Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions

Abstract Non-ideal thermodynamics of solid solutions can greatly impact materials degradation behavior. We have investigated an actinide silicate solid solution system (USiO4–ThSiO4), demonstrating that thermodynamic non-ideality follows a distinctive, atomic-scale disordering process, which is usua...

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Autores principales:	J. Marcial, Y. Zhang, X. Zhao, H. Xu, A. Mesbah, E. T. Nienhuis, S. Szenknect, J. C. Neuefeind, J. Lin, L. Qi, A. A. Migdisov, R. C. Ewing, N. Dacheux, J. S. McCloy, X. Guo
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Materials of engineering and construction. Mechanics of materials TA401-492
Acceso en línea:	https://doaj.org/article/92aa8949682b40bbac3d6d8693d80fc1
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spelling	oai:doaj.org-article:92aa8949682b40bbac3d6d8693d80fc12021-12-02T16:04:26ZThermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions10.1038/s41529-021-00179-02397-2106https://doaj.org/article/92aa8949682b40bbac3d6d8693d80fc12021-06-01T00:00:00Zhttps://doi.org/10.1038/s41529-021-00179-0https://doaj.org/toc/2397-2106Abstract Non-ideal thermodynamics of solid solutions can greatly impact materials degradation behavior. We have investigated an actinide silicate solid solution system (USiO4–ThSiO4), demonstrating that thermodynamic non-ideality follows a distinctive, atomic-scale disordering process, which is usually considered as a random distribution. Neutron total scattering implemented by pair distribution function analysis confirmed a random distribution model for U and Th in first three coordination shells; however, a machine-learning algorithm suggested heterogeneous U and Th clusters at nanoscale (~2 nm). The local disorder and nanosized heterogeneous is an example of the non-ideality of mixing that has an electronic origin. Partial covalency from the U/Th 5f–O 2p hybridization promotes electron transfer during mixing and leads to local polyhedral distortions. The electronic origin accounts for the strong non-ideality in thermodynamic parameters that extends the stability field of the actinide silicates in nature and under typical nuclear waste repository conditions.J. MarcialY. ZhangX. ZhaoH. XuA. MesbahE. T. NienhuisS. SzenknectJ. C. NeuefeindJ. LinL. QiA. A. MigdisovR. C. EwingN. DacheuxJ. S. McCloyX. GuoNature PortfolioarticleMaterials of engineering and construction. Mechanics of materialsTA401-492ENnpj Materials Degradation, Vol 5, Iss 1, Pp 1-14 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Materials of engineering and construction. Mechanics of materials TA401-492
spellingShingle	Materials of engineering and construction. Mechanics of materials TA401-492 J. Marcial Y. Zhang X. Zhao H. Xu A. Mesbah E. T. Nienhuis S. Szenknect J. C. Neuefeind J. Lin L. Qi A. A. Migdisov R. C. Ewing N. Dacheux J. S. McCloy X. Guo Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
description	Abstract Non-ideal thermodynamics of solid solutions can greatly impact materials degradation behavior. We have investigated an actinide silicate solid solution system (USiO4–ThSiO4), demonstrating that thermodynamic non-ideality follows a distinctive, atomic-scale disordering process, which is usually considered as a random distribution. Neutron total scattering implemented by pair distribution function analysis confirmed a random distribution model for U and Th in first three coordination shells; however, a machine-learning algorithm suggested heterogeneous U and Th clusters at nanoscale (~2 nm). The local disorder and nanosized heterogeneous is an example of the non-ideality of mixing that has an electronic origin. Partial covalency from the U/Th 5f–O 2p hybridization promotes electron transfer during mixing and leads to local polyhedral distortions. The electronic origin accounts for the strong non-ideality in thermodynamic parameters that extends the stability field of the actinide silicates in nature and under typical nuclear waste repository conditions.
format	article
author	J. Marcial Y. Zhang X. Zhao H. Xu A. Mesbah E. T. Nienhuis S. Szenknect J. C. Neuefeind J. Lin L. Qi A. A. Migdisov R. C. Ewing N. Dacheux J. S. McCloy X. Guo
author_facet	J. Marcial Y. Zhang X. Zhao H. Xu A. Mesbah E. T. Nienhuis S. Szenknect J. C. Neuefeind J. Lin L. Qi A. A. Migdisov R. C. Ewing N. Dacheux J. S. McCloy X. Guo
author_sort	J. Marcial
title	Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
title_short	Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
title_full	Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
title_fullStr	Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
title_full_unstemmed	Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
title_sort	thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/92aa8949682b40bbac3d6d8693d80fc1
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_version_	1718385220363747328

Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions

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