Isolating trace fission product elements in separated plutonium for applications in nuclear forensics
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Isolating trace fission product elements in separated plutonium for applications in nuclear forensics Kevin J. Glennon1,2,3 · Evelyn M. Bond3 · Todd A. Bredeweg3 · Sunil S. Chirayath4,5 · Charles M. Folden III1,2 Received: 10 July 2020 / Accepted: 4 October 2020 © Akadémiai Kiadó, Budapest, Hungary 2020
Abstract A chemical methodology has been selected to isolate and concentrate select trace fission product (FP) elements from separated Pu for nuclear forensics. The methodology employs several different resins and eluents to chromatographically separate U and the FP elements of interest into their own fractions. The U, rare-earth element, Cs, and Ba fractions were isolated with relative yields of ≥ 73.8%, ≥ 80.7%, ≥ 98.5%, and ≥ 98.0%, respectively. The methodology was able to successively isolate select FP elements on the order of 10–10 g out of much larger samples of Pu. Keywords Plutonium · Nuclear forensics · Ion-exchange chromatography · Fission products · Separations
Introduction Determining the origin of suspect material is a key component in all fields of forensics [1–8]; identifying facts about the origin of such material may reveal information about the entities responsible for its production or proliferation. Pu source discrimination has been a recent focus in the field of nuclear forensics for these same reasons [8–14]. When samples of special nuclear material (SNM, 233U, enriched 235U, or Pu) have been interdicted during smuggling operations in the past, some of the first questions asked were “Where did it come from,” and “Is there more?” [15–18] Developing Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10967-020-07448-3) contains supplementary material, which is available to authorized users. * Charles M. Folden III [email protected] 1
Cyclotron Institute, Texas A&M University, College Station, TX 77843, USA
2
Department of Chemistry, Texas A&M University, College Station, TX 77843, USA
3
Nuclear and Radiochemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA
4
Center for Nuclear Security Science and Policy Initiatives, Texas A&M University, College Station, TX 77843, USA
5
Department of Nuclear Engineering, Texas A&M University, College Station, TX 77843, USA
modern procedures to discriminate the origin of SNM is necessary to ensure these questions may be answered quickly and accurately [19–27]. Traditionally, nuclear forensics has used 3-dimensional plots of various Pu isotope ratios to discriminate the origin of separated Pu by reactor type, fuel burnup, and cooling time [22, 26–28]. This approach to forensics has been proven effective for determining the reactor origin of Pu separated from high burnup fuel up to 50 GWd/MTU, such as would be produced in a power reactor. However, these plots tend to converge at lower fuel burnups around 1 GWd/MTU, making it difficult or impossible to discriminate the reactor origin of weapons-grade Pu without initial assumptions about its origin. In recent years, a novel appr
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