1. High temperature heat capacity of (U, Am)O2±x
- Author
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Christine Guéneau, O.S. Vălu, Florent Lebreton, R.J.M. Konings, Philippe Martin, Ondřej Beneš, J. Zappey, E. Epifano, Département de recherche sur les procédés pour la mine et le recyclage du combustible (DMRC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Service de Chimie Physique (SCP), Département de Physico-Chimie (DPC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, JRC Institute for Transuranium Elements [Karlsruhe] (ITU ), and European Commission - Joint Research Centre [Karlsruhe] (JRC)
- Subjects
Nuclear and High Energy Physics ,Standard enthalpy of reaction ,Enthalpy ,chemistry.chemical_element ,Thermodynamics ,Americium ,[CHIM.MATE]Chemical Sciences/Material chemistry ,02 engineering and technology ,Calorimetry ,Atmospheric temperature range ,021001 nanoscience & nanotechnology ,01 natural sciences ,7. Clean energy ,Heat capacity ,010305 fluids & plasmas ,Enthalpy change of solution ,Nuclear Energy and Engineering ,chemistry ,0103 physical sciences ,[CHIM.CRIS]Chemical Sciences/Cristallography ,[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] ,General Materials Science ,0210 nano-technology ,CALPHAD ,ComputingMilieux_MISCELLANEOUS - Abstract
Mixed uranium and americium dioxides (U, Am)O 2±x are candidates as possible transmutation targets for generation IV reactors. In this work, the enthalpy increments of this solid solution were measured in the 470–1750 K temperature range by drop calorimetry for Am/(Am + U) ratios equal to 0.32, 0.39, 0.49, 0.58 and 0.68. Then, the heat capacity functions were obtained by derivation of the enthalpy data. The results of this work were compared to the heat capacity and enthalpy functions reported in the literature for the UO 2 [1] and AmO 2 [2] binary oxides and for the U 0.9 Am 0.1 O 2±x , U 0.8 Am 0.2 O 2±x mixed oxides [3]. From the obtained trend, it was found out that an excess contribution to the enthalpy increment appears for T > 1100 K in the compositions with Am/(Am + U)≥0.4 and a possible explanation attributing this effect to oxygen hypostoichiometry is provided. Finally, to verify the hypothesis, thermodynamic computations based on the CALPHAD method were performed for AmO 2-x under air and the results confirmed that the source of the excess contribution is the formation of oxygen vacancies.
- Published
- 2017
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