Thermodynamic Study of UO3(g), UO2(OH)2(g), UO2Cl2(g), and UO2F2(g)

Technical Report · Thu Nov 07 04:00:00 EST 2002

DOI:https://doi.org/10.2172/15002517· OSTI ID:15002517

Ebbinghaus, B B; Krikorian, O H; Fleming, D L

Using the transpiration method, the volatility of uranium oxide in the presence of oxygen and water vapor has been measured at temperatures ranging from 1173 to 1573 K and the volatility of uranium oxide in the presence of oxygen and chlorine has been measured at 1175 K. The major vapor species in the presence of oxygen and water vapor are found to be UO{sub 3}(g) and UO{sub 2}(0H){sub 2}(g). Third law treatment of the vaporization data yields {Delta}H{sub f}{sup o}(298) values of -790.52 {+-} 7.32 and -1199.94 {+-} 10.25 kJ/mol, respectively. The major vapor species in the presence of oxygen and chlorine is found to be UO{sub 2}Cl{sub 2}(g). Third law treatment of the vaporization data yields a {Delta}H{sub f}{sup o}(298) value of -1002.04 {+-} 3.26 kJ/mol. From an assessment of all the thermodynamic data available for UO{sub 3}(g), UO{sub 2}(OH){sub 2}(g), UO{sub 2}Cl{sub 2}(g), and UO{sub 2}F{sub 2}(g), the best {Delta}H{sub f{sup o}}(298) values for each of these species are calculated to be -796.74 {+-} 3.52, -1199.94 {+-} 10.25, -999.64 {+-} 2.40, and -1369.22 {+-} 2.87 kJ/mol, respectively. From these, the {Delta}H{sub f{sup o}} (298) values for UO{sub 2}ClOH(g), UO{sub 2}FOH(g), and UO{sub 2}FCl(g) are estimated to be -1099.79, -1284.58, and -1184.43 kJ/mol, respectively. The thermodynamic data for all the vapor species are then applied to conditions one might expect in a thermal oxidation processor for mixed waste to estimate the amount of uranium volatility.

• Research Organization: Lawrence Livermore National Lab., CA (US)
• Sponsoring Organization: US Department of Energy (US)
• DOE Contract Number: W-7405-ENG-48
• OSTI ID: 15002517
• Report Number(s): UCRL-ID-150979
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CHLORINE
EVAPORATION
OXIDATION
OXYGEN
THERMODYNAMICS
TRANSPIRATION
URANIUM
URANIUM OXIDES
VOLATILITY
WASTES
WATER VAPOR