A novel chronometry technique for dating irradiated uranium fuels using Cm isotopic ratios

Christl, Marcus; Guérin, Nicolas; Totland, Marina; Gagné, Alexandre; Kazi, Zakir H.; Burrell, Sean; Synal, Hans-Arno

doi:10.1007/s10967-019-06767-4

Cited by 8 publications

(6 citation statements)

References 10 publications

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“…A calibration curve has been fitted to a plot of log( 244 Cm/ 246 Cm) versus log( 245 Cm/ 246 Cm) for various types of nuclear fuel with a high linear correlation, regardless of the fuel type. 2 Therefore, correcting the ( 244 Cm/ 246 Cm)/( 245 Cm/ 246 Cm) of a sample of nuclear fuel of unknown age to this calibration curve will yield the age when it was retired from its neutron flux. This was performed by feeding the 245 Cm/ 246 Cm ratio of the sample (both spiked and unspiked aliquots were measured) into the power law relationship described by eq 15 to calculate the 244 Cm/ 246 Cm ratio at the origin [ 244 Cm/ 246 Cm] 0 …”

Section: Experimental Sectionmentioning

confidence: 99%

“…Using the 244 Cm/ 246 Cm (at/at) and 245 Cm/ 246 Cm (at/at) ratios of the Cm captured in the IIP-Y 3+ DGT sampler, the age when the nuclear fuel was retired from its neutron flux was calculated according to a model reported by Christl et al In brief, this is inferred from the decay of the shorter-lived isotope 244 Cm ( t 1/2 = 18 a), which diminishes the 244 Cm/ 246 Cm ratio significantly over several years, while the 245 Cm/ 246 Cm ratio is essentially constant over several centuries as both isotopes are longer-lived ( 245 Cm t 1/2 = 8250 a, 246 Cm t 1/2 = 4723 a). A calibration curve has been fitted to a plot of log( 244 Cm/ 246 Cm) versus log( 245 Cm/ 246 Cm) for various types of nuclear fuel with a high linear correlation, regardless of the fuel type . Therefore, correcting the ( 244 Cm/ 246 Cm)/( 245 Cm/ 246 Cm) of a sample of nuclear fuel of unknown age to this calibration curve will yield the age when it was retired from its neutron flux.…”

Section: Experimental Sectionmentioning

confidence: 99%

“…Employing AMS also allowed us to assess the validity of a recently developed Cm dating method for nuclear fuel. 2 We also report a novel radiochemical methodology to measure Am and Cm isotopes in the same fraction by AMS herein, enabling the production of c DGT for isotopes of both elements with a single 243 Am spike.…”

Section: Introductionmentioning

confidence: 99%

“…AMS allowed us to produce a comprehensive isotopic report, including for the spectrum of Cm isotopes 242–246 Cm following a short deployment period in the SFP of 24 h. This is not possible using α-spectrometry due to the overlapping α-emission energies of 243 Cm and 244 Cm, and 245 Cm and 246 Cm. Employing AMS also allowed us to assess the validity of a recently developed Cm dating method for nuclear fuel . We also report a novel radiochemical methodology to measure Am and Cm isotopes in the same fraction by AMS herein, enabling the production of c DGT for isotopes of both elements with a single 243 Am spike.…”

Section: Introductionmentioning

confidence: 99%

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Passive Sampling Tool for Actinides in Spent Nuclear Fuel Pools

et al. 2022

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Spent nuclear fuel must be carefully managed to prevent pollution of the environment with radionuclides. Within the framework of correct radioactive waste management, spent fuel rods are stored in cooling pools to allow short-lived fission products to decay. If fuel rods leak, they liberate radionuclides into the cooling water; therefore, it is essential to determine radionuclide concentrations in the pool water for monitoring purposes and to plan the decommissioning process. In this work, we present, to our knowledge, the first passive sampling technique for measures of actinides in spent nuclear fuel pools, based on recently developed diffusive gradients in thin-film (DGT) configurations. These samplers eliminate the need to retrieve and handle large samples of fuel pool water for radiochemical processing by immobilizing their targeted radionuclides in situ on the solid phase within the sampler. This is additionally the first application of the DGT technique for Cm measure. Herein, we make the calibrated effective diffusion coefficients of U, Pu, Am, and Cm in borated spent fuel pool water available. We tested these samplers in the fuel pool of a nuclear facility and measured samples using accelerator mass spectrometry to provide high-precision isotopic reports, allowing for the first independent implementation of a recently developed technique for dating nuclear fuel based on its Cm isotope signature.

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Section: Experimental Sectionmentioning

confidence: 99%

Section: Experimental Sectionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Passive Sampling Tool for Actinides in Spent Nuclear Fuel Pools

et al. 2022

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“…Material dispersed in fallout will often have a higher proportion of 244 Pu (ref. 16 ), whereas higher-burnup manufacture in thermal spectrum nuclear reactors, might afford an inventory effectively limited to 240 Pu and 241 Pu, generally with a higher proportion of 240 Pu; the decay of 241 Pu affords for the activation of americium products by neutrons and the formation of curium isotopes 17 , also less prominent in contributions from weapons fallout. While the isotopic association, particularly to identify plutonium in fallout, is well understood we are not aware of its use to discern the local contribution to breeder-borne material in the environment: hence the focus of this study.…”

Section: Introductionmentioning

confidence: 99%

Local and global trace plutonium contributions in fast breeder legacy soils

et al. 2021

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Trace-level plutonium in the environment often comprises local and global contributions, and is usually anthropogenic in origin. Here, we report estimates of local and global contributions to trace-level plutonium in soil from a former, fast-breeder reactor site. The measured 240Pu/239Pu ratio is anomalously low, as per the reduced 240Pu yield expected in plutonium bred with fast neutrons. Anomalies in plutonium concentration and isotopic ratio suggest forensic insight into specific activities on site, such as clean-up or structural change. Local and global 239Pu contributions on-site are estimated at (34 ± 1)% and (66 ± 3)%, respectively, with mass concentrations of (183 ± 6) fg g−1 and (362 ± 13) fg g−1. The latter is consistent with levels at undisturbed and distant sites, (384 ± 44) fg g−1, where no local contribution is expected. The 240Pu/239Pu ratio for site-derived material is estimated at 0.05 ± 0.04. Our study demonstrates the multi-faceted potential of trace plutonium assay to inform clean-up strategies of fast breeder legacies.

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