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Title: Oxidation and Hydration of U3O8 Materials Following Controlled Exposure to Temperature and Humidity

Journal Article · · Analytical Chemistry
DOI:https://doi.org/10.1021/ac504105t· OSTI ID:1329579
 [1];  [2];  [3];  [2];  [2];  [2];  [2];  [4];  [2];  [2];  [2];  [5];  [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Missouri, Columbia, MO (United States). Dept. of Chemistry
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry and Biochemistry
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Univ. of Missouri, Columbia, MO (United States). Dept. of Chemistry
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Chemical signatures correlated with uranium oxide processing are of interest to forensic science for inferring sample provenance. Identification of temporal changes in chemical structures of process uranium materials as a function of controlled temperatures and relative humidities may provide additional information regarding sample history. In this study, a high-purity α-U3O8 sample and three other uranium oxide samples synthesized from reaction routes used in nuclear conversion processes were stored under controlled conditions over 2–3.5 years, and powder X-ray diffraction analysis and X-ray absorption spectroscopy were employed to characterize chemical speciation. Signatures measured from the α-U3O8 sample indicated that the material oxidized and hydrated after storage under high humidity conditions over time. Impurities, such as uranyl fluoride or schoepites, were initially detectable in the other uranium oxide samples. After storage under controlled conditions, the analyses of the samples revealed oxidation over time, although the signature of the uranyl fluoride impurity diminished. The presence of schoepite phases in older uranium oxide material is likely indicative of storage under high humidity and should be taken into account for assessing sample history. The absence of a signature from a chemical impurity, such as uranyl fluoride hydrate, in an older material may not preclude its presence at the initial time of production. LA-UR-15-21495.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Nuclear Science and Security Consortium
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC52-06NA25396; AC02-76SF00515; HSGQDC-13-X-00269; HDHQDC-08-X-00805; 2012-DN-130-NF0001-02; NA0000979
OSTI ID:
1329579
Alternate ID(s):
OSTI ID: 1454611
Report Number(s):
LA-UR-15-21495
Journal Information:
Analytical Chemistry, Vol. 87, Issue 8; ISSN 0003-2700
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

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Cited By (2)

Comparison of morphologies of a uranyl peroxide precursor and calcination products journal January 2016
Energetics of hydration on uranium oxide and peroxide surfaces journal June 2019

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