TY - JOUR
T1 - Corrigendum to “REGAL International Program
T2 - Analysis of experimental data for depletion code validation” [Ann. Nucl. Energy 172 (2022) 109057](S0306454922000925)(10.1016/j.anucene.2022.109057)
AU - Eysermans, J.
AU - Verwerft, M.
AU - Govers, K.
AU - Ichou, R.
AU - Ilas, G.
AU - Meryturek, U.
AU - Messaoudi, N.
AU - Romojaro, P.
AU - Slosse, N.
N1 - Publisher Copyright:
© 2024 The Author(s)
PY - 2024/9/15
Y1 - 2024/9/15
N2 - In the original submission of this paper, comparison between the calculated and experimental nuclide inventory of UO2 and (U, Gd)O2 fuel rod samples was presented [1]. The experimental analysis of the Gd inventory was recently found to be biased on the two isotopes of interest, 155Gd and 157Gd, which were both close to full depletion in the (U, Gd)O2 sample discussed in the paper. The analysis of the Gd isotopic inventory was performed by Isotope Dilution Thermal Ionization Mass Spectrometry (ID-TIMS) after column separation of fission generated lanthanides which could isobarically interfere with the isotopes of interest. Gadolinium was analysed using its monoxide ion signals (GdO+), while TIMS analyses of the other elements were performed on the metal ion signals (M+). The reason for this relates back to the original TIMS method development at SCK CEN and has been applied as such for decades: measurements on the direct Gd metal ion signals were often unstable, hence the choice to measure Gd at its monoxide GdO+ ion masses. The gadolinium vector (Gd-152 to Gd-160) was thus measured on masses 168 to 176. The data processing, however, did not originally include corrections for the isotopes of oxygen ([16O] = 0.99757(16), [17O] = 0.00038(1), [18O] = 0.00205(14)) [2]. When deep burnout is reached on isotopes 155Gd and 157Gd, interference of the 155Gd16O monoxide signal at mass 171 due to 154Gd17O and of the 157Gd16O signal at mass 173 due to 156Gd17O become significant. The interference on mass 173 due to 155Gd18O remains negligible since 155Gd is present in low concentrations only. As the effect of the minor oxygen isotopes was not taken into account in the experimental analysis, the isotopic abundances of both 155Gd and 157Gd were overestimated. For 155Gd, the overestimation was 5.6%, and for 157Gd, the overestimation was 60%. Concentrations of other nuclides remained unaffected as they were analysed on the metal ion (M+) signal. In the original paper, comparison between calculated and experimental nuclide concentrations were reported for several codes and code-library combinations [1]. For the 155Gd and 157Gd isotopes, the C/E – 1 values showed a systematic bias with of 6.4% and 60%, respectively. When performing the same assessment using the 155Gd and 157Gd concentrations properly corrected for the oxygen isotope effect, the systematic bias disappears. For 155Gd, deviations are of the same order of magnitude as the experimental uncertainty (3.4% at 2 sigma) for all codes. The experimental uncertainty of 157Gd is larger (8.4% at 2 sigma), and most codes calculate the measured 157Gd concentration reasonably well. Only the WIMS code, in combination with the ENDF/B VII.1 library, has a significant deviation for 157Gd. Table 4 and Figure 7 of the original publication are revised. For completeness, the entire Table 4 and complete Figure 4 are reproduced, but only the experimental values for the two gadolinium nuclides, 155Gd and 157Gd have changed. A paper on the experimental methodology is under preparation. Table 4. Comparison of code predictions to experimental measurements for the E14 sample, expressed in percentage as C/E–1 with C the calculated value (per code) and E the experimental value in g/gfuel. The nuclide ‘‘Fissile” is the sum of U-235, Pu-239, and Pu-241. [Table presented][Formula presented] Fig. 1 Comparison of code predictions to experimental measurements for the E14 sample, expressed in percentage as C/E–1 with C the calculated value (per code) and E the experimental value in g/gfuel. Due to the large discrepancy, the C/E–1 value for the WIMS code for Gd-157 is outside of the scale shown. The error bars represent the uncertainty (2 sigma) of the experimental data. References [1] J. Eysermans, M. Verwerft, K. Govers, R. Ichou, G. Ilas, U. Meryturek, N. Messaoudi, P. Romojaro, N. Slosse, REGAL International Program: Analysis of experimental data for depletion code validation, Annals of Nuclear Energy 2022, 172. [2] J.S. Coursey, D.J. Schwab, J.J. Tsai, R.A. Dragoset, Atomic Weights and Isotopic Compositions (version 4.1). [Online] Available: http://physics.nist.gov/Comp 2015. (Accessed 2023-05-31 2023). The authors would like to apologise for any inconvenience caused.
AB - In the original submission of this paper, comparison between the calculated and experimental nuclide inventory of UO2 and (U, Gd)O2 fuel rod samples was presented [1]. The experimental analysis of the Gd inventory was recently found to be biased on the two isotopes of interest, 155Gd and 157Gd, which were both close to full depletion in the (U, Gd)O2 sample discussed in the paper. The analysis of the Gd isotopic inventory was performed by Isotope Dilution Thermal Ionization Mass Spectrometry (ID-TIMS) after column separation of fission generated lanthanides which could isobarically interfere with the isotopes of interest. Gadolinium was analysed using its monoxide ion signals (GdO+), while TIMS analyses of the other elements were performed on the metal ion signals (M+). The reason for this relates back to the original TIMS method development at SCK CEN and has been applied as such for decades: measurements on the direct Gd metal ion signals were often unstable, hence the choice to measure Gd at its monoxide GdO+ ion masses. The gadolinium vector (Gd-152 to Gd-160) was thus measured on masses 168 to 176. The data processing, however, did not originally include corrections for the isotopes of oxygen ([16O] = 0.99757(16), [17O] = 0.00038(1), [18O] = 0.00205(14)) [2]. When deep burnout is reached on isotopes 155Gd and 157Gd, interference of the 155Gd16O monoxide signal at mass 171 due to 154Gd17O and of the 157Gd16O signal at mass 173 due to 156Gd17O become significant. The interference on mass 173 due to 155Gd18O remains negligible since 155Gd is present in low concentrations only. As the effect of the minor oxygen isotopes was not taken into account in the experimental analysis, the isotopic abundances of both 155Gd and 157Gd were overestimated. For 155Gd, the overestimation was 5.6%, and for 157Gd, the overestimation was 60%. Concentrations of other nuclides remained unaffected as they were analysed on the metal ion (M+) signal. In the original paper, comparison between calculated and experimental nuclide concentrations were reported for several codes and code-library combinations [1]. For the 155Gd and 157Gd isotopes, the C/E – 1 values showed a systematic bias with of 6.4% and 60%, respectively. When performing the same assessment using the 155Gd and 157Gd concentrations properly corrected for the oxygen isotope effect, the systematic bias disappears. For 155Gd, deviations are of the same order of magnitude as the experimental uncertainty (3.4% at 2 sigma) for all codes. The experimental uncertainty of 157Gd is larger (8.4% at 2 sigma), and most codes calculate the measured 157Gd concentration reasonably well. Only the WIMS code, in combination with the ENDF/B VII.1 library, has a significant deviation for 157Gd. Table 4 and Figure 7 of the original publication are revised. For completeness, the entire Table 4 and complete Figure 4 are reproduced, but only the experimental values for the two gadolinium nuclides, 155Gd and 157Gd have changed. A paper on the experimental methodology is under preparation. Table 4. Comparison of code predictions to experimental measurements for the E14 sample, expressed in percentage as C/E–1 with C the calculated value (per code) and E the experimental value in g/gfuel. The nuclide ‘‘Fissile” is the sum of U-235, Pu-239, and Pu-241. [Table presented][Formula presented] Fig. 1 Comparison of code predictions to experimental measurements for the E14 sample, expressed in percentage as C/E–1 with C the calculated value (per code) and E the experimental value in g/gfuel. Due to the large discrepancy, the C/E–1 value for the WIMS code for Gd-157 is outside of the scale shown. The error bars represent the uncertainty (2 sigma) of the experimental data. References [1] J. Eysermans, M. Verwerft, K. Govers, R. Ichou, G. Ilas, U. Meryturek, N. Messaoudi, P. Romojaro, N. Slosse, REGAL International Program: Analysis of experimental data for depletion code validation, Annals of Nuclear Energy 2022, 172. [2] J.S. Coursey, D.J. Schwab, J.J. Tsai, R.A. Dragoset, Atomic Weights and Isotopic Compositions (version 4.1). [Online] Available: http://physics.nist.gov/Comp 2015. (Accessed 2023-05-31 2023). The authors would like to apologise for any inconvenience caused.
UR - http://www.scopus.com/inward/record.url?scp=85192258366&partnerID=8YFLogxK
U2 - 10.1016/j.anucene.2024.110607
DO - 10.1016/j.anucene.2024.110607
M3 - Comment/debate
AN - SCOPUS:85192258366
SN - 0306-4549
VL - 205
JO - Annals of Nuclear Energy
JF - Annals of Nuclear Energy
M1 - 110607
ER -