladding.
iii
CONTENTS
ABSTRACT ............................... iii
ACKNOWLEDGMENT.S.......................... xiv
ACRONYMS............................... xv
KEYDEFINITIONS ........................... xvi
1.0 INTRODUCTION ....... . .................. 1.1
2.0 SUMMARAYNDCONCLUSIONS..................... 2.1
3.0 FABRICATION,IRRADIATION, ANDHANDLINGHISTORYFORATM-lO4 . . . 3.1
3.1 ASSEMBLYANDFUELRODDESCRIPTIONS .............. 3.1
3.2 IRRADIATIONANDHANDLINGHISTORY .............. 3.8
4.0 CHARACTERIZATIOPNLANFORATM-lO4 ................ 4.1
4.1 STANDARDEXAMINATIONS ................... 4.1
4.2 DETAILEDEXAMINATIONS ................... 4.2
4.3 SELECTIONOFRODSFORDETAILEbEXAMINATION ......... 4.7
4.4 RODSECTIONING ....................... 4.8
4.4.1 GammaScans ..................... 4.8
4.4.2 Rod Sectioning and Sample Selection ......... 4.11
5.0 NUCLIDEINVENTORYANDRADIOACTIVITYCALCULATIONS ........ 5.1
5.1 INPUTDATAFORORIGEN2CALCULATIONS ............ 5.1
5.2 EVALUATIONOFORIGEN2LIBRARIESFORMODERATEANDHIGH
BURNUPS ......................... 5.3
6.0 CLADDINGCHARACTERIZATION.................. 6.1
6.1 RADIOCHEMICAALNALYSIS .................. 6.2
6.1.1 Cesium on the Cladding Exterior Surface ...... 6.3
6.1.2 Carbon-14 In the Cladding ............. 6.5
6.1.3 Cladding Hydrogen Content ............. 6.8
V
6.2 METALLOGRAPHIECXAMINATIONS ................ 6.9
6.2.1 Cladding Oxide Examinations ............. 6.11
6.2.2 Cladding Hydrid Examinations ............ 6.21
7.0 FUELRADIONUCLIDEINVENTORY................... 7.1
7.1 FUELBURNUPMEASUREMENTS.................. 7.2
7.1.1 Burnup Results and Correlation with GammaScan . . . 7.2
7.1.2 Rod-Average Burnups ................. 7.7
7.2 FUELRADIOCHEMICAALNALYSESANDCOMPARISONWSITHORIGEN2
PREDICTIONS ........................ 7.9
7.2.1 Results of Fuel Radiochemistry ........... 7.9
q
7.2.2 Comparison with Other ATMS ............. 7.10
7.3 RADIALDISTRIBUTIONOF FISSION PRODUCTASNDACTINIDES . . . 7.15
7.3.1 Autoradiography .................... 7.16
7.3.2 Electron Probe Microanalyses ............ 7.21
8.0 REDISTRIBUTIONOF FISSION OF FISSIONPRODUCTS.......... 8.1
J
8.1 GASESRELEASEDFROMTHEFUEL ................ 8.2
8.1.1 Elemental and Isotopic GasAnalyses ......... 8.2
8.1.2 Fission Gas Release ................. 8.8
8.2 CERAMOGRAPHEICXAMINATIONS................. 8.10
8.2.1 Polished Fuel Condition ............... 8.10
8.2.2 Etched Fuel Condition ................ 8.22
8.3 CESIUMANDIODINE PLATEOUTONINNERCLADDINGSURFACES . . . 8.30
8.3.1 Results of Cesium and lodine Measurements ...... 8.31
8.3.2 Comparison of Cesium and lodine Deposits with Other
Fuel Features .................... 8.32
vi
8,4 ANALYTICALELECTRONMICROSCOPEYXAMINATIONS .... 8.38
8.4.1 Experimental Details of AEM ....... 8.39
8.4.2 Results of AEM ............. 8.40
9.0 REFERENCES ..................... 9.1
APPENDIXA - POWERIIISTORYFORASSEMBLYD047 ....... A.I
APPENDIXB - GAMMASCANNINGFORATM-lO4 .......... B.I
APPENDIXC - SECTIONINGDIAGRAM.............. C.I
APPENDIXD - RESULTSOFORIGEN2RADIONUCLIDEINVENTORYCALCULATIONS . D.I
APPENDIXE - DETAILSOFCERAMOGRAPHY/METALLOGRA.P...H..Y... E.I
APPENDIXF - DETAILSOF ELECTRONMICROPROBAENALYSES ........ F.I
APPENDIXG - FISSION GASSAMPLII_G.................. G.I
vii
FIGURES
3.1 Combustion Engineering 14 x 14 Fuel Assembly Schematic .... 3.3
3.2 ATM-lO4 Pellet and Fuel Rod Dimensions ............ 3.4
3.3 Locations of 12B ATM-lO4 Rods in Assembly D047 ........ 3.7
3.4 Core MapShowing the Location of Assembly D047 ........ 3.9
3.5 Calvert Cliffs No. i Operating History . ........... 3.10
3.6 Power History for Rod MKPI04from Assembly D047 ........ 3.11
4.1 General Characterization of Spent Fuel ATMs ........... 4.3
4.2 GammaScan for 137Cs- RodMKPI09 ................ 4.10
4.3 Locations and Types of Metallographic/Ceramographic Samples
from RodMKPI09 to ATM-lO4 ................... 4.12
4.4 Locations and Types of Radiochemical Samples from Rod MKPI09
of ATM-104 ........................... 4.13
5.1 Isotope Concentrations Predicted by ORIGEN2Cross-Section
Libraries Compared with Values Measured in Sample I04-MKPIOg-P
with a Burnup of 44.34 MWd/kgM ................. 5.5
5.2 Isotope Concentrations Predicted by ORIGENCross-Section
Libraries Comparedwith Values Measured in Sample I04-MKPIOg-LL
with a Burnup off 27.35 MWd/kgM ................. 5.6
6.1 Schematic of Cladding Examinations ................ 6.2
6.2 Comparison of 14CContent in Zircaloy-4 Cladding from ATM-lO3,
ATM-lO4, and ATM-lO6 ...................... 6.7
6.3 Axial Variation of Hydrogen in Cladding from RodMKPI09 . .... 6.10
6.4 Cladding Exterior and Interior Surfaces of Polished Sample
I04-MKPIO9-JJ from a Region at Approximately 72%of the
Peak Power ........................... 6.13
6.5 Cladding Exterior and Interior Surfaces of Polished Sample
I04-MKPIO9-N from the Peak-Power Region ............. 6.14
6.6 Variation of Exterior Oxide Thickness Along ATM-lO1, ATM-lO3,
ATM-lO4, and ATM-lO6 Rods .................... 6.17
6.7 Estimated MaximumOxide Thickness in ATMs-I03, 104, and 106 . . . 6.17
• viii
6.8 Comparison of Hydrogen in the Cladding to Exterior Cladding
Oxide Thickness in Rod I04-MKPI09 ................ 6.19
6.9 Comparison of Hydriding in Etched Cladding from Rod I04-MKPI09 . 6,22
7.1 Correlation between 137CsGammaActivity and 14BNdBurnup
Analyses ............................ 7.6
7.2 Fractional 137Cs Activity as a Function of Decay Period ..... 7.8
7.3 Ratios of Measured-to-Predicted Values for Nuclides in ATM-lO4 . 7.13
7.4 Comparison of lac in the fuel from ATM-IOI, ATM-lO3, ATM-lO4,
ATM-lO5 and ATM-lO6 .............. ......... 7.14
7.5 Trends in 1291in the Fuel Versus Burnup in Rod MLA098of
ATM-lO3 and MKPI09 of ATM-lO4 .................. 7.15
7.6 Alpha Autoradiograph of Longitudinal Sample I04-MKPIOg-N from
Peak-Power Region ........................ 7.18
7.7 Beta/GammaAutoradiograph of Longitudinal Sample I04-MKPIO9-N
from Peak-Power Region ..................... 7.19
7.8 Alpha Autoradiograph of Transverse Sample I04-MKPI09-O ..... 7.20
7.9 Beta/GammaAutoradiograph of Transverse Sample I04-MKPI09-O . . . 7.20
7.10 Plutonium Concentration Across Radius of Sample I04-MKPIOg-H . . 7.24
7.11 NeodymiumConcentration Across Radius of Sample I04-MKPIOg-H . . 7.24
7.12 Cesium Concentration Across Radius of Sample I04-MKPIO9-H .... 7.25
7.13 Xenon Concentration Across Radius of Sample I04-MKPIO9-H . . . 7.2_
7.14 Xenon Concentration Across Radius of Sample I03-'4KA-O98-H
with 33 MWd/kgMBurnup .................... 7.26
7.15 Radial Burnup Profile in Sample I04-MKPIO9-H with a Pellet-
Average of 44.3 MWd/kgM .................... 7.29
8.1 Photomacrograph of Polished Transverse Sample I04-MKPI09-O
from the Peak-Power Region .................. 8.12
8.2 Photomacrograph of Polished Longitudinal Sample I04-MKPIOg-N
from the Peak-Power Region .................. 8.13
8.3 Photomacrograph of Polished Transverse Sample I04-MKPIO_J-KK
from a Region at Approximately 68,%of Peak Power ....... 8.14
ix
8.4 Photomacrographof PolishedLongitudinalSample I04-MKPIO9-JJ
from a Regionat Approximately72% of PeakPower ........ 8.15
8.5 Photomicrographsof PolishedTransverseSampleI04-MKPIO9-KK
from a Regionat Approximately68% of Peak Power ......... 8.18
8.6 Photomicrographsof PolishedLongitudinalSample I04-MKP109JJ
from a Regionat Approximately72% of Peak Power ........ 8.19
8.7 Photomicrographsof PolishedTransverseSample I04-MKPIOg-O
from the Peak-PowerRegion ................... 8.20
8.8 Photomicrographsof PolishedLongitudinalSample I04-MKPIOg-N
from the Peak-PowerRegion ................... 8.21
8.9 Photomicrographsof Argon Ion-EtchedTransverseSample
I04-MKPIOg-KKfrom a Region at Approximately68% of Peak Power . 8.23
8.]0 Photomicrographsof Argon Ion-EtchedLongitudinalSample
I04-MKPIOg-]Jfrom a Region at Approximately72% of Peak Powes . 8.24
8.11 Photomicrographsof Argon Ion-EtchedTransverseSample
I04-MKPI09-Ofrom the Peak-PowerRegion ............. 8.25
8.12 Photomicrographsof Argon Ion-EtchedLongitudinalSample
I04-MKPIO9-Nfrom the Peak-PowerRegion ............. 8.26
,,
8.13 Variationin True GrainSize Acrossthe Radiusof Transverse
Fuel Samplesfrom Rod MKPI09 .................. 8.27
8.14 Variationin True Grain SizeAcrossthe Radiusof Longitudinal
Fuel SamplesfromRod MKPI09 ..... . ............ 8.28
8.15 Trend in 137Cs Depositson InteriorCladdingSurfacesof
ATM-lO3,ATM-lO4and ATM-lO6 ................ 8.34
8.16 Trend in 12_IDepositson InteriorCladdingSurfacesof
ATM-lO3,ATM-lO4and ATM-lO6 ................ 8.34
8.17 LocalInventoryof CesiumDepositedon InteriorCladding
Surfacesof ATM-lO3,ATM-lO4,ATM-lO5and ATM-lO6 ...... 8.35
8.18 Local Inventoryof IodineDepositedorlInteriorCladding
Surfacesof ATM-lO3,ATM-lO4,ATM-lO5and ATM-lO6 ...... 8.35
8.19 Local Inventoryof Cesium Depositson InteriorCladdingof
Fuel Rods with DifferentRod-AverageFissionGas Releases . . 8.37
8.20 Local Inventoryof IodineDepositson InteriorCladdingof
Fuel Rodswith DifferentRod-AverageFissionGas Releases . . 8.37
L
X