X-ray diffraction, differential scanning calorimetry and evolved gas analysis of aged plutonium tetrafluoride (PuF4)

被引:3
|
作者
Wayne, David M. [1 ]
Stritzinger, Jared T. [2 ]
Casella, Amanda J. [3 ]
Sweet, Lucas E. [3 ]
Corbey, Jordan F. [3 ]
Garcia, Daniel J. [2 ,6 ]
Wylie, E. Miller [4 ]
Tandon, Lav [5 ]
Olson, Angela C. [4 ]
Rim, Jung Ho [4 ]
机构
[1] Alamos Natl Lab, Mat Sci & Technol, Nucl Mat Sci, MST16,MS E574, Los Alamos, NM 87545 USA
[2] Alamos Natl Lab, Actinide Mat Proc & Power, AMPP3, MS E511, Los Alamos, NM 87545 USA
[3] Pacific Northwest Natl Lab, Nucl & Radiochem Team, POB 999, Richland, WA 99352 USA
[4] Alamos Natl Lab, Actinide Analyt Chem, CAAC, MS E554, Los Alamos, NM 87545 USA
[5] Alamos Natl Lab, Met Prod, PT1, MS E551, Los Alamos, NM 87545 USA
[6] Alamos Natl Lab, Training & Miss Serv, ORI1, MS E523, Los Alamos, NM 87545 USA
关键词
Plutonium tetrafluoride; Differential scanning calorimetry; Thermal analysis; Evolved gas analysis; Annealing; Radiation damage; RADIATION-DAMAGE; THERMODYNAMIC PROPERTIES; ACCUMULATION; FLUORINATION; DIFFUSION; DIOXIDE; SALTS; OXIDE;
D O I
10.1007/s10967-021-07810-z
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
A 30 year-old PuF4 sample consisting of brown powder (PuF4-b) and pink granules (PuF4-p) was analyzed. X-ray diffraction shows the bulk is comprised of three compounds: PuF4, -PuO2, and -PuF4 center dot 1.6H(2)O. Broadening of PuF4 XRD peaks suggests possible a-damage. After annealing at 650 degrees C, crystalline PuF4 and PuO2 remain. Thermogravimetric analysis and differential scanning calorimetry-with simultaneous evolved gas analysis- of the separated PuF4-p and PuF4-b components reveal a distinct sequence of reactions. Dehydration occurs between similar to 90 and 300 degrees C. Exothermic annealing of the a-damage occurs in two stages: at 350-355 degrees C and at 555-558 degrees C. Hydrofluoric acid, fluorine and helium desorb during the first exotherm. Above 700 degrees C, PuF4 reacts with -PuO2, resulting in oxygen release and mass loss.
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页码:741 / 756
页数:16
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