Active neutron coincidence counting to determine fissile mass of uranium oxide containing 233U and 235U

Madeline Lockhart, Richard L. Reed, Louise G. Evans, Vlad Henzl, John Mattingly

Research output: Contribution to journalArticlepeer-review

Abstract

Active neutron coincidence measurements of uranium oxide (UO3) were conducted with an active well coincidence counter (AWCC) at Oak Ridge National Laboratory (ORNL). We performed systematic measurements with the AWCC in fast and thermal mode of well-documented uranium oxide items containing 233U, 235U, and mixtures of the two isotopes up to 144 g of total fissile mass. The objective was to document active neutron coincidence measurements of items containing 233U and to assess the feasibility of 233U characterization and discrimination from 235U using existing neutron-based safeguards instrumentation and measurement methods. The colocation of 233U with other isotopes of uranium, including 235U, presents a challenge because existing nondestructive assay (NDA) methods are not tailored to these isotopic mixtures. Therefore, neutron signatures of 233U-bearing materials were performed and documented to inform the safeguards community when addressing future nuclear nonproliferation needs related to 233U for material control and accountability and potential thorium-based advanced reactors, which breed 233U. The neutron coincidence measurements described contribute to the foundation for future development of material characterization methods and provide experimental data points for validation of simulations. We measured active calibration curves, which relate the fissile mass to the coincident count rate, for 2–80 g of 233U, 2–64 g235U, and 4–144 g of a mixture of 233U and 235U. In thermal mode, the total fissile mass could be determined, but isotope discrimination is not possible. An unknown mixed item was measured in thermal mode and the total fissile mass was calculated within 1σ of the declared mass. In fast mode, we observe a difference between the 233U and 235U curves, but a low coincidence count rate and high uncertainty prevent statistically meaningful determination of fissile mass, especially for 235U.

Funding

This work was supported by the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) Office of Defense Nuclear Nonproliferation Research and Development (DNN R&D) Safeguards program. This research was performed under appointment to the Nuclear Nonproliferation International Safeguards Fellowship Program sponsored by the National Nuclear Security Administration's Office of International Nuclear Safeguards. This work was completed on behalf of DNN R&D by a multi-laboratory team including researchers from Los Alamos National Laboratory (LANL), Oak Ridge National Laboratory (ORNL), Sandia National Laboratories (SNL), and Y-12 National Security Complex with contributions from students at the University of Tennessee, North Carolina State University, and the University of Michigan. The authors would like to acknowledge and thank research collaborators including Dr. Holly Trellue and Dr. Daniel Jackson of LANL; Dr. Heather Reedy, Dr. Oskar Searfus, Dr. Peter Marleau, Dr. Eva Uribe of SNL; and Dr. Matt Cook and Mr. Alex Roberts of Y-12 National Security Complex. The authors would also like to acknowledge and thank Greg Nutter, Dr. Robert D. McElroy, Jr. Dr. Karen Koop Hogue, Dr. Susan Smith, Ms. Rachel Hunneke, Mr. Scotty Mathews, and Mr. Dave Aguero of ORNL for assisting with the coordination, facilitation, and supervision of numerous experimental measurement campaigns, as well as for productive discussions on this topic. This work was supported by the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) Office of Defense Nuclear Nonproliferation Research and Development (DNN R&D) Safeguards program. This research was performed under appointment to the Nuclear Nonproliferation International Safeguards Fellowship Program sponsored by the National Nuclear Security Administration\u2019s Office of International Nuclear Safeguards.

Keywords

  • AWCC
  • Active coincidence calibration curve
  • Active neutron interrogation
  • Fast mode
  • Fissile mass
  • Neutron coincidence counting
  • Thermal mode
  • Uranium oxide
  • Uranium-233
  • Uranium-235

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