Chemical durability and corrosion-induced microstructure evolution of compositionally complex titanate pyrochlore waste forms with uranium incorporation

Kun Yang; Keith Bryce; Tiankai Yao; Dong Zhao; Jie Lian

doi:10.1016/j.jeurceramsoc.2023.09.071

Chemical durability and corrosion-induced microstructure evolution of compositionally complex titanate pyrochlore waste forms with uranium incorporation

Kun Yang
, Keith Bryce
, Tiankai Yao
, Dong Zhao
, Jie Lian

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

Chemical durability of compositionally-complex rare-earth titanate pyrochlore solid solutions with or without uranium incorporation was investigated by semi-dynamic leaching testing. A Ti-enriched amorphous passivation film formed on the surface due to the surface alteration-reorganization mechanism with preferential release of the weakly oxygen-bonded rare earth elements. Elemental release was found to be strongly correlated with chemical disorder, with a negligible correlation with entropy. The release rate of the uranium gradually decreased with increasing numbers of components, implying a possibility of designing and optimizing waste form performance with enhanced chemical durability by controlling composition complexity and chemical disorder for effective nuclear waste management.

Original language	English
Pages (from-to)	1102-1114
Number of pages	13
Journal	Journal of the European Ceramic Society
Volume	44
Issue number	2
Early online date	Sep 27 2023
DOIs	https://doi.org/10.1016/j.jeurceramsoc.2023.09.071
State	Published - Feb 2024

Keywords

Chemical durability
Multicomponent pyrochlore
Nuclear wasteform
Passivation film

INL Publication Number

INL/JOU-23-72855
156597

Access to Document

10.1016/j.jeurceramsoc.2023.09.071

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title = "Chemical durability and corrosion-induced microstructure evolution of compositionally complex titanate pyrochlore waste forms with uranium incorporation",

abstract = "Chemical durability of compositionally-complex rare-earth titanate pyrochlore solid solutions with or without uranium incorporation was investigated by semi-dynamic leaching testing. A Ti-enriched amorphous passivation film formed on the surface due to the surface alteration-reorganization mechanism with preferential release of the weakly oxygen-bonded rare earth elements. Elemental release was found to be strongly correlated with chemical disorder, with a negligible correlation with entropy. The release rate of the uranium gradually decreased with increasing numbers of components, implying a possibility of designing and optimizing waste form performance with enhanced chemical durability by controlling composition complexity and chemical disorder for effective nuclear waste management.",

keywords = "Chemical durability, Multicomponent pyrochlore, Nuclear wasteform, Passivation film",

author = "Kun Yang and Keith Bryce and Tiankai Yao and Dong Zhao and Jie Lian",

note = "Funding Information: The synthesis of the multicomponent titanate pyrochlore solid solutions was supported by NSF under the Award DMREF-2119423 . The dissolution testing of the multicomponent pyrochlore solid solution was supported as part of the Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD), an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy , Office of Science, Basic Energy Sciences under Award DE-SC0016584 . The TEM characterization was supported by Laboratory Directed Research and Development (LDRD) ( 21A1050–075FP ) project of Idaho National Laboratory (INL) which is operated by U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07–05ID14517 . Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

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language = "English",

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AU - Bryce, Keith

AU - Yao, Tiankai

AU - Zhao, Dong

AU - Lian, Jie

N1 - Funding Information: The synthesis of the multicomponent titanate pyrochlore solid solutions was supported by NSF under the Award DMREF-2119423 . The dissolution testing of the multicomponent pyrochlore solid solution was supported as part of the Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD), an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy , Office of Science, Basic Energy Sciences under Award DE-SC0016584 . The TEM characterization was supported by Laboratory Directed Research and Development (LDRD) ( 21A1050–075FP ) project of Idaho National Laboratory (INL) which is operated by U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07–05ID14517 . Publisher Copyright: © 2023 Elsevier Ltd

PY - 2024/2

Y1 - 2024/2

N2 - Chemical durability of compositionally-complex rare-earth titanate pyrochlore solid solutions with or without uranium incorporation was investigated by semi-dynamic leaching testing. A Ti-enriched amorphous passivation film formed on the surface due to the surface alteration-reorganization mechanism with preferential release of the weakly oxygen-bonded rare earth elements. Elemental release was found to be strongly correlated with chemical disorder, with a negligible correlation with entropy. The release rate of the uranium gradually decreased with increasing numbers of components, implying a possibility of designing and optimizing waste form performance with enhanced chemical durability by controlling composition complexity and chemical disorder for effective nuclear waste management.

AB - Chemical durability of compositionally-complex rare-earth titanate pyrochlore solid solutions with or without uranium incorporation was investigated by semi-dynamic leaching testing. A Ti-enriched amorphous passivation film formed on the surface due to the surface alteration-reorganization mechanism with preferential release of the weakly oxygen-bonded rare earth elements. Elemental release was found to be strongly correlated with chemical disorder, with a negligible correlation with entropy. The release rate of the uranium gradually decreased with increasing numbers of components, implying a possibility of designing and optimizing waste form performance with enhanced chemical durability by controlling composition complexity and chemical disorder for effective nuclear waste management.

KW - Chemical durability

KW - Multicomponent pyrochlore

KW - Nuclear wasteform

KW - Passivation film

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ER -

Chemical durability and corrosion-induced microstructure evolution of compositionally complex titanate pyrochlore waste forms with uranium incorporation

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