First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2

Details First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2 First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2

2010-12-09

arxiv.org/abs/1012.1905v1

Physics

Condensed Matter

Materials Science

8 pages, 6 figures

Scientific paper

10.1103/PhysRevB.84.085131

The formalism of electronic density-functional-theory, with Hubbard-U corrections (DFT+U), is employed in a computational study of the energetics of U_{1-x} Ce_x O_2 mixtures. The computational approach makes use of a procedure which facilitates convergence of the calculations to multiple self-consistent DFT+U solutions for a given cation arrangement, corresponding to different charge states for the U and Ce ions in several prototypical cation arrangements. Results indicate a significant dependence of the structural and energetic properties on the nature of both charge and cation ordering. With the effective Hubbard-U parameters that reproduce well the measured oxidation-reduction energies for urania and ceria, we find that charge transfer between U(IV) and Ce(IV) ions, leading to the formation of U(V) and Ce(III), gives rise to an increase in the mixing energy in the range of 4-14 kJ/mol of formula unit, depending on the nature of the cation ordering. The results suggest that although charge transfer between uranium and cerium ions is disfavored energetically, it is likely to be entropically stabilized at the high temperatures relevant to the processing and service of urania-based solid solutions.

Affiliated with

Also associated with

No associations

Rating

First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2 does not yet have a rating. At this time, there are no reviews or comments for this scientific paper.

If you have personal experience with First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2, we encourage you to share that experience with our LandOfFree.com community. Your opinion is very important and First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2 will most certainly appreciate the feedback.

Rate now

Comments { 0 }

Profile ID: LFWR-SCP-O-76429