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Chemical and spectroscopic characterization of plutonium tetrafluoride

Journal Article · · Dalton Transactions
DOI:https://doi.org/10.1039/d4dt02509a· OSTI ID:2500263
 [1];  [1];  [2];  [2];  [1];  [1];  [1];  [1];  [3];  [3];  [3];  [3];  [3];  [3];  [3]
  1. Savannah River National Laboratory (SRNL), Aiken, SC (United States)
  2. University of Notre Dame, IN (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Anhydrous plutonium tetrafluoride is an important intermediate in the production of metallic Pu. This historically important compound is also known to exist in at least two distinct, yet understudied hydrate forms, PuF4·xH2O(s) (0.5 ≤ x ≤ 2) and PuF4·2.5H2O(s). X-ray diffraction (XRD), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM) are the most common tools used to characterize these materials, often in a context for studying structural and morphological changes that arise from aging or calcination. However, fundamental electronic and vibrational spectroscopic information is rather scarce. Here, in this study, we measured the visible and shortwave infrared (SWIR) diffuse reflectance, Fourier transform infrared (FTIR), fluorescence and Raman spectra of PuF4(s) and PuF4·xH2O(s) to obtain a better electronic and vibrational fingerprint. Our work provides clear indication of the polymeric structure of anhydrous PuF4, consistent with the Raman spectrum of UF4(s) and its hydrates. This is supplemented with XRD, TGA and SEM analysis. Findings in this study indicate that the spectra are modified by particle size, which in turn is influenced by synthetic technique.

Research Organization:
Savannah River National Laboratory (SRNL), Aiken, SC (United States)
Sponsoring Organization:
USDOE Office of Environmental Management (EM); USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation
Grant/Contract Number:
89303321CEM000080
OSTI ID:
2500263
Alternate ID(s):
OSTI ID: 2475226
OSTI ID: 2552933
Report Number(s):
SRNL-STI--2024-00356-REV
Journal Information:
Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 48 Vol. 53; ISSN 1477-9226
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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