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Lee, Jeongmook,Kim, Jandee,Youn, Young-Sang,Liu, Nazhen,Kim, Jong-Goo,Ha, Yeong-Keong,Shoesmith, David W.,Kim, Jong-Yun ELSEVIER 2017 JOURNAL OF NUCLEAR MATERIALS Vol.486 No.-
<P><B>Abstract</B></P> <P>The U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2−x</SUB> solid solutions with y = 0.005, 0.01, 0.03, 0.05 and 0.1 were characterized by Raman spectroscopy to investigate the defect structure induced by oxygen vacancies. The oxygen deficiencies of solid solutions were estimated by the relation between the doping level and a lattice parameter calculated from X-ray diffraction patterns. Raman mode shifts to higher wavenumber with increasing doping level showed that crystal lattice disorder due to oxygen vacancies. The frequency shifts and relative ratio of Raman modes were enabled to be the indicator for composition, defect and oxygen vacancy of U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2−x</SUB> solid solutions.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Investigation of structural character of U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2−x</SUB> solid solutions. </LI> <LI> Defect structures in U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2−x</SUB> solid solutions were evaluated by Raman spectroscopy. </LI> <LI> Oxygen deficiency due to Gd content causes Raman band related to oxygen vacancy. </LI> </UL> </P>
Kim, Jandee,Lee, Jeongmook,Youn, Young-Sang,Liu, Nazhen,Kim, Jong-Goo,Ha, Yeong-Keong,Bae, Sang-Eun,Shoesmith, David W.,Kim, Jong-Yun Pergamon Press 2017 Electrochimica Acta Vol. No.
<P><B>Abstract</B></P> <P>The influence of Gd-doping level and oxygen stoichiometry on the structural properties and electrochemical reactivity of U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2±x</SUB> have been investigated. The stoichiometry of UO<SUB>2</SUB> matrices with different Gd contents was determined using the lattice parameter obtained by XRD. The extent of lattice contraction, defined by a contraction factor, was found to be dependent on the stoichiometry. The surface morphologies exhibited differences in grain size which varied with stoichiometry and its influence on the U atom diffusivity during fabrication. The differences in grain size and, hence, the density of grain boundaries was reflected in variations in electrical conductivity, with hyperstoichiometric specimens with a low number of boundaries, yielding an increase in conductivity with increasing Gd content. Cyclic voltammetry showed that a variation in Gd content had only a minor influence on the electrochemical reactivity of stoichiometric U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2</SUB>. By contrast, the reactivity of hypostoichiometric U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2−x</SUB> and hyperstoichiometric U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2+x</SUB> increased and decreased, respectively, with increasing Gd content. The formation of Gd-O<SUB>v</SUB> clusters in hyperstoichiometric U<SUB>1−y</SUB>Gd<SUB>y</SUB>O<SUB>2+x</SUB> has a more marked influence on reactivity than the accompanying changes in grain size and electrical conductivity.</P>
Influence of Gd Doping on the Structure and Electrochemical Behavior of UO<sub>2</sub>
Liu, Nazhen,Kim, Jandee,Lee, Jeongmook,Youn, Young-Sang,Kim, Jong-Goo,Kim, Jong-Yun,Noë,l, James J.,Shoesmith, David W. Elsevier 2017 ELECTROCHIMICA ACTA Vol.247 No.-
<P><B>Abstract</B></P> <P>A series of (U<SUB>1−<I>y</I> </SUB>Gd<I> <SUB>y</SUB> </I>)O<SUB>2</SUB> materials (<I>y</I> =0, 0.01, 0.03, 0.05, 0.07 and 0.10) were characterized by X-ray diffractometry and Raman spectroscopy to determine the influence of Gd<SUP>III</SUP> doping on the structure of (U<SUB>1−<I>y</I> </SUB>Gd<I> <SUB>y</SUB> </I>)O<SUB>2</SUB> solid solutions. The XRD results show that, while the fluorite structure is maintained, Gd doping up to 10% leads to a contraction of the fluorite lattice. Raman spectroscopy shows Gd<SUP>III</SUP> doping distorts the fluorite lattice structure due to the formation of oxygen vacancies (O<SUB>v</SUB>) and, possibly, MO<SUB>8</SUB>-type complexes, as a consequence of the differences in both the oxidation state and the ionic radius of Gd<SUP>3+</SUP> compared to that of the U<SUP>4+</SUP>. The influence of Gd doping on the electrochemical reactivity of the (U<SUB>1−<I>y</I> </SUB>Gd<I> <SUB>y</SUB> </I>)O<SUB>2</SUB> specimens was shown to be minor, possibly due to a competition between the increase in the number of O<SUB>v</SUB> and the contraction of the lattice.</P>