Isotopic and Compositional Variations in Single Nuclear Fuel Pellet Particles Analyzed by Nanoscale Secondary Ion Mass Spectrometry

Connaugh M Fallon; William R Bower; Ian C Lyon; Francis R Livens; Paul Thompson; Matthew Higginson; Jane Collins; Sarah L Heath; Gareth T W Law

doi:10.1021/acsomega.9b02703

Isotopic and Compositional Variations in Single Nuclear Fuel Pellet Particles Analyzed by Nanoscale Secondary Ion Mass Spectrometry

ACS Omega. 2019 Dec 27;5(1):296-303. doi: 10.1021/acsomega.9b02703. eCollection 2020 Jan 14.

Authors

Connaugh M Fallon^{1

1}, William R Bower^{1

2}, Ian C Lyon^{1

1}, Francis R Livens^{1

1}, Paul Thompson³, Matthew Higginson³, Jane Collins³, Sarah L Heath¹, Gareth T W Law^{1

2}

Affiliations

¹ Centre for Radiochemistry Research, Department of Chemistry, Department of Earth and Environmental Sciences and Photon Science Institute, School of Natural Sciences, The University of Manchester, Manchester M13 9PL, United Kingdom.
² Radiochemistry Unit, Department of Chemistry, The University of Helsinki, Helsinki 00014, Finland.
³ Atomic Weapons Establishment, Aldermaston RG7 4PR, United Kingdom.

Abstract

The Collaborative Materials Exercise (CMX) is organized by the Nuclear Forensics International Technical Working Group, with the aim of advancing the analytical capabilities of the participating organizations and providing feedback on the best approaches to a nuclear forensic investigation. Here, model nuclear fuel materials from the 5^th CMX iteration were analyzed using a NanoSIMS 50L (CAMECA) in order to examine inhomogeneities in the ²³⁵U/²³⁸U ratio and trace element abundance within individual, micrometer scale particles. Two fuel pellets were manufactured for the exercise and labelled CMX-5A and CMX-5B. These pellets were created using different processing techniques, but both had a target enrichment value of ²³⁵U/²³⁸U = 0.01. Particles from these pellets were isolated for isotopic and trace element analysis. Fifteen CMX-5A particles and 20 CMX-5B particles were analyzed, with both sample types displaying inhomogeneities in the U isotopic composition at a sub-micrometer scale within individual particles. Typical particle diameters were ∼1.5 to 41 μm for CMX-5A and ∼1 to 61 μm for CMX-5B. The CMX-5A particles were shown to be more isotopically homogeneous, with a mean ²³⁵U/²³⁸U atom ratio of 0.0130 ± 0.0066. The CMX-5B particles showed a predominantly depleted mean ²³⁵U/²³⁸U atom ratio of 0.0063 ± 0.0094, which is significantly different to the target enrichment value of the pellet and highlights the potential variation of ²³⁵U/²³⁸U in U fuel pellets at the micrometer scale. This study details the successful application of the NanoSIMS 50L in a mock nuclear forensic investigation by optimizing high-resolution imaging for uranium isotopics.