Home Physical Sciences Non-destructive assay of plutonium in absence of gamma-ray spectrometry
Article
Licensed
Unlicensed Requires Authentication

Non-destructive assay of plutonium in absence of gamma-ray spectrometry

  • Sanhita Chaudhury ORCID logo EMAIL logo , Ashwani Kumar , Sabyasachi Patra and Rahul Tripathi EMAIL logo
Published/Copyright: February 14, 2024

Abstract

Gamma-ray spectrometry-based isotopic composition analysis is a prerequisite for absolute non-destructive assay of Pu by neutron counting or calorimetry. However, gamma-ray spectrometry can be complicated in samples that are heavily shielded or have a high 241Am fraction. Herein, for the absolute non-destructive assay of Pu, a simple yet potent empirical methodology combining neutron multiplicity counting and calorimetry is proposed, which obviates the need for gamma-ray spectrometry-based isotopic composition analysis. The approach includes stepwise correlation between the parameters obtained from neutron multiplicity counting, i.e., α ((α, n) neutron to spontaneous fission neutron ratio), effective mass of 240Pu, and D (doubles neutron rate) with the thermal power output (W Pu) due to radioactive decay (measured by calorimetry). Because D and W Pu both are governed by the Pu isotopic composition, their correlation should be sensitive to the isotopic information in a given sample. Mandatory correction for the 241Am contribution in W Pu was done using the linear plot between its weight fraction and the corresponding α. The proposed methodology was validated by analyzing several PuO2 standards containing high 241Am fraction (0.02–0.09). The measured Pu amounts were within 8 % of the actual values with measurement uncertainties between 8 and 10 %, which shows the potential of the proposed methodology for the assay of samples having high 241Am content or for the quantification of Pu in heavily shielded samples.


Corresponding authors: Sanhita Chaudhury and Rahul Tripathi, Radiochemistry Division, Bhabha Atomic Research Centre, Mumbai 400085, India; and Chemical Sciences Department, Homi Bhabha National Institute, Mumbai 400094, India, E-mail: (S. Chaudhury), (R. Tripathi)

  1. Research ethics: Not applicable.

  2. Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Competing interests: The authors state no conflict of interest.

  4. Research funding: None declared.

  5. Data availability: Not applicable.

References

1. Reilly, D., Ensslin, N., Smith, H., Kreiner, S. Passive Nondestructive Assay of Nuclear Materials; Los Alamos National Laboratory: Los Alamos, 1991.10.2172/5428834Search in Google Scholar

2. Krachler, M., Wallenius, M., Nicholl, A., Mayer, K. Spatially-resolved uranium isotopic analysis of contaminated scrap metal using laser ablation multi-collector ICP-MS. RSC Adv. 2020, 10, 16629–16636; https://doi.org/10.1039/d0ra02899a.Search in Google Scholar PubMed PubMed Central

3. Straub, M. D., Arnold, J., Fessenden, J., Kiplinger, J. L. Recent advances in nuclear forensic chemistry. Anal. Chem. 2021, 93, 3–22; https://doi.org/10.1021/acs.analchem.0c03571.Search in Google Scholar PubMed

4. Clapham, M., Farese, N., Jaime, R., Lezzoli, L., Schillebeeckx, P. Performance comparison of different active neutron interrogation techniques for safeguards applications. In Proc. of the 19th ESARDA Symposium on Safeguards and Nuclear Material Management; ESARDA: Montpellier, 1997; pp. 359–367.Search in Google Scholar

5. Ferrer, M. M., Peerani, P., Looman, M. R., Dechamp, L. Design and performances of the scrap neutron multiplicity counter. Nucl. Instrum. Methods Phys. Res. A 2007, 574, 297–314; https://doi.org/10.1016/j.nima.2007.01.167.Search in Google Scholar

6. Sakaguchi, A., Steier, P., Takahashi, Y., Yamamoto, M. Isotopic compositions of 236U and Pu isotopes in “black substances” collected from roadsides in Fukushima Prefecture: fallout from the Fukushima Daiichi nuclear power plant accident. Environ. Sci. Technol. 2014, 48, 3691–3697; https://doi.org/10.1021/es405294s.Search in Google Scholar PubMed

7. Sampson, T. E. Plutonium Isotopic Analysis Using PC/FRAM, Los Alamos National Laboratory Report: Los Alamos, LA-UR-03-4403, 2003, pp. 2-1–2-56.Search in Google Scholar

8. Wu, J., Zheng, J., Dai, M., Huh, C., Chen, W., Tagami, K., Uchida, S. Isotopic composition and distribution of plutonium in northern south China sea sediments revealed continuous release and transport of Pu from the Marshall Islands. Environ. Sci. Technol. 2014, 48, 3136–3144; https://doi.org/10.1021/es405363q.Search in Google Scholar PubMed

9. Chaudhury, S., Agarwal, C., Patra, S., Goswami, A. Isotopic composition analysis of dilute Pu solutions using 90−105 keV region of gamma ray spectra. Appl. Rad. Isotopes 2017, 119, 66–71; https://doi.org/10.1016/j.apradiso.2016.11.009.Search in Google Scholar PubMed

10. Patra, S., Agarwal, C., Chaudhury, S., Newton Nathaniel, T., Gathibandhe, M., Goswami, A. Isotopic ratio correlation for the isotopic composition analysis of plutoniumin in Am–Pu mixed samples having high americium content. Appl. Rad. Isotopes 2013, 78, 139–144; https://doi.org/10.1016/j.apradiso.2013.04.007.Search in Google Scholar PubMed

11. Chaudhury, S., Ali, M. Y., Patra, S., Agarwal, C., Jadhav, R. T., Pujari, P. K. Development of a 3He Based Neutron Multiplicity Counter, BARC Report, BARC/2018/I/008; Mumbai, 2018; pp. 1–24.Search in Google Scholar

12. Goddard, B., Croft, S. High-fidelity passive neutron multiplicity measurements and simulations of uranium oxide. Nucl. Instrum. Methods Phys. Res. A 2013, 712, 147–156; https://doi.org/10.1016/j.nima.2013.02.007.Search in Google Scholar

13. Ensslin, N., Harker, W. C., Krick, M. S., Langner, D. G., Pickrell, M. M., Stewart, J. E. Application Guide to Neutron Multiplicity Counting, Los Alamos National Laboratory Report, LA-13422-M, UC-700, 1998, pp. 1–105.Search in Google Scholar

14. Patra, S., Mhatre, A. M., Chaudhury, S., Agarwal, C., Naik, H., Pujari, P. K. Non-destructive assay of special nuclear materials by calorimetry. In Proceedings of the 13th DAE-BRNS Nuclear and Radiochemistry Symposium; Bhubaneswar, 2017, INIS ref no. 48054061.Search in Google Scholar

15. Abousahl, S., van Belle, P., Ottmar, H. Measurement of the Pu content and isotope abundances by combined calorimetry, neutron coincidence counting and gamma spectrometry (CANEGA). In Proceedings of the 2003 ESARDA Symposium – 25th ESARDA Annual Meeting, 2003, pp. 283–291.Search in Google Scholar

16. Abousahl, S., van Belle, P., Ottmar, H. Combined calorimetry/neutron coincidence counting/gamma spectrometry (CANEGA) measurements for plutonium mass and isotopic assay. Nucl. Instrum. Methods Phys. Res. A 2005, 543, 608–618; https://doi.org/10.1016/j.nima.2004.12.011.Search in Google Scholar

17. Ottmar, H., Abousahl, S., van Belle, P., van Vuure, T., Burke, K., Mason, J., Tolchar, A., Towner, A. A combined calorimetry, neutron coincidence counting and gamma spectrometry system (CANEGA) for enhanced plutonium mass and isotopic assay. In Proceedings of an International Safeguards Symposium on Addressing Verification Challenges Organized by IAEA in Cooperation with the Institute of Nuclear Materials Management and the European Safeguards Research and Development Association; Vienna, 2006, pp. 495–505.Search in Google Scholar

18. Patra, S., Agarwal, C. Combined calorimetry – neutron counting – gamma spectrometry (C-N-G) approach for the isotopic composition analysis of plutonium. In Proceedings of the 14th DAE-BRNS Nuclear and Radiochemistry Symposium; DAE-BRNS: Mumbai, 2019; p. 178.Search in Google Scholar


Supplementary Material

This article contains supplementary material (https://doi.org/10.1515/ract-2023-0193).


Received: 2023-07-13
Accepted: 2023-12-30
Published Online: 2024-02-14
Published in Print: 2024-08-27

© 2024 Walter de Gruyter GmbH, Berlin/Boston

Articles in the same Issue

  1. Frontmatter
  2. Preface
  3. NUCAR-2023: Foreword
  4. Research Articles
  5. Theoretical analysis of light and heavy-ion induced reactions: production of medically relevant 97Ru
  6. Excitation functions of alpha-particle induced nuclear reactions on nat Sn
  7. Non-destructive assay of plutonium in absence of gamma-ray spectrometry
  8. Catalytic destruction of oxalate in the supernatant stream generated during plutonium reconversion process
  9. Quantification of Zr in simulated dissolver solution of U–Zr fuel by laser-induced breakdown spectroscopy
  10. Radiochemical and chemical characterization of fuel, salt, and deposit from the electrorefining of irradiated U-6 wt% Zr in hot cells
  11. Zirconium sponge production: an integrated approach for chemical characterization of process intermediates using ICP-OES
  12. Determination of 10B/11B in boric acid and B4C using LA-ICPMS
  13. Evaluating sustainability of Bhuj aquifer system, Western India using nuclear dating techniques
  14. Nanocrystalline Ce(OH)4-based materials: ruthenium selective adsorbent for highly alkaline radioactive liquid waste
  15. Production and radiochemical separation of 68Ge from irradiated Ga–Ni alloy target in 30 MeV cyclotron
  16. Preparation of [64Cu]Cu–NOTA complex as a potential renal PET imaging agent using 64Cu produced via the direct activation route
  17. Total chemical synthesis of PSMA-617: an API for prostate cancer endotherapeutic applications
  18. Rapid screening technique for gross α and gross β estimations in aqueous samples during radiation emergency
  19. Development of Dy3+ doped lithium magnesium borate glass system for thermoluminescence based neutron dosimetry applications
Downloaded on 30.12.2025 from https://www.degruyterbrill.com/document/doi/10.1515/ract-2023-0193/html
Scroll to top button