| Autor: |
Kinyon JS; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Villa-Aleman E; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Ciprian E; University of Notre Dame, Notre Dame, IN, 46556, USA., Hixon AE; University of Notre Dame, Notre Dame, IN, 46556, USA., Foley BJ; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Christian JH; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Darvin JR; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Dick DD; Savannah River National Laboratory, Aiken, SC, 29808, USA. Eliel.villa-aleman@srnl.doe.gov., Casella AJ; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Sweet LE; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Buck EC; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Heller FD; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Nicholas AD; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Nizinski CA; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA., Clark RA; Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA. |
| Abstrakt: |
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, PuF 4 · x H 2 O(s) (0.5 ≤ x ≤ 2) and PuF 4 ·2.5H 2 O(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, we measured the visible and shortwave infrared (SWIR) diffuse reflectance, Fourier transform infrared (FTIR), fluorescence and Raman spectra of PuF 4 (s) and PuF 4 · x H 2 O(s) to obtain a better electronic and vibrational fingerprint. Our work provides clear indication of the polymeric structure of anhydrous PuF 4 , consistent with the Raman spectrum of UF 4 (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. |
