REVIEW OF RESULTS FOR THE OECD/NEA PHASE VII BENCHMARK: STUDY OF SPENT FUEL COMPOSITIONS FOR LONG-TERM DISPOSAL

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REVIEW OF RESULTS FOR THE OECD/NEA PHASE VII BENCHMARK: STUDY OF SPENT FUEL COMPOSITIONS FOR LONG-TERM DISPOSAL Georgeta Radulescu John Wagner (presenter) Oak Ridge National Laboratory International Workshop on Advances in Applications of Burnup Credit for Spent Fuel Storage, Transport, Reprocessing, and Disposition Organized by: Nuclear Safety Council of Spain (CSN) and the International Atomic Energy Agency (IAEA) October 27 30, 2009, Cordoba, Spain

Outline Overview of the benchmark specification Participating organizations, computer codes, and nuclear data Results Decay calculations for selected isotopes Criticality calculations Sensitivity calculations Summary Remarks / Observations 2

Overview of the benchmark specification (1/2) Purpose Study the ability of relevant computer codes and associated nuclear data to predict spent fuel isotopic compositions and corresponding k eff values in a cask configuration over the time duration relevant to SNF disposal Objective Improve understanding and confidence in our ability to predict k eff and source terms for timeframes relevant to long-term disposal of SNF 3

Overview of the benchmark specification (1/2) Specification (issued Nov 2008) http://www.nea.fr/html/science/wpncs/buc/specifications/phase-vii/phase-vii_benchmarkspecification_rev01.pdf PWR UO 2 discharge fuel compositions for decay calculations 4.5-wt% 235 U initial enrichment and 50 GWd/MTU burnup Isotopes relevant to burnup credit and public dose as well as their precursors (113 total isotopes) Representative cask model for k eff calculations Borrowed from previous benchmark specifications Requested results Predicted isotopic concentrations for 30 time steps (0 1 M yrs) Predicted k eff values for each time step Actinide-only (11 total isotopes) fuel compositions Actinide and fission product (30 total isotopes) fuel compositions 4

Excerpts from benchmark specification 5

Excerpts from benchmark specification 6

Excerpts from benchmark specification 7

Participating Organizations and Computer Codes/Data Used Country Organization Decay Code Decay Data Library Criticality Code Cross-section Data Library Slovakia VUJE a SCALE 5.1/ ORIGEN-S USA ORNL b SCALE 6/ ORIGEN-S (CCC-750) ENDF/B-VI and V SCALE 5.1/ KENO VI ENDF/B-VI and V SCALE 6/ KENO V.a ENDF/B-V, 44 energy groups (EGs) ENDF/B-VII.0, continuous energy (CE) Japan JAEA c ORIGEN2.2UPJ (NEA-1642) ORLIB33 d MCNP-4C2 JENDL3.3, CE Sweden E Mennerdahl Systems SCALE6/ ORIGEN-S ENDF/B-VI and V SCALE 6/ KENO V.a ENDF/B-VII.0, CE Spain DENIM/CSN/ SEA Ingenieria e ACAB V2008 (NEA-1839) JEFF-3.1 MCNPX-2.5 JEFF-3.1.1, CE MCNPX-2.4.0 ENDF/B-VI, CE ACAB V2008 From ORIGEN-S MCNPX-2.5 JEFF-3.1.1, CE France AREVA-TN DARWIN 2.1 JEF-2.2 CRISTAL V1.0 JEF-2.2, 172 EGs a Nuclear Power Plant Research Institute Trnava Inc, VUJE b Oak Ridge National Laboratory c Japan Atomic Energy Agency d JNDC FP nuclear data library and JENDL3.3 e Additional criticality calculations and analyses were provided by these organizations to be included as an Annex to the final report. 8

Participating Organizations and Computer Codes/Data Used Country Organization Decay Code Decay Data Library Criticality Code Cross-section Data Library France IRSN a DARWIN 2.0 JEF-2 MORET 5 b JEFF-3.1, CE PHOENIX 1.0.0a b DECAY.LIB ( ORGEN2.2 ) N/A N/A Germany GRS c ORIGEN-X- 2008 ENDF/B-VI SCALE 6/ KENO V.a ENDF/B-VII.0, 238 EGs Czech Republic Nuclear Research Institute at Rez SCALE 6/ ORIGEN-S ENDF/B-VI and V SCALE 6/ KENO V.a ENDF/B-VII.0, 238 EGs SCALE 6/ KENO V.a ENDF/B-VII.0, CE Finland VTT d SCALE 6/ ORIGEN-S ENDF/B-VI and V MCNP5, version 1.40 ENDF/B-VI, CE Hungary KFKI e SCALE 6/ ORIGEN-S ENDF/B-VI and V MCNP5 ENDF/B-VI.2 and V, CE TIBSO (NEA-1592) JEF-2.2 MCNP5 ENDF/B-VI.2 and V, CE a Institut de Radioprotection et de Sûreté Nucléaire b Under development c Gesellschaft für Anlagen-und Reaktorsicherheit mbh d VTT Technical Research Centre of Finland e KFKI Atomic Energy Research Institute 9

Summary: Participation 11 countries, 13 organizations, 14 decay calculations, 15 criticality calculations ORIGEN, ORIGEN-based, DARWIN, PHOENIX decay calculation codes Numerical and analytical methods for solving decay chain equations Matrix exponential method (ORIGEN, PHOENIX) Analytical method and 4th order Runge Kutta numerical method (DARWIN, PHOENIX) Decay data libraries ENDF/B-V, VI JENDL3.3 JEFF-3.1 JEF-2.2 SCALE, MCNP, MORET Monte Carlo criticality codes Neutron cross-section data libraries ENDF/B-V, 44 energy groups ENDF/B-VI continuous energy ENDF/B-VII.0 continuous energy ENDF/B-VII.0 238 energy groups JEF-2.2, 172 energy groups JENDL3.3 continuous energy JEFF-3.1 continuous energy JEFF-3.1.1 continuous energy 10

ISOTOPIC RESULTS 11

Time-dependent Actinide Concentrations 13

Comparison of Decay Calculation Results for U-233 Note: ORIGEN-X-2008 results were obtained using 3 different runs and were affected by the choice of one big time step for the beginning of the second (150 years) and third (20,000 years) runs. 14

Comparison of Decay Calculation Results for U-235 15

Comparison of Decay Calculation Results for Pu-241 241 Pu (14.4y) 241 Am (432.7y) 241 Pu result variability for the first 200 years after fuel discharge indicates differences in 241 Pu half-life values. 16

Time-dependent FP Concentrations 17

Comparison of Decay Calculation Results for Sm-151 Note: Different trends between the results obtained with JEF and JENDL decay libraries (DARWIN, TIBSO, and ORIGEN2.2UPJ) and the other results. 18

Comparison of Decay Calculation Results for Eu-151 Note: Different trends between the results obtained with JEF and JENDL decay libraries (DARWIN, TIBSO, and ORIGEN2.2UPJ) and the other results. 151 Sm (90y) 151 Eu. 19

Comparison of Decay Calculation Results for Gd-155 Note: DARWIN, TIBSO, and PHONIX 1.0.0a beta results are lower than the results of the other calculations for short decay times. 155 Eu (4.75 y) 155 Gd. 20

CRITICALITY RESULTS 21

k eff Values difference from mean 0,008 0,006 0,004 0,002 0,000-0,002 1: SCALE 5.1 (ENDF/B-V, 44EGs) 2: SCALE 6 (ENDF/B-VII.0, CE) 3: MCNP-4C2 (JENDL3.3) 4: SCALE6 (ENDF/B-VII.0, CE) 5: MCNPX-2.5 (JEFF-3.1.1, CE) 6: MCNPX-2.4.0 (ENDF/B-VI, CE) 7: MCNPX-2.5 (JEFF-3.1.1, CE) 8: CRISTAL V1.0 (JEF 2.2, 172 EGs) 9: MORET 5 (JEFF-3.1) 10: SCALE 6 (ENDF/B-VII.0, 238 EGs) 11: SCALE 6 (ENDF/B-VII.0, 238 EGs) 12: SCALE 6 (ENDF/B-VII.0, CE) 13: MCNP5 V1.40 (ENDF/B-VII, CE) 14: MCNP5 (ENDF/B-VI.2, CE) 15: MCNP5 (ENDF/B-VI.2, CE) -0,004-0,006-0,008 Fresh Fuel: Mean=1.1481; StdDev=0.0031 Act: Mean=0.9551; StdDev=0.0025 Act + FP: Mean=0.8610; StdDev=0.0021 1 3 5 7 9 11 13 15 22

k eff as a Function of Decay Time for Actinide-only Fuel Compositions Actinide-only Fuel Compositions SCALE 5.1/KENO VI (ENDF/B-V, 44 EGs) keff 0.96 0.95 0.94 0.93 0.92 0.91 0.9 0.89 0.88 0.87 0.86 0.85 0.84 1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05 1.E+06 Decay Time (years) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP-4C2 (JENDL3.3) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (JEFF-3.1) MCNPX-2.4.0 (ENDF/B-VI); ACAB (JEFF-3.1) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (ORIGEN-S) CRISTAL V1.0 (JEF 2.2, 172 EGs) MORET 5 (JEFF-3.1) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP5 V1.40 (ENDF/B-VI, CE) MCNP5 (ENDF/B-VI.2, CE); ORIGEN-S MCNP5 (ENDF/B-VI.2, CE); TIBSO 23

k eff Result Variability as a Function of Decay Time (keff - keff_average)/keff_average (%) Actine-only Fuel Compositions 1.00% 0.80% 0.60% 0.40% 0.20% 0.00% -0.20% -0.40% -0.60% -0.80% -1.00% 1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05 1.E+06 Decay Time (years) SCALE 5.1/KENO VI (ENDF/B-V, 44 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP-4C2 (JENDL3.3) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (JEFF-3.1) MCNPX-2.4.0 (ENDF/B-VI); ACAB (JEFF-3.1) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (ORIGEN-S) CRISTAL V1.0 (JEF 2.2, 172 EGs) MORET 5 (JEFF-3.1) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP5 V1.40 (ENDF/B-VI, CE) MCNP5 (ENDF/B-VI.2 and V, CE); ORIGEN-S MCNP5 (ENDF/B-VI.2 and V, CE); TIBSO Δk eff-min = 0.0062 (150 years) Δk eff-max = 0.0153 (1,000,000 years) 24

Actinide-only k eff Values Mean and Standard Deviation as a Function of Decay Time 0,9600 0,0045 0,0040 0,9400 0,0035 0,9200 0,0030 0,0025 0,9000 0,0020 0,8800 0,0015 0,0010 0,8600 keff 0,0005 0,8400 0,01 0,1 1 10 100 1000 10000 100000 1000000 0,0000 25

k eff as a Function of Decay Time for Actinide and FP Fuel Compositions Actinide and FP Fuel Compositions SCALE 5.1/KENO VI (ENDF/B-V, 44 EGs) keff 0.86 0.85 0.84 0.83 0.82 0.81 0.8 0.79 0.78 0.77 0.76 0.75 0.74 0.73 1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05 1.E+06 Decay Time (years) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP-4C2 (JENDL3.3) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (JEFF-3.1) MCNPX-2.4.0 (ENDF/B-VI); ACAB (JEFF-3.1) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (ORIGEN-S) CRISTAL V1.0 (JEF 2.2, 172 EGs) MORET 5 (JEFF-3.1) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP5 V1.40 (ENDF/B-VI, CE) MCNP5 (ENDF/B-VI.2, CE) MCNP5 (ENDF/B-VI.2, CE) 26

k eff Result Variability as a Function of Decay Time (keff - keff_average)/keff_average (%) Actine and FP Fuel Compositions 0.80% 0.60% 0.40% 0.20% 0.00% -0.20% -0.40% -0.60% -0.80% -1.00% -1.20% 1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05 1.E+06 Decay Time (years) SCALE 5.1/KENO VI (ENDF/B-V, 44 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP-4C2 (JENDL3.3) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (JEFF-3.1) MCNPX-2.4.0 (ENDF/B-VI); ACAB (JEFF-3.1) MCNPX-2.5 (JEFF-3.1.1, CE); ACAB (ORIGEN-S) CRISTAL V1.0 (JEF 2.2, 172 EGs) MORET 5 (JEFF-3.1) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, 238 EGs) SCALE 6/KENO V.a (ENDF/B-VII.0, CE) MCNP5 V1.40 (ENDF/B-VI, CE) MCNP5 (ENDF/B-VI.2 and V, CE); ORIGEN-S MCNP5 (ENDF/B-VI.2 and V, CE); TIBSO Δk eff-min = 0.0059 (20 and 40 years) Δk eff-max = 0.0112 (45,000 years) 27

Cross-section Data Sensitivity and Uncertainty Analysis ENDF/B-VII Neutron Cross-Section Data Actinide and Fission Product Compositions 28

SCALE/TSUNAMI Cross-section Sensitivity and Uncertainty Analysis SCALE ENDF/B-VII 238 energy-group library Covariance data from ENDF/B-VII, ENDF/B-VI and JENDL3.3 Energy and region integrated k eff sensitivity to total and reaction-specific cross section (sensitivity coefficient) δk eff eff S n = k, Σ x n n δσ x / Σ x k eff uncertainty due to cross-section covariance data / k 29

k eff Sensitivity to ENDF/B-VII Cross-section Data for Actinides 31

k eff Sensitivity to ENDF/B-VII Cross-section Data for FPs 32

k eff Uncertainty Due to Cross-section Covariance Data 33

Main Contributions to k eff Uncertainty: 5-Year Composition 34

Main Contributions to k eff Uncertainty: 100-Year Composition 35

Main Contributions to k eff Uncertainty: 100,000-Year Composition 36

Summary Remarks / Observations 37

Summary: Participation 11 countries, 13 organizations, 14 decay calculations, 15 criticality calculations ORIGEN, ORIGEN-based, DARWIN, PHOENIX decay calculation codes Numerical and analytical methods for solving decay chain equations Matrix exponential method (ORIGEN, PHOENIX) Analytical method and 4th order Runge Kutta numerical method (DARWIN, PHOENIX) Decay data libraries ENDF/B-V, VI JENDL3.3 JEFF-3.1 JEF-2.2 SCALE, MCNP, MORET Monte Carlo criticality codes Neutron cross-section data libraries ENDF/B-V, 44 energy groups ENDF/B-VI continuous energy ENDF/B-VII.0 continuous energy ENDF/B-VII.0 238 energy groups JEF-2.2, 172 energy groups JENDL3.3 continuous energy JEFF-3.1 continuous energy JEFF-3.1.1 continuous energy 38

Preliminary Observations: Decay Calculations Several different trends identified Different trends between the results obtained with JENDL and ORIGEN2 DECAY.LIB data libraries (ORIGEN2.2UPJ and PHOENIX 1.0.0a) and the other results for 239 Pu, 240 Pu, 242 Pu, 242m Am Different trends among the results obtained with different libraries for 241 Pu, 243 Am Different trends between the results obtained with JEF and JENDL decay data libraries (DARWIN, TIBSO, and ORIGEN2.2UPJ) and the other results for 151 Sm, 151 Eu Different trends between the results obtained with JEF and ORIGEN2 DECAY.LIB data libraries (DARWIN, TIBSO, and PHOENIX 1.0.0a) and the other results for 155 Gd ( 155 Eu) 39

Preliminary Observations: Criticality Calculations k eff calculations were performed using a variety of criticality codes and cross-section data Results for specified compositions provide insights into variations due to criticality code and cross-section data Fresh fuel composition k eff varied from 1.1429 ± 0.0008 (SCALE 5.1, ENDF/B-V 44 EGs) to 1.1540 ± 0.0003 (CRISTAL V1.0, JEF-2.2, 172 EGs) Discharge actinide-only fuel composition k eff varied from 0.9507 ± 0.0004 (SCALE 6, ENDF/B-VII.0 CE) to 0.9582 ± 0.0003 (MCNPX-2.5, JEFF-3.1.1 CE) Discharge actinide and FP fuel composition k eff varied from 0.8568 ± 0.0003 (SCALE 6, ENDF/B-VII.0 CE) to 0.8639 ± 0.0005 (MCNP-4C2, JENDL3.3 CE) 40

Preliminary Observations: Criticality Calculations k eff results for time-dependent compositions show the impact of nuclear data, calculation method, and isotopic composition bias Computational method and cross-section data appear to have a larger impact on k eff than differences in isotopic composition predictions k eff results for time-dependent actinide-only compositions Δk eff-min = 0.0062 (150 years) Δk eff-max = 0.0153 (1,000,000 years) k eff results for time-dependent actinide and FP compositions Δk eff-min = 0.0059 (20 and 40 years) Δk eff-max = 0.0112 (45,000 years) k eff uncertainty due to covariance data Min %Δk eff/ k eff = 0.4845 (100,000 years) Max %Δk eff/ k eff = 0.7601 (100 years) 41

Next steps Complete analysis of participant s results Communicate with participants about their results, as needed Perform sensitivity calculations for isotopic predictions Complete and circulate draft report to participants for review Propose follow-up activity, if identified Publish benchmark report 42

Backup Slides 43

Comparison of Decay Calculation Results for U-234 44

Comparison of Decay Calculation Results for Np-237 241 Pu (14.4y) 241 Am (432.7y) 237 Np (2.14E6y) 45

Comparison of Decay Calculation Results for Pu-239 46

Comparison of Decay Calculation Results for Pu-240 Note: Different trends between ORIGEN2.2UPJ and PHONIX 1.0.0a beta results and the results of the other calculations for long decay times. 47

Comparison of Decay Calculation Results for Pu-242 Note: Different trends between ORIGEN2.2UPJ and PHONIX 1.0.0a beta results and the results of the other calculations for long decay times. 48

Comparison of Decay Calculation Results for Am-241 241 Pu (14.4y) 241 Am (432.7y) 49

Comparison of Decay Calculation Results for Am-242m Note: Different trends between ORIGEN2.2UPJ and PHONIX 1.0.0a beta results and the results of the other calculations for long decay times. 50

Comparison of Decay Calculation Results for Am-243 51

Comparison of k eff Values for the Fresh Fuel Composition 1.156 Fresh Fuel Composition keff 1.154 1.152 1.15 1.148 1.146 1.144 1.142 1: SCALE 5.1 (ENDF/B-V, 44EGs) 2: SCALE 6 (ENDF/B-VII.0, CE) 3: MCNP-4C2 (JENDL3.3) 4: SCALE6 (ENDF/B-VII.0, CE) 5: MCNPX-2.5 (JEFF-3.1.1, CE) 6: MCNPX-2.5 (ENDF/B-VI, CE) 7: MCNPX-2.5 (JEFF-3.1.1, CE) 8: CRISTAL V1.0 (JEF 2.2, 172 EGs) 9: MORET 5 (JEFF-3.1) 10: SCALE 6 (ENDF/B-VII.0, 238 EGs) 11: SCALE 6 (ENDF/B-VII.0, 238 EGs) 12: SCALE 6 (ENDF/B-VII.0, CE) 13: MCNP5 V1.40 (ENDF/B-VI, CE) 1.14 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 Criticality Calculation No. k eff-max k eff-min = 0.01109 52

Comparison of k eff Values for Discharge Actinide-only Fuel Composition 0.96 Discharge Actinide-only Fuel Composition keff 0.959 0.958 0.957 0.956 0.955 0.954 0.953 0.952 0.951 1: SCALE 5.1 (ENDF/B-V, 44EGs) 2: SCALE 6 (ENDF/B-VII.0, CE) 3: MCNP-4C2 (JENDL3.3) 4: SCALE6 (ENDF/B-VII.0, CE) 5: MCNPX-2.5 (JEFF-3.1.1, CE) 6: MCNPX-2.4.0 (ENDF/B-VI, CE) 7: MCNPX-2.5 (JEFF-3.1.1, CE) 8: CRISTAL V1.0 (JEF 2.2, 172 EGs) 9: MORET 5 (JEFF-3.1) 10: SCALE 6 (ENDF/B-VII.0, 238 EGs) 11: SCALE 6 (ENDF/B-VII.0, 238 EGs) 12: SCALE 6 (ENDF/B-VII.0, CE) 13: MCNP5 V1.40 (ENDF/B-VI, CE) 14: MCNP5 (ENDF/B-VI.2, CE) 15: MCNP5 (ENDF/B-VI.2, CE) 0.95 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 Criticality Calculation No. k eff-max k eff-min = 0.00749 53

Comparison of k eff Values for Discharge Actinide and FP Fuel Composition 0.866 Discharge Actinide and Fission Product Fuel Composition keff 0.865 0.864 0.863 0.862 0.861 0.86 0.859 0.858 0.857 1: SCALE 5.1 (ENDF/B-V, 44EGs) 2: SCALE 6 (ENDF/B-VII.0, CE) 3: MCNP-4C2 (JENDL3.3) 4: SCALE6 (ENDF/B-VII.0, CE) 5: MCNPX-2.5 (JEFF-3.1.1, CE) 6: MCNPX-2.4.0 (ENDF/B-VI, CE) 7: MCNPX-2.5 (JEFF-3.1.1, CE) 8: CRISTAL V1.0 (JEF 2.2, 172 EGs) 9: MORET 5 (JEFF-3.1) 10: SCALE 6 (ENDF/B-VII.0, 238 EGs) 11: SCALE 6 (ENDF/B-VII.0, 238 EGs) 12: SCALE 6 (ENDF/B-VII.0, CE) 13: MCNP5 V1.40 (ENDF/B-VI, CE) 14: MCNP5 (ENDF/B-VI.2, CE) 15: MCNP5 (ENDF/B-VI.2, CE) 0.856 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 Criticality Calculation No. k eff-max k eff-min = 0.00714 54

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