Probing disorder in pyrochlore oxides using in situ synchrotron diffraction from levitated solids–A thermodynamic perspective

Maram, Pardha S.; Ushakov, Sergey V.; Weber, Richard J.  K.; Benmore, Chris J.; Navrotsky, Alexandra

doi:10.1038/s41598-018-28877-x

Title: Probing disorder in pyrochlore oxides using in situ synchrotron diffraction from levitated solids–A thermodynamic perspective

Journal Article · 13 July 2018 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-018-28877-x · OSTI ID:1459466

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^[1]; Weber, Richard J. K. ^[2]; Benmore, Chris J. ^[3];

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Univ. of California, Davis, CA (United States). Peter A. Rock Thermochemistry Lab. and NEAT ORU
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division; Materials Development, Inc., Arlington Heights, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division

Pyrochlore, an ordered derivative of the defect fluorite structure, shows complex disordering behavior as a function of composition, temperature, pressure, and radiation damage. We propose a thermodynamic model to calculate the disordering enthalpies for several RE₂Zr₂O₇ (RE = Sm, Eu, Gd) pyrochlores from experimental site distribution data obtained by in situ high temperature synchrotron X-ray diffraction. Site occupancies show a gradual increase in disorder on both cation and anion sublattices with increasing temperature and even greater disorder is achieved close to the phase transition to defect fluorite. The enthalpy associated with cation disorder depends on the radius of the rare earth ion, while the enthalpy of oxygen disordering is relatively constant for different compositions. The experimental data support trends predicted by ab initio calculations, but the obtained enthalpies of disordering are less endothermic than the predicted values. Thermal expansion coefficients are in the range (8.6-10.8) x 10^-6 K^-1. These new experimental determinations of defect formation energies are important for understanding the stability of pyrochlore oxides and their disordering mechanisms, which are essential in the context of their potential applications in nuclear waste management and other technologies.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1459466

Alternate ID(s):: OSTI ID: 1480857

Journal Information:: Scientific Reports, Vol. 8, Issue 1; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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