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AECL-9881

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ATOMIC ENERGY

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ENERGIE ATOMIQUE

OF CANADA LIMITED

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DUCANADA LIMITEE

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Societe de Recherche

DERIVATION OF INITIAL RADIONUCUDE INVENTORIES FOR THE SAFETY ASSESSMENT

OF THE DISPOSAL OF USED CANDU® FUEL

OBTENTION DESINVENTAIRES INITIAUX DE RADIONUCLIDES POUR DEVALUATION DE L'EVACUATION

DU COMBUSTIBLE IRRADIE DEREACTEUR CANDU®QUANT ALASURETE

J. C. Tait, I. C. Gould, G. B. Wilkin

Whit«sh«ll Nucl«ar R«s«arch Establishment

Pinawa, Manitoba

ROE UO

August 1989 aout

Etablisstmant d* recherches nucl«air«s d« Whiteshell

Copyright ® Atomic Energy of Canada Limited, 1989.

ATOMIC ENERGY OF CANADA LIMITED

DERIVATION OF INITIAL RADIONUCLIDE INVENTORIES FOR THE SAFETY ASSESSMENT OF THE DISPOSAL OF USED CANDU®FUEL

by

J.C. Tait, I.C. Gauld and G.B. Uilkin

Vhiteshell Nuclear Research Establishnent Pinava, Manitoba ROE 1L0

1989

AECL-9881

OBTENTION DES INVENTAIRES INITIAUX DE RADIONUCLIDES POUR L'ÉVALUATION DE L'ÉVACUATION DU COMBUSTIBLE IRRADIÉ DE RÉACTEUR CÀNDU© QUANT À LA SÛRETÉ

par

J.C. Tait, I.C. Gauld et G.B. Vilkin

RÉSUMÉ

On s'est servi du programme ORIGEN-S de calcul de la production et diminution de radionuclides pour prédire la masse, la radioactivité et la chaleur de désintégration des radionuclides produits dans le combustible d'UO 2 du réacteur Bruce "A" et sa gaine de zircaloy ainsi que des radionuclides produits par activation neutronique des impuretés de ce combustible et de cette gaine. La compilation a été réalisée pour fournir des résultats d'inventaires initiaux de radionuclides à utiliser pour l'évalua- tion de l'évacuation du combustible irradié de réacteur CANDU quant à la sûreté. En outre, on présente une comparaison des résultats avec ceux obtenus à l'aide du programme de calcul CANIGEN-II.

Énergie atomique du Canada limitée Établissement de recherches nucléaires de Vhiteshell Pinava, Manitoba ROE 1L0

1989

AECL-9881

DERIVATION OF INITIAL RADIONUCLIDE INVENTORIES FOR THE SAFETY ASSESSMENT OF THE DISPOSAL OF USED CANDU® FUEL

J.C.

Tait ,

I.C .

by

Gauld and G.B.

ABSTRACT

Villein

The ORIGEN-S radionuclide generation decay heat of radionuclides produced

radionuclides produced by neutron activation o f impurities in both the U0 2 fuel and the Zircaloy cladding. This compilation has been produced to provide initial radionuclide inventory data for use in the safety assessment of the disposal of used CANDU fuel. The methods used to generate the inventories are described. A comparison of the results vith tho n generated using the CANIGEN-II code is also presented.

and depletion code has been used to predict the mass, activityand in Bruce "A" U0 2 reactor fuel and the Zircaloy cladding and of

Atomic Energy of Canada Limited Vhiteshell Nuclear Research Establishment Pinava, Manitoba ROE1L0

1989

AECL-9881

CONTENTS

 

Page

1. INTRODUCTION

1

2. COMPUTER COuo SELECTION

2

2.1 ORIGEN-S CODE

3

2.2 ORIGEN-S CODE COMPARISONS AND VALIDATION

4

3. CALCULATION OF STABLE ELEMENT AND RADIONUCLIDE INVENTORIES

6

 

3.1 UO 2 FUEL

7

3.2 ZIRCALOT AND IMPURITIES IN UO 2 AND ZIRCALOY

7

3.3 DERIVATION OF INITIAL INVENTORIES

8

4. RADIONUCLIDE INVENTORY TABLES

9

ACKNOWLEDGEMENTS

10

REFERENCES

11

TABLES

14

APPENDIX A

U0 2 FUEL - ACTINIDES AND FISSION PRODUCTS

A.I

APPENDIX B

U0 2 FUEL - IMPURITY ACTIVATION PRODUCTS

B.I

continued

CONTENTS (concluded)

APPENDIX C

ACTIVATION PRODUCTS FOR ZIRCALOY-4 CLADDING AND IMPURITIES IN ZIRCALOY-4

APPENDIX D

PROGRAM INPUT DATA AND OUTPUT VERIFICATION DATA

APPENDIX E

CREATION AND BENCHMARKING OF ORIGEN-S CROSS-SECTION DATA LIBRARIES FOR USE IN BRUCE "A" CANDU FUEL BURNUP CALCULATIONS

APPENDIX F

CALCULATION OF THE ACTINIDE, FISSION PRODUCT, AND NEUTRON ACTIVATION PRODUCT INVENTORIES IN USED BRUCE "A" CANDU FUEL

Page

C.I

D.I

E.I

F.I

LIST OF TABLES

 

Page

TABLE 1

COMPARISON OF PREDICTED INVENTORIES

(g/kg U)

14

TABLE 2

BRUCE "A" FUEL ASSEMBLY AND REACTOR

CORE SPECIFICATIONS

23

TABLE 3

ZIRCALOY IMPURITIES (MAXIMUM PERMITTED LEVEL)

25

TABLE 4

25

TABLE 5

UO 2 FUEL IMPURITIES RADIONUCLIDE INVENTORIES

(MASS) OF IRRADIATED CANDU UO 2 FUEL - ORIGEN-S CODE

26

TABLE 6

RADIONUCLIDE ACTIVITY OF

IRRADIATED CANDU UO 2 FUEL - ORIGEN-S CODE

27

1. INTRODUCTION

Atomic Energy of Canada Limited (ABCL) is assessing the concept of used U0 2 fuel disposal deep in the plutonic rock of the Canadian Precambrian Shield. This concept involves sealing intact used-fuel bundles in corrosion-resistant metal containers and placing them in boreholes in an underground vault (Dormuth, 1987; Hancox, 1988). The only credible scenario for the release of radionuclides to the environment is corrosion of the containers and subsequent dissolution of radionuclides in the groundvater, where they could be transported through the geosphere to the biosphere. The objective of the safety assessment of the disposal concept is to perform a pathways analysis to estimate the dose consequence to man from exposure to any released radionuclides that reach the biosphere from the vault. In addition, the safety

of the storage of used fuel and transportation of used fuel to a waste packaging centre and disposal site is being assessed. These assessments will require information on the quantities of radionuclides present

in a used-fuel bundle. The purpose of this report is to provide a tabulation of initial radionuclide

inventories in the used U0 2 fuel and its Zircaloy sheath, and to outline the conditions and assumptions used in calculating these inventories.

The sources for radiotoxic elements in the disposal of used fuel are the U0 2 fuel, the Zircaloy bundle components, and impurities in both the Zircaloy and 00 2 . The used fuel contains both stable and radioactive isotopes that arise from fission and neutron activation of the U0 2 in the reactor. Additional stable and radioactive isotopes are generated in the Zircaloy and U0 2 fuel as a result of

neutron activation of zirconium and of inherent manufacturing impurities in the Zircaloy sheath and U0 2 . The remainder of the components cf the engineered barriers in the disposal system may contain non- radioactive toxic materials; however, these materials vill not be considered here, but are dealt with in

a separate report (Nehta, in preparation).

2. COMPUTER CODE SELECTION

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The stable and radioactive nuclide inventories at discharge from the reactor in Bruce "A" fuel have previously been calculated using the isotope generation and depletion code CANIGEN (Smith et al., 1987). The mass, activity, decay heat and gamma-source inventories were presented as a function of cooling time for burnups of SOS, 68S, 86S and 1045 GJ/kg initial U 1 for both used-fuel bundles and fuel that had been reprocessed to remove 99.5* (U + Pu) after various discharge times from the reactor.

The ability of the CANIGEN code to accurately predict isotopic concentrations was partially verified by comparison with selected U and Pu isotope analyses of used fuel and by comparison of measured decay heats and radiation fields with values predicted by CANIGEN. The predicted isotopic mass for U and Pu agreed to within - IX of the analytical values and the predictions of decay heat and radiation fields agreed to vithin - 13% and - 152, respectively, of the measured values. The CANIGEN code predictions were also compared with other independent codes such as FISSPROD and ORIGEN. The details of the comparisons and the methodology and error analysis for the calculations using CANIGEN were presented by Smith et al.

(1987).

The original ORIGEN code (Bell, 1973) was developed to characterize the bulk properties of used nuclear fuel. It has since been updated to produce two separate codes - 0RIGEN2 (Croff, 1980a, 1980b, 1982, 1983) and ORIGEN-S (Hermann and Vestfall, 1984; Ryaan, 1984). All three ORIGEN codes use the same basic model, numerical methods, decay data, and photon data. The major difference is that the updated codes use cross-sections and fission product yield data that are significantly improved compared to those of ORIGEN. The 0RIGEN2 code uses burnup-dependent libraries (delivered with the code) developed for

1/ Burnup is defined as GJ/kg of initial uranium, but vill be abbreviated hereafter as GJ/kg U

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specific reactor types and fuel cycles. The majority of these libraries are based on the uranium-fueled pressurized-vater reactors (PWRs) and boiling-water reactors (BVRs) using the once-through fuel cycle. The ORIGEN-S code was developed to provide the user with the capability of producing reactor-specific, burnup-dependent cross-section libraries. This is accomplished through the facilities of the SCALE code system (NUREG, 1982), which includes the COUPLE code (Hermann, 1984). These libraries have received heavy use in applications that require data-library flexibility, including the calculation of the decay heats used in the USNRC Regulatory Guide 3.54 (USNRC, 1984).

The development and support of the CANIGEN code has been discontinued at AECL in favour of the more recent isotope generation/depletion code ORIGEN-S, discussed above. The rationale for this decision is that the ORIGEN-S code is more versatile for the development of new reactor types, is capable of providing additional calculations not available with CANIGEN (e.g., activation of impurities in Zircaloy and U0 2 , and neutron energy spectra) and has a more recent and more extensive radionuclide library database than that available to CANIGEN. The ORIGEN-S code was used at AECL to produce new radionuclide inventories for the reference burnup case (685 GJ/kg U) for used-fuel disposal and also to provide inventories for activation products arising from impurities in the Zircaloy and U0 2 . These inventories vill be used in the safety assessment of the nuclear fuel waste disposal concept.

2.1 ORIGEN-S CODE

In order to produce radionuclide inventory tables, it was necessary to generate a new cross-section library for Bruce CANDU® 2 fuel to be used by ORIGEN-S. The original nuclear data library supplied with ORIGEN-S was modified using the SCALIAS-3.1 (RSIC, 1986) cross-section processing system (a subset of the SCALE system) to transform the library intc one that describes the CANDU heavy-water-moderated PVR.

2/ CANada Deuttrium Uranium. Registered in the U.S. Patent and Trademark Office.

COUPLE was used to update the library using multi-group fluxes and cross-sections determined with an XSDRNPM-S transport calculation. The inventory calculations were then carried out with this new library and ORIGEN-S, run stand-alone in fixed-power mode, to a burn-up of 685 GJ/kg U. A comparison was then made between isotope inventories (one year after exit from the reactor) predicted by the ORIGEN-S, CANIGEN (Smith et al., 1987) and VIMS codes. VIMS is a detailed physics lattice-cell transport and burnup code used within AECL for reactor design and development (Askew et al., 1966; Donnelly, 1986) and uses state-of-the-art ENDF/B-V cross-section data. The details of reactor conditions used, fuel assembly specifications and details of the comparative cases are described in Appendix E.

During this comparative process, several differences were observed between the predicted ORIGEN-S inventories and those predicted by the CANIGEN and VIMS codes. The source of these differences involves the original ORIGEN-S library data for the 236 Pu decay chain (missing production channel from decay of 23 *Np), and 214 Pu decay chain (missing neutron capture data for 243 Fu). The ORIGEN-S database was revised to produce new cross-section library data for the Bruce fuel calculations performed here (see Appendices E and F) .

2.2 ORIGEN-S CODE COMPARISONS AND VALIDATION

The results from the ORIGEN-S (with corrected library), CANIGEN (Smith et al., 1987) and VIMS calculations a, presented in Table 1, for an exit burnup of 685 GJ/kg U and a cooling time of one year, as ratios of ORIGEN/CANIGEN, CANIGEN/VTHS and ORIGEN/VIMS. It should be noted that, in the database used for the CANIGEN case, the concentration of 234 U in the unirradiated fuel was assumed to be zero. For consistency, the initial 234 U concentration was also assumed to be zero in the ORIGEN-S and VIM" comparative runs. (Note thrt in the ORIGEN-S results reported in Appendices A to C, the initial concentration of 234 U was included at its natural abundance of 0.0054Z.) The inventories calculated by ORIGEN-S (Table 1) are in reasonable agreement with the CANIGEN results, with the exception of some cf

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the actinides in the 232 U, 233 U and 234 U decay chains, where differences of factors of four or more are observed. In these instances, however, the significance of these differences is minimized by the

extremely lov

concentrations are bordering on the detection limits of the best analytical techniques and it would be extremely difficult to verify, with any certainty, which code was predicting the sore accurate value. Generally, the code predictions agree to within a factor of two for the U and transuranic isotopes. Concentrations of the fission products generally agree to within a factor of about 1.2, with the exception of 152 Gd and 129 Xe (a stable isotope and a short-lived daughter isotope of 129 I, respectively). ORIGEN-5 tends to predict higher concentrations than CANIGEN, particularly for the actinides, and thus, for the majority of nuclides, it is more conservative to use ORIGEN-S results in the safety assessment calculations. Overall agreement between the limited isotope library of the VIMS code and the CANIGEN and ORIGEN-S codes is very good.

activity of the isotopes involved (usually

less than 10~ 3 Bq/kg U) . Such low

Several studies have been conducted comparing calculated and measured decay heats. Hermann, Parks and Ryman (1986) report that ORIGEN-S overpredicts by about 5X. Heeb (1986) reports that 0RIGEN2 predictions are within 3X of measurements for cooling times of less than ten years when detailed pover histories are used, and that the code overpredicts by as much as 20Z when average power histories are used. A complete survey of available measurements and comparisons to calculations is found in DOE/RW (1987).

The ORIGEN-S, CANIGEN and VIMS codes predict slightly different radionuclide inventories. The differences, however, are mostly due to isotope cross-section differences in their respective database libraries or are due to the different methods employed by each code to calculate the neutron-flux spectrum at different periods throughout the burnup of the fuel, and the methods used to account for the self-shielding effects of the strong resonance absorbing radionuclides as their concentrations increase with burnup. A more comprehensive discussion of the differences between ORIGEN-S and CANIGEN results is presented in Appendix E.

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It should be emphasized that all codes that have been used to predict isotopic concentrations or bulk properties of used fuel have not been developed from the viewpoint of long-term waste management, but rather to describe the neutronics of the reactor and bulk property behaviour for short ti«es after fuel discharge from the reactor. For example, many isotopes that may be of importance from a waste management perspective have little or no importance for modelling reactor neutronics, or for predicting short-term decay heats or radiation fields. As a result, the cross-section data, production/decay-chain data and

half-life data may not have been verified for radionuclides that are unimportant to reactor physics calculations, used-fuel transportation or interim fuel storage facilities. Verification of this library data is important for prediction of isotope concentrations or decay heats for long-term waste management purposes. Codes such as 0RIGEN2 and ORIGEN-S are currently being verified for light-water reactor (LVR) fuel through a quality-assured fuel characterization program in the United States waste management program (Roddy and Mailen, 1987). Only limited analytical data are currently available for CANDU fuels

(Smith et al., 1987) and none are available for fuel cladding.

Over the next several years, the ORIGEN-S

code needs to be validated by performing rigorous chemical and isotopic analyses, and physical property measurements on typical CANDU used-fuel bundles and the results compared with the predicted ORIGEN-S isotopic concentrations and bulk property values. In addition, the cross-section and production/decay- chain data in the code libraries need to be verified. A program has been initiated to verify the databases for the code and validate the predicted inventories by radiochemical analysis.

3. CALCULATION OP STABLE ELEMENT AND RADIONUCLIDE INVENTORIES

The radionuclides that need to b« considered for the safety assessment of fuel disposal can be categorized according to their origins:

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(i)

fission of uranium and heavier fissile elements (to give fission products), and neutron activation of uranium and heavier elements (to give actinides) in the U0 2 fuel; and

(ii)

neutron activation of Zircaloy cladding, fuel bundle structural materials, and impurities in the Zircaloy and U0 2 .

3.1 UP, FUEL

The inventory of stable and radioactive nuclides in used U0 2 fuel will be a function of the burnup and pover history of the fuel, the cooling time out-of-reactor and thfc fuel type. The reference fuel chosen to demonstrate the concept of used-fuel disposal is Bruce "A" U0 2 fuel irradiated to a burnup of 685 GJ/kg U and cooled for ten years after discharge from the reactor (Baumgartner, 1989). The specifications for the fuel elements, fuel assemblies, and reactor operating conditions for the reference burnup are given in Table 2 (see Appendices E and F for details).

3.2 ZIRCALOY AND IMPURITIES IN UP, AND ZIRCALOY

The concentrations of impurities in U0 2 and Zircaloy vere taken from Crosthvaite (unpublished report) and are reproduced in Tables 3 and 4. These concentrations are similar to those chosen by Hehta (1982) for the second interim safety assessment of a used-fuel disposal vault (Wuschke et al., 1985). In both cases, the upper range of the "allowed limits" for impurities was assumed for the calculation of inventories. Although U and Th could have been considered as impurities in the Zircaloy and U0 2 , respectively, they vere not included in the calculation as their inventory was many orders of magnitude lover than that present or generated in the used fuel itself.

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3.3 DERIVATION OF INITIAL INVENTORIES

In calculating the inventories (grams or moles), activities (bequerels) and decay heats (vatts) of radionuclides for both the used U0 2 fuel and activation of impurities in the U0 2 and Zircaloy, a cutoff value of 1 x 10" 20 units/kg U or Zircaloy (units = g, nol, Ci 3 , or V) has been arbitrarily imposed to limit the number of radionuclides reported in the calculations. This limit is many orders of magnitude belov any value that could be reasonably verified by analytical measurements.

In the comparative runs described above, ORIGEN-S did not use burnup-dependent cross-sections, but rather cross-sections determined for fresh-fuel conditions. The effect of this limitation vill be most pronounced in the resonance self-shielding in the strong-resonance absorbing nuclides. Burnup-dependent libraries vere inherently part of the CANIGEN analysis. This deficiency was recognized in the ORIGEN-S calculation method, and as a result, two burnup-dependent libraries vere created for the inventories reported here, to allov for a mid-burnup correction to the cross-section data (See Appendix F) . The first irradiation cycle vas performed to half-burnup using a cross-section library generated from fuel compositions representative of the cycle midpoint, i.e., at 25X burnup. The second irradiation cycle vas continued using a separate library created from the second cycle mid-point compositions. As a result of this more rigorous modification to the ORIGEN-S calculation method, inventories for isotopes, such as

" 3 Pu, 2 "Pu, "°Pu, 2 < 2 -An, " 3 A m and 2 "Am , that differed by as much as 80* from

the CANIGEN results

(Table 1) nov agree to within 30*. In general, most other actinide inventories moved closer to the CANIGEN inventories; however, some moved slightly further avay from the CANIGEN values, but these changes vere generally less than 20*. It is likely that additional cycling of the libraries including three or •ore burnup correction steps vould result in further improvements. (Note that the SAS2 control module in SCALIAS-3.1 (NUREG, 1982) developed for producing burnup-dependent libraries is not currently available

3/ 1 Ci - 37 GBq

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at AECL. Thus, the tvo-cycle libraries used here were created manually.) Addition of further cycling steps, and any other changes that are indicated as being necessary based on comparisons of predicted inventories with analytical results will be implemented during the ORIGEN-S code validation program.

4. RADIONUCLIDE INVENTORY TABLES

The results generated by the ORIGEN-S code (as corrected and enhanced as described above) for used fuel at a burnup of 685 GJ/kg U are presented in Appendix A (See Appendix F for details). The results are presented as actinide and fission product inventories: mass in mol/kg U and g/kg U; activities in Bq/kg U and Ci/kg U; and decay heat in V/kg U.

The results for activation of impurities in UO, are presented similarly in Appendix B and the results for the activation of the Zircaloy and impurities in the Zircaloy are presented in Appendix C. (No decay heat results are presented for the U0 2 or Zircaloy impurities.)

The input parameters to the ORIGEN-S code and the program ouput verification data are presented in Appendix D.

It should be noted again that a particular radionuclide vill not necessarily appear in every appendix table, since each table has a cutoff value of 1 x 10~ 20 . The inclusion of a radionuclide in the tables vill thus be dependent on the units.

A summary of the fission product and selected actinide masses and activities for Bruce fuel vith a burnup of 685 GJ/kg U and cooled for ten years is presented in Tables 5 and 6.

ACKNOWLEDGEMENTS

The author s vis h t o thank D. Chen, L.H. Johnson and K. Mehta for helpfu l suggestions and review of report.

thi s

REFERENCES

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Askew, J.R., F.J. Payers, and P.B. Kemshell. 1966. A General Description of the Lattice Code VIMS. JBNES 4, 564.

Bauogartner, P. 1989. Technical Specifications for a Used Fuel Disposal Centre. Atomic Energy of Canada Limited Technical Record*, TR-A10.

Bell, M.J. 1973. ORIGEN - The ORNL Isotope Generation and Depletion Code. Oak Ridge National Laboratory Report, ORNL-4628.

Croff, A.G. 1980a. A Revised and Updated Version of the Oak Ridge Isotope Generation and Depletion Code. Oak Ridge National Laboratory Report, 0RNL-5621.

Croff, A.G. 1980b. A User's Manual for the 0RIGEN2 Computer Code. Oak Ridge National Laboratory Report, ORNL/TM-7175, 1980.

Croff, A.G. 1982. 0RIGEN2 - Isotope Generation and Depletion Code - Matrix Exponential Method. Oak Ridga National Laboratory Report, ORNL-CCC-371.

Croff, A.G. 1983. ORIGEN2: A Versatile Computer Code for Calculating the Nuclide Compositions and Characteristics of Nuclear Materials. Nucl. Tech. 62, 335.

DOE/Rtf REPORT. 1987. Characteristics of Spent Fuel, High-Level Waste, and Other Radioactive Vastes which May Require Long-Term Isolation. U.S. Department of Energy Report, Office of Civilian Radioactive Vaste Management, DOE/RV-0184, Vol. 2, Appendix 1A.

Donnelly, J.V. 1986. WIMS-CRNL J A Users Manual for the Chalk River Version of VIMS. Atomic Energy of Canada Limited Report, AECL-8955.

Dormuth, R.tf. (ed.) 1987. Canadian Nuclear Fuel Vaste Management Program. Rad. Vaste Manage. Nucl. Fuel Cycle, 8 (2-3).

Bancox, V.T .

.losing the Circle: Returning Used Uranium Fuel to the Geologic Environment.

Presented at the Canadian Nuclear Society Symposium on Uranium and Electricity. Saskatoon, Sask., 1988 Sept. 18-21.

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Heeb, CM . 1986. Comparison of Spent Fuel Decay Heat Rate 0RIGEN2 Predictions and Calorimeter Measurements. Presented at the Third International Spent Fuel Storage Technology Symposium/Workshop, 1986 April 8-10, Seattle, VA.

Hermann, O.V. 1984. COUPLE: SCALE System Module to Process Problem-Dependent Cross Sections and Neutron Spectral Data for ORIGEN-S Analysis. Oak Ridge National Laboratory Report, NUREG/CR-0200, Rev. 2, Vol. 2, Section F6.

Hermann, O.M., R.M. Westfall. 1984. ORIGEN-S: SCALE System Module to Calculate Fuel Depletion, Actinide Transmutation, Fission Product Buildup and Decay, and Associated Radiation Source Terms. Oak Ridge National Laboratory Report, NUREG/CR-0200, Rev. 2, Vol. 2, Section F7.

Hermann, O.V., C.V. Parks, J.C. Flyman. 1986. Spent Fuel Decay Heat Calculations Using ORIGEN-S. Presented at the Third International Spent Fuel Storage Technology Symposium/Workshop, April 8-10, 1986, Seattle, VA.

Mehta, K. 1982. Nuclide Inventory for Nuclear Fuel Waste Management: Post-Closure Phase. Atomic Energy of Canada Limited Report, AECL-6830.

Mehta, K. In preparation. Identification and Treatment of Nuclides and Nuclide-Chains for Post-Closure SYVAC Assessment. Atomic Energy of Canada Limited Report.

NUREG. 1982. SCALE: A Modular Code System for Performing Standardized Computer Analyses for Licensing Evaluation. NUREG/CR-0200, Oak Ridge National Laboratory Report. Volumes I, II, and III. Revised 1983 and 1984.

Roddy, J.W. and J.C. Mailen. 1987. Radiological Characteristics of Light-Water Reactor Spent Fuel: A Literature Survey of Experimental Data. Oak Ridge National Laboratory Report, ORNL/TM-10105.

RSIC. 1986. SCALIAS 3.1: Selected FORTRAN 77 Modules From SCALE 3.1. RSIC Code Package CCC-47S.

Ryman, J.C. 1984. ORIGEN-S Data Libraries. NUREG/CR-0200, Rev. 2, Vol. 3, Section M6.

Smith, B.J., J.C. Tait and R. von Massov. 1987. Radioactive Decay Properties of BRUCE "A" CANDU™ U0 2 Fuel and Fuel Recycle Waste. Atomic Energy of Canada Limited Report, AECL-9072.

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Wuschke, D.M., P.A. Gillespie, K.K. Mehta, V.F. Heinrich, D.M. LeNeveu, V.M. Guvanasen, G.R. Sherman, D.C. Donahue, B.V. Goodwin, T.H. Andres and R.B. Lyon. 1985. Second Interim Assessment of the Canadian Concept for Nuclear Fuel Vaste Disposal. Volume 4: Post-Closure Assessment. Atomic Energy of Canada Limited Report, AECL-8373-A.

USNRC. 1984. Spent Fuel Heat Generation in an Independent Spent Fuel Storage Installation. Regulatory Guide 3.54. U.S. Nuclear Regulatory Commission, Vashington, DC.

* Unrestricted, unpublished report available from SDDO, Atomic Energy of Canada Limited Research Company, Chalk River, Ontario KOJ 1J0.

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TABLE 1 COMPARISON OF PREDICTED INVENTORIES (g/kg U) BRUCE "A" FUEL, BURNUP 685 GJ/kg U, ONE YEAR COOLED

Ratio

Muclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

ORIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Cf

251

2.39e-15

1.92e-15

0.80

Cf

250

1.57e-14

7.70e-15

0.49

Cf

249

4.92e-14

2.60e-14

0.53

Bk

249

3.84C-14

2.04e-14

0.53

Cm

248

2.86e-ll

1.43e-U

0.50

Cm

247

1.31e-09

6.04e-10

0.46

Ca

246

2.22e-07

1.90e-07

0.86

Ca

245

2.29e-06

1.99e-06

0.87

Ca

244

2.34e-04

2.37e-O4

1.01

Ca

243

4.81e-06

4.43e-06

0.92

Ca

242

1.12e-04

1.12e-04

1.00

Aa

243

2.87e-03

3.19e-O3

3.67e-03

1.11

0.87

0.78

Aa

242a

1.73e-05

3.19e-05

1.42e-05

1.84

2.25

1.22

Aa

242

2.08e-10

3.82e-10

1.84

Aa

241

l.lle-02

1.64e-02

1.27e-02

1.48

1.29

0.87

Pu 244

1.35e-06

l.Ole-06

0.75

Pu 243

4.75e-20

2.15e-20

0.45

Pu 242

6.65e-02

8.18e-02

7.44e-02

1.23

1.10

0.89

Pu 241

1.99e-01

2.93c-01

2.25e-01

1.47

1.30

0.88

Pu 240

l.Ue+00

9.02e-01

1.06e+00

0.79

0.85

1.08

Pu 239

2.7Oe+OO

2.56*1-00

2.6U+OO

0.95

0.98

1.03

Pu 238

4.53e-03

4.68e-03

4.24e-03

1.03

1.10

1.07

Pu 236

1.45e-07

2.3U-08

1.39«-08

0.16

1.66

10.41

continued

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TABLE 1

(continued)

Ratio

Nuclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

ORIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Np 240m

2.28e-19

1.69e-19

0.74

Np

239

2.47e-09

2.74e-09

1.11

Np

237

3.09e-02

3.45e-02

2.84e-02

1.12

1.21

1.09

U

240

2.57e-17

1.93e-17

0.75

U

238

9.85e+02

9.85e+02

9.85e+02

1.00

1.00

1.00

U

237

5.68e-09

9.08e-09

1.60

U

236

7.64e-01

7.65e-01

7.58e-01

1.00

1.01

1.01

0 235

2.07e+0O

2.00e+00

2.12e+OO

0.97

0.94

0.98

U

234

3.99e-05

7.54e-05

3.62e-05

1.89

2.08

1.10

U

233

1.62e-08

3.2Oe-O8

1.98

U

232

4.63e-08

7.93e-09

0.17

Pa 234a

4.82e-13

4.82e-13

1.00

Pa233

1.05e-09

1.17e-09

1.11

Pa 231

3.96e-09

3.81e-09

0.96

Th234

1.43e-08

1.43e-08

1.00

Th 232

3.04e-08

3.06e-08

1.01

Th 231

8.43e-12

8.15e-12

0.97

Th230

6.53«-ll

1.97e-10

3.02

Th229

4.88e-14

2.89e-13

5.92

Th 228

2.36e-10

4.27e-ll

0.18

Th 227

1.63e-16

1.72e-16

1.06

Ac228

1.09e-22

1.19e-22

1.09

Ac 227

7.49e-14

7.40e-14

0.99

Ac 225

1.55e-19

1.06e-18

6.84

Ra 228

8.94e-19

9.79e-19

1.10

Ra226

2.28c-16

1.03e-15

4.52

Ra 225

2.44e-19

1.57e-18

6.43

continued

- 16 -

TABLE 1 (continued)

Ratio

Huclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

ORIGEN-S/

CANIGSN/

 

CANIGEN

VIMS

VIMS

Ra 224

1.18e-12

2.2Oe-13

0.19

Ra 223

9.28e-17

1.05e-16

1.13

Rn 222

1.41e-21

6.63e-21

4.70

Rn 220

2.05e-16

3.79e-17

0.18

Rn 219

3.65e-22

4.12e-22

1.13

Pr 221

5.08e-23

3.47e-22

6.83

Po 218

7.67e-25

3.60e-24

4.69

Po 216

5.43e-19

1.00e-19

0.18

Po 215

1.61e-25

1.82e-25

1.13

Po 214

6.74e-31

3.18e-30

4.72

Po 212

6.80e-25

1.26e-25

0.19

Po 213

6.64e-31

4.77e-30

7.18

Po 210

1.26e-22

1.17e-21

9.29

At 217

5.54e-27

3.82e-26

6.90

Bi 214

4.89e-24

2.31e-23

4.72

Bi 213

4.69e-22

3.18e-21

6.78

Bi 212

1.29e-14

2.39e-15

0.19

Bi 211

1.14e-20

1.28e-20

1.12

Bi 210

1.48e-23

l.O8e-22

7.30

Bi 209

1.43e-18

7.97e-17

55.73

Pb 214

6.62e-24

3.1U-23

4.70

Pb 212

1.36e-13

2.52e-14

0.19

Pb 211

1.93e-19

2.17e-19

1.12

Pb 210

2.57e-20

1.75e-19

6.81

continued

-

17

-

TABLE 1

(continued)

Ratio

Nuclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

ORIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Pb209

1.98e-21

1.33e-20

6.72

Pb208

3.19e-ll

6.32e-12

0.20

Pb207

9.61e-16

1.19e-15

1.24

Pb206

4.50e-23

6.24e-22

13.87

Tl209

4.84e-25

3.25e-24

6.71

Tl208

2.29e-16

4.27e-17

0.19

Tl207

2.50e-20

2.8Oe-2O

1.12

H

3

1.74e-05

1.37e-05

0.79

As

75

2.75e-05

3.00e-05

1.09

Ge

76

7.57e-05

3.30e-05

1.10

Se

77

1.78e-04

1.96e-04

1.10

Se

78

4.73e-04

5.07e-04

1.07

Se 79

1.17e-03

1.30e-03

1.11

Se 80

2.98e-03

3.21e-03

1.08

Se 82

7.24e-03

7.86e-03

1.09

Br

79

1.62e-08

2.19e-08

1.35

Br

81

4.90e-03

5.33e-03

1.09

Rr

83

9.12«-03

9.92t-03

9.8Oe-O3

1.09

1.01

0.93

Rr 84

2.2Oe-O2

2.43c-02

1.10

Rr 85

5.05C-03

5.60e-03

1.11

Rr 86

3.76e-02

4.19t-02

1.11

Rb 85

2.06«-02

2.29«-O2

1.11

Rb 87

4.91e-02

5.48C-02

1.12

continued

-

18

-

TABLE 1

(continued)

Ratio

Nuclide

CANIGEN*

0RIGEN-S

VIMS

ORIGEN-S/

RIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Sr 88

7.

lle-02

7.92e-02

1.11

Sr 89

2.

17e-04

1.88e-O4

0.87

Sr 90

1.

13e-01

1.26e-01

1.12

Y

89 9.

39e-02

1.05e-01

1.12

Y

90 2.

84e-05

3.16e-05

1.11

Y

91 5.

56e-04

5.71e-04

1.03

Zr 90

3.

63e-03

4.Ue-03

1.14

Zr 91

1.

23e-01

1.37e-01

1.11

Zr 92

1.

34e-01

1.47e-01

1.10

Zr 93

1.

54e-01

1.68e-01

1.09

Zr 94

1

64e-01

1.79e-01

1.09

Zr 95

1.

27e-03

1.29e-03

1.02

Zr 96

1

76e-01

1.89e-01

1.07

Nb 93

7

54e-09

1.18e-O8

1.56

Nb 93a

8

52e-08

9.57e-08

1.12

Nb 95

1

.50e-03

1.60e-03

1.07

No 95

1

.70e-01

1.84e-01

1 .83e-01

1.08

1.01

0.93

No 96

1

.13e-03

1.31e-03

1.16

No

97

1

.81e-01

1.93e-01

1.07

No

98

1

.85e-01

1.96e-01

1 .95e-01

1.06

1.01

0.95

No

100

2

•15e-01

2.26e-01

1.05

Tc

99

1

.92e-01

2.05e-01

2 .03e-01

1.07

1.01

0.94

Ru

100

6

.08e-03

6.89c-03

1.13

Ru

101

1

.81c-01

1.89e-01

1 .89e-01

1.04

1.00

0.96

Ru

102

1

.74e-01

1.80«-01

1.03

continued

- 19 -

TABLE 1 (continued)

Ratio

Nuclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/ ORIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Ru 103

8.09e-05

7.53e-05

7.33e-05

0.93

1.03

1.10

Ru 104

1.35e-01

1.33e-01

0.99

Ru 106

3.51e-02

3.30e-02

0.94

Rh

103

1.54e-01

1.55e-01

1.53e-01

1.01

1.02

1.01

Rh

106

3.3Oe-08

3.10e-08

0.94

Pd

105

8.39e-02

9.08e-02

9.01e-02

1.08

1.01

0.93

Fd

106

7.62e-02

6.42e-02

0.84

Pd

107

5.96e-02

5.48e-02

0.92

Pd

108

4.02e-02

3.72e-02

3.78e-02

0.93

0.98

1.06

Pd

110

1.16e-02

1.06e-02

0.91

Ag

107

7.95e-09

7.27e-09

0.91

Ag

109

2.27e-02

2.16e-02

2.87e-02

0.95

0.75

0.79

Ag

110B

3.26e-05

3.04e-05

0.93

Cd

110

3.33e-03

2.54e-03

0.76

Cd

111

5.33e-03

4.87e-03

0.91

Cd

112

2.37e-03

2.19e-03

0.92

Cd

113B

2.77e-05

3.12e-05

1.13

Cd

113

3.23e-05

3.39e-05

2.77e-O5

1.05

1.23

1.17

Cd

114

2.81e-03

2.66e-03

0.95

Cd

116

8.75e-04

8.68e-04

0.99

In

115

6.55e-04

6.6Oe-OA

6.78e-04

1.01

0.97

0.97

Sn

117

8.77e-04

8.75e-04

1.00

Sn 118

9.02e-04

9.07e-04

1.01

Sn 119a

4.40e-06

3.69e-06

0.84

Sn 119

9.05e-04

9.04e-04

1.00

Sn 120

9.26e-04

9.32e-04

1.01

continued

- TABLE 1 (continued)

20

-

Ratio

Hudide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

RIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Sn 121B

9.35e-07

7.26e-07

0.78

Sn122

1.04e-03

1.04e-03

1.00

Sn123

5.16e-05

2.50e-05

0.48

Sn124

1.55e-03

1.57e-03

1.01

Sn126

4.87e-03

4.98e-03

1.02

Sb 121

9.67e-04

9.83e-04

1.02

Sb123

1.13e-03

1.19e-03

1.05

Sb124

6.38e-08

8.92e-08

1.40

Sb125

2.17e-03

2.23e-03

1.03

Sb126

2.31e-10

2.37e-10

1.03

Te125B

3.06e-05

3.10e-05

1.01

Te125

7.89e-04

7.87e-04

1.00

Te 126

1.56e-04

1.41e-04

0.90

Te 127a

1.06e-04

1.00e-04

0.94

Te128

2.43e-02

2.50e-02

1.03

Te129B

1.35e-06

8.52e-O7

0.63

Te

130

8.23e-02

8.50e-02

1.03

I

127

1.18e-02

1.23c-02

1.18e-02

1.04

1.04

1.00

I

129

4.35e-02

4.49e-02

1.03

I

131

1.72e-16

1.70e-16

1.92e-16

0.99

0.89

0.90

Xc

129

2.35e-09

3.12t-O7

132.77

Xc*131

1.24e-01

1.31e-01

1.06

Xt

132

2.20e-01

2.3Ot-Ol

1.05

Xt134

3.28t-01

3.51t-01

1.07

Xc136

5.75e-01

6.02t-01

1.05

Cs

133

2.81e-01

3.02«-01

2.9SC-01

1.07

1.02

0.95

C«134

9.23c-03

8.06t-03

7.88t-03

0.87

1.02

1.17

continutd

- 21 -

TABLE 1 (continued)

Ratio

Nuclide

CANIGEN*

ORIGEN-S

VIMS

ORIGEN-S/

ORIGEN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Cs 135

2.01e-02

2.37e-02

2.25e-02

1.18

1.05

0.89

Cs 137

2.80e-01

2.94e-01

1.05

Ba 134

4.57e-O3

4.00e-03

0.88

Ba 135

1.08e-06

1.56e-06

1.44

Ba 137a

4.26e-08

4.48e-08

1.05

Ba 137

8.50e-03

9.05e-03

1.06

Ba 138

2.81e-01

3.00e-01

1.07

La 139

2.73e-01

2.90e-01

2.86e-01

1.06

1.01

0.95

Ce 140

2.73e-01

3.05e-01

1.12

Ce 141

2.26e-05

2.26e-05

1.00

Ce 142

2.53e-01

2.71e-01

1.07

Ce 144

6.94e-02

7.3le-02

7.23e-02

1.05

1.01

0.96

Pr 141

2.52e-01

2.69e-01

1.07

Pr 143

1.67e-10

1.75e-10

1.05

Pr 144

2.93e-06

3.09e-06

1.05

Pr 144a

1.46e-08

1.54e-08

1.05

Nd 142

1.80e-03

2.18e-03

1.21

Nd 143

1.89e-01

2.05e-01

1.89e-01

1.08

1.08

1.00

Nd 144

2.05e-01

2.22e-01

2.28e-01

1.08

0.97

0.90

Nd 145

1.58e-01

1.70e-01

1.67e-01

1.08

1.02

0.95

Nd 146

1.43e-01

1.51.-01

1.49e-01

1.06

1.01

0.96

Nd 147

7.6Oe-13

8.65e-13

7.12e-13

1.14

1.21

1.07

Nd 148

8.37e-02

8.7U-02

9.15e-02

1.04

0.95

0.91

Nd 150

4.17e-02

4.24«-02

4.24e-02

1.02

1.00

0.98

continued

- 22 -

TABLE 1 (concluded)

Ratio

Ruclide

CANIGEN*

ORIGEN-S

W1MS

ORIGEN-S/

ORIGBN-S/

CANIGEN/

 

CANIGEN

VIMS

VIMS

Pa 147

6.06e-02

6.38e-02

6.04e-02

1.05

1.06

1.00

Pa 148

7.62e-09

4.64e-09

6.45e-09

0.61

0.72

1.18

Pa 148a

8.50e-07

6.34e-07

7.02e-07

0.75

0.90

1.21

Sa 147

2.37e-02

2.54e-02

2.41e-02

1.07

1.06

0.98

Sa 148

1.06e-02

9.95*-03

9.61e-03

0.94

1.04

1.10

Sa 149

1.69e-03

1.76e-03

1.60e-03

1.04

1.10

1.06

Sa 150

6.23e-02

6.82e-02

6.39e-02

1.09

1.07

0.98

Sa 151

2.67e-03

2.51e-03

2.74e-03

0.94

0.92

0.97

Sa 152

4.16e-02

4.43e-02

4.40e-02

1.06

1.01

0.95

S B 154

1.03G-02

8.76e-03

0.85

Eu 151

2.1Oe-05

2.02e-05

2.20e-05

0.96

0.92

0.95

Eu 152

1.03e-06

1.82e-06

1.77

Eu 153

1.92e-02

2,O2e-O2

2.10e-02

1.05

0.96

0.91

Eu 154

3.7Oe-03

3.73e-03

3.06e-03

1.01

1.22

1.21

Eu 155

1.7Oe-03

1.58e-03

1.19e-03

0.93

1.32

1.42

Eu 156

7.99e-ll

8.69e-ll

6.44e-ll

1.09

1.35

1.24

Gd 152

2.15e-08

2.09e-06

97.21

Gd 154

3.92e-04

3.78e-04

0.96

Gd 155

2.66e-04

2.39e-04

3.64e-04

0.90

0.66

0.73

Gd 156

8.14«-03

9.02e-03

6.60e-03

1.11

1.37

1.23

Gd 157

5.5O«-05

2.16t-05

1.27e-05

0.39

1.71

4.34

Gd 158

5.84C-03

3.12t-03

0.53

Gd 160

2.78C-04

2.43e-04

0.87

Tb 159

5.87t-04

5.36e-04

0.91

(Saith «t al., 1987)

- 23 -

TABLE 2

BRUCE "A" FUEL ASSEMBLY AND REACTOR CORE SPECIFICATIONS

Fuel Element

Fuel (natural UO 2 ) composition

radius area (cross section) density temperature (average)

0.0054

vt.Z 234 U

0.7110

vt.Z 235 U

99.2836

vt.Z 23 «U

0.6077

cm

1.1602

cm 2

10.3590

g/cm 3

1155 K

Cladding (Zircaloy-4) outside radius thickness air-gap radius (outside) air-gap thickness temperature

Cladding (Zircaloy-4) outside radius thickness air-gap radius (outside) air-gap thickness temperature
Cladding (Zircaloy-4) outside radius thickness air-gap radius (outside) air-gap thickness temperature
Cladding (Zircaloy-4) outside radius thickness air-gap radius (outside) air-gap thickness temperature
Cladding (Zircaloy-4) outside radius thickness air-gap radius (outside) air-gap thickness temperature

0.6538

0.0419

0.6119

0.0042

cm

cm

cm

cm

546 R

546 R

Fuel Assembly

Number of elements

37 (one central)

radii (to element centre) inner ring (31-36) intermediate ring (19-30) outer ring (1-18)

radii (to element centre) inner ring (31-36) intermediate ring (19-30) outer ring (1-18)
radii (to element centre) inner ring (31-36) intermediate ring (19-30) outer ring (1-18)

1.4885

2.8755

4.3305

cm

cm

cm

continued

-

24

-

TABLE 2

(concluded)

Reactor Core

Coolant

and aoderator (D 2 0)

aoderator teaperature

359

R

coolant teaperature

549

R

Pressure tube (Zircaloy-4) inside radius

5.169

ca

thickness

0.406

ca

teaperature

549

R

Insulating gap (C0 2 ) inside radius thickness teaperature

Calandria (Zircaloy-4) inside radius thickness temperature

5.575ca

0.873ca

359 R

6.448ca

0.140 ca

359 R

-

25

-

TABLE 3 ZIRCALOY* IMPURITIES (MAXIMUM PERMITTED LEVEL)

TABLE 4

UP, FUEL IMPURITIES

Element

Sn

Al

B

Cd

C

Co

Cu

Hf

H

J

Pb

Mg

°2

(Zr)

Mg/g Zr"

17 000.0

75.0

0.5

0.5

270.0

20.0

50.0

100.0

25.0

130.0

20.0

1 500.0

977 735.0

Element

pg/g Zr**

Element

ug/g u

Element

vg/g u

Fe

2 400.0

Mn

50.0

Al

50.0

Fe

100.0

Mo

50.0

B

0.3

Hg

50.0

Ni

70.0

Cd

0.2

Mn

10.0

Nb

100.0

Ca

50.0

Mo

4.0

N 2

80.0

C

100.0

Ni

30.0

Si

120.0

Cr

25.0

Si

60.0

Ta

200.0

Cu

20.0

Ag