Insights into dynamic processes of cations in pyrochlores and other complex oxides

Uberuaga, Blas Pedro; Perriot, Romain

doi:10.1039/c5cp03372a

Title: Insights into dynamic processes of cations in pyrochlores and other complex oxides

Journal Article · Wed Aug 26 00:00:00 EDT 2015 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c5cp03372a· OSTI ID:1221616

Uberuaga, Blas Pedro ^[1]; Perriot, Romain ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Complex oxides are critical components of many key technologies, from solid oxide fuel cells and superionics to inert matrix fuels and nuclear waste forms. In many cases, understanding mass transport is important for predicting performance and, thus, extensive effort has been devoted to understanding mass transport in these materials. However, most work has focused on the behavior of oxygen while cation transport has received relatively little attention, even though cation diffusion is responsible for many phenomena, including sintering, radiation damage evolution, and deformation processes. Here, we use accelerated molecular dynamics simulations to examine the kinetics of cation defects in one class of complex oxides, A₂B₂O₇ pyrochlore. In some pyrochlore chemistries, B cation defects are kinetically unstable, transforming to A cation defects and antisites at rates faster than they can diffuse. When this occurs, transport of B cations occurs through defect processes on the A sublattice. Further, these A cation defects, either interstitials or vacancies, can interact with antisite disorder, reordering the material locally, though this process is much more efficient for interstitials than vacancies. Whether this behavior occurs in a given pyrochlore depends on the A and B chemistry. Pyrochlores with a smaller ratio of cation radii exhibit this complex behavior, while those with larger ratios exhibit direct migration of B interstitials. Similar behavior has been reported in other complex oxides such as spinels and perovskites, suggesting that this coupling of transport between the A and B cation sublattices, while not universal, occurs in many complex oxide.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

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

Grant/Contract Number:: 2013LANL8400; AC52-06NA25396

OSTI ID:: 1221616

Report Number(s):: LA-UR-15-24397; PPCPFQ

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 17, Issue 37; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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Disorder-induced transition from grain boundary to bulk dominated ionic diffusion in pyrochlores Perriot, Romain; Dholabhai, Pratik P.; Uberuaga, Blas P. Nanoscale, Vol. 9, Issue 20 https://doi.org/10.1039/c7nr01373f	journal	January 2017
Insights into the fabrication and structure of plutonium pyrochlores Finkeldei, S.; Stennett, M. C.; Kowalski, P. M. Journal of Materials Chemistry A, Vol. 8, Issue 5 https://doi.org/10.1039/c9ta05795a	journal	January 2020
Evidence for percolation diffusion of cations and material recovery in disordered pyrochlore from accelerated molecular dynamics simulations Perriot, Romain; Uberuaga, Blas P.; Zamora, Richard J. arXiv https://doi.org/10.48550/arxiv.1607.07101	text	January 2016

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