Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of Radioanalytical and Nuclear Chemistry

A 30 year-old PuF4 sample consisting of brown powder (PuF4-b) and pink granules (PuF4-p) was analyzed. X-ray difraction shows the bulk is comprised of three compounds: PuF4, PuO2, and PuF4·1.6H2O. Broadening of PuF4 XRD peaks suggests possible a-damage. After annealing at 650 °C, crystalline PuF4 and PuO2 remain. Thermogravimetric analysis and diferential 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~90 and 300 °C. Exothermic annealing of the a-damage occurs in two stages: at 350–355 °C and at 555–558 °C. Hydrofuoric acid, fuorine and helium desorb during the frst exotherm. Above 700 °C, PuF4 reacts with PuO2, resulting in oxygen release and mass loss.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1818130
Report Number(s):
PNNL-SA-157080
Journal Information:
Journal of Radioanalytical and Nuclear Chemistry, Vol. 329, Issue 2
Country of Publication:
United States
Language:
English

References (43)

Radiation damage and annealing in plutonium tetrafluoride journal December 2017
Review of major plutonium pyrochemical technology journal July 1984
Thermodynamic properties and phase diagrams of fluoride salts for nuclear applications journal January 2009
The oxide chemistry of plutonium in molten fluorides and the free energy of formation of PuF3 and PuF4 journal March 1971
Electrochemical behavior of plutonium fluoride species in LiF-CaF2 eutectic melt journal April 2019
Hydration of plutonium oxide and process salts, NaCl, KCl, CaCl2, MgCl2: effect of calcination on residual water and rehydration journal November 2000
Moisture and surface area measurements of plutonium-bearing oxides journal December 2009
Radiation damage in nuclear materials journal March 1992
Energetics of radiation damage in natural zircon (ZrSiO4) journal July 1994
Quantification of actinide α-radiation damage in minerals and ceramics journal January 2007
Evolution of spent nuclear fuel in dry storage conditions for millennia and beyond journal August 2014
Characterization of radiation damage in ceramics: Old challenge new issues? journal April 2015
Self-Radiation Damage in Actinide Host Phases of Nuclear Waste Forms journal January 1984
Radionuclide Decay Effects on Waste Glass Corrosion journal January 1993
Radiation damage from long-term alpha particle bombardment of silicates – a microfocus XRD and Fe K -edge XANES study journal November 2015
Alpha-decay damage and aqueous durability of actinide host phases in natural systems journal February 2001
Radiation damage in Nacl journal November 1991
A new mechanism for radiation damage processes in alkali halides journal December 1999
New scenario for the accumulation and release of radiation damage in rock salt and related materials
  • den Hartog, H. W.; Vainshtein, D. I.; Dubinko, V. I.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 191, Issue 1-4 https://doi.org/10.1016/S0168-583X(02)00548-7
journal May 2002
Spectroscopic studies of .alpha.-induced radiation damage in divalent metal fluorides journal September 1982
Microscopic effects of self-radiation damage in 244 Cm-doped LuPO 4 crystals journal February 2001
Radiation damage effects of crystal journal March 2007
Seeing is believing: Visualization of He distribution in zircon and implications for thermal history reconstruction on single crystals journal February 2017
Characterization and modelling of helium bubbles in self-irradiated plutonium alloys journal February 2005
Probing He bubbles in naturally aged and annealed δ-Pu alloys using ultra-small-angle x-ray scattering journal January 2018
Helium diffusion in uranium and plutonium oxides journal February 2004
Zircon (U-Th)/He Thermochronometry journal January 2005
Apatite (U–Th)/He thermochronometry using a radiation damage accumulation and annealing model journal April 2009
Helium diffusion in natural zircon: Radiation damage, anisotropy, and the interpretation of zircon (U-Th)/He thermochronology journal March 2013
Influence of radiation damage on titanite He diffusion kinetics journal May 2017
Annealing kinetics of radiation damage in zircon journal March 2019
Zircon grain selection reveals (de)coupled metamictization, radiation damage, and He diffusivity journal June 2018
The preparation and some properties of plutonium fluorides journal January 1954
The hydrated tetrafluorides of uranium and plutonium journal January 1954
On the fluorination of plutonium dioxide by ammonium hydrogen fluoride journal March 2016
Synthesis of plutonium trifluoride by hydro-fluorination and novel thermodynamic data for the PuF3-LiF system journal May 2018
Halides Of The Actinide Elements book January 1960
Adsorption of Gases in Multimolecular Layers journal February 1938
TEM study of alpha-damaged plutonium and americium dioxides journal March 2015
A review of plutonium oxalate decomposition reactions and effects of decomposition temperature on the surface area of the plutonium dioxide product journal October 2015
The Chemical Thermodynamic Properties of Plutonium Compounds journal June 1967
Phase relations in the system LiF-PuF3 journal March 1961
Cerium tetrafluoride. II. The system cerium tetrafluoride-cerium trifluoride journal January 1965