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000848119 0247_ $$2doi$$a10.1021/acs.inorgchem.8b00463
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000848119 1001_ $$0P:(DE-HGF)0$$aMurphy, Gabriel L.$$b0
000848119 245__ $$aUnexpected Crystallographic Phase Transformation in Nonstoichiometric SrUO 4– x : Reversible Oxygen Defect Ordering and Symmetry Lowering with Increasing Temperature
000848119 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2018
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000848119 520__ $$aIn situ synchrotron powder X-ray diffraction measurements have demonstrated that SrUO4 undergoes a reversible phase transformation under reducing conditions at high temperatures, associated with the ordering of oxygen defects resulting in a lowering of crystallographic symmetry. When substoichiometric rhombohedral α-SrUO4–x, in space group R3̅m with disordered in-plane oxygen defects, is heated above 200 °C in a hydrogen atmosphere it undergoes a first order phase transformation to a (disordered) triclinic polymorph, δ-SrUO4–x, in space group P1̅. Continued heating to above 450 °C results in the appearance of superlattice reflections, due to oxygen-vacancy ordering forming an ordered structure δ-SrUO4–x. Cooling δ-SrUO4–x toward room temperature results in the reformation of the rhombohedral phase α-SrUO4–x with disordered defects, confirming the reversibility of the transformation. This suggests that the transformation, resulting from oxygen vacancy ordering, is not a consequence of sample reduction or decomposition, but rather represents a change in the energetics of the system. A strong reducing atmosphere is required to generate a critical amount of oxygen defects in α-SrUO4–x to enable the transformation to δ-SrUO4–x but once formed the transformation between these two phases can be induced by thermal cycling. The structure of δ-SrUO4–x at 1000 °C was determined using symmetry representation analysis, with the additional reflections indexed to a commensurate distortion vector k = ⟨1/4 1/4 3/4⟩. The ordered 2D layered triclinic structure of δ-SrUO4–x can be considered a structural distortion of the disordered 2D layered rhombohedral α-SrUO4–x structure through the preferential rearrangement of the in-plane oxygen vacancies. Ab initio calculations using density functional theory with self-consistently derived Hubbard U parameter support the assigned ordered defect superstructure model. Entropy changes associated with the temperature dependent short-range ordering of the reduced U species are believed to be important and these are discussed with respect to the results of the ab initio calculations.
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000848119 536__ $$0G:(DE-Juel1)jara0037_20181101$$aAtomistic modeling of radionuclide-bearing materials for safe management of high level nuclear waste. (jara0037_20181101)$$cjara0037_20181101$$fAtomistic modeling of radionuclide-bearing materials for safe management of high level nuclear waste.$$x1
000848119 536__ $$0G:(DE-Juel1)jara0038_20121101$$aInvestigation of the new materials for safe management of high level nuclear waste. (jara0038_20121101)$$cjara0038_20121101$$fInvestigation of the new materials for safe management of high level nuclear waste.$$x2
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000848119 7001_ $$0P:(DE-HGF)0$$aWang, Chun-Hai$$b1
000848119 7001_ $$0P:(DE-Juel1)156345$$aBeridze, George$$b2
000848119 7001_ $$0P:(DE-HGF)0$$aZhang, Zhaoming$$b3
000848119 7001_ $$0P:(DE-HGF)0$$aKimpton, Justin A.$$b4
000848119 7001_ $$00000-0003-2366-5809$$aAvdeev, Maxim$$b5
000848119 7001_ $$0P:(DE-Juel1)137024$$aKowalski, Piotr$$b6
000848119 7001_ $$00000-0002-7187-4579$$aKennedy, Brendan J.$$b7$$eCorresponding author
000848119 773__ $$0PERI:(DE-600)1484438-2$$a10.1021/acs.inorgchem.8b00463$$gVol. 57, no. 10, p. 5948 - 5958$$n10$$p5948 - 5958$$tInorganic chemistry$$v57$$x1520-510X$$y2018
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