TY - JOUR
T1 - Energetics of cation mixing in urania-ceria solid solutions with stoichiometric oxygen concentrations
AU - Hanken, Benjamin E.
AU - Shvareva, Tatiana Y.
AU - Grønbech-Jensen, Niels
AU - Stanek, Christopher R.
AU - Asta, Mark
AU - Navrotsky, Alexandra
N1 - Copyright:
Copyright 2012 Elsevier B.V., All rights reserved.
PY - 2012/4/28
Y1 - 2012/4/28
N2 - Cation mixing energetics in urania-ceria solid solutions with stoichiometric oxygen concentrations (U 1-yCe yO 2) have been measured by high-temperature oxide-melt drop-solution calorimetry. Measurements have been performed on eight samples with compositions spanning y = 0.119 to y = 0.815. The measured mixing enthalpies (ΔH mix) range from -0.6 ± 3.3 to 3.9 ± 3.0 kJ mol -1. These values are discussed in the context of results from atomistic modeling which take into consideration the possibility of charge transfer between uranium and cerium cations to form solid solutions with mixed charge states. A comparison between measured and calculated results for ΔH mix suggests that such charge transfer takes place to a limited extent in the most concentrated mixtures studied.
AB - Cation mixing energetics in urania-ceria solid solutions with stoichiometric oxygen concentrations (U 1-yCe yO 2) have been measured by high-temperature oxide-melt drop-solution calorimetry. Measurements have been performed on eight samples with compositions spanning y = 0.119 to y = 0.815. The measured mixing enthalpies (ΔH mix) range from -0.6 ± 3.3 to 3.9 ± 3.0 kJ mol -1. These values are discussed in the context of results from atomistic modeling which take into consideration the possibility of charge transfer between uranium and cerium cations to form solid solutions with mixed charge states. A comparison between measured and calculated results for ΔH mix suggests that such charge transfer takes place to a limited extent in the most concentrated mixtures studied.
UR - http://www.scopus.com/inward/record.url?scp=84859341998&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84859341998&partnerID=8YFLogxK
U2 - 10.1039/c2cp40295e
DO - 10.1039/c2cp40295e
M3 - Article
C2 - 22434034
AN - SCOPUS:84859341998
SN - 1463-9076
VL - 14
SP - 5680
EP - 5685
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 16
ER -