Engineered mineralogical interfaces as radionuclide repositories

Effective capture of fugitive actinides and daughter radionuclides constitutes a major remediation challenge at legacy or nuclear accident sites globally. The ability of double-layered, anionic clay minerals known as hydrotalcites (HTC) to contemporaneously sequester a range of contaminants from sol...

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Main Authors: Douglas, Grant B., Reddy, Steven, Saxey, David, MacRae, C.M., Webster, N.A.S., Beeching, L.J.
Format: Journal Article
Language:English
Published: 2023
Online Access:http://hdl.handle.net/20.500.11937/92422
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author Douglas, Grant B.
Reddy, Steven
Saxey, David
MacRae, C.M.
Webster, N.A.S.
Beeching, L.J.
author_facet Douglas, Grant B.
Reddy, Steven
Saxey, David
MacRae, C.M.
Webster, N.A.S.
Beeching, L.J.
author_sort Douglas, Grant B.
building Curtin Institutional Repository
collection Online Access
description Effective capture of fugitive actinides and daughter radionuclides constitutes a major remediation challenge at legacy or nuclear accident sites globally. The ability of double-layered, anionic clay minerals known as hydrotalcites (HTC) to contemporaneously sequester a range of contaminants from solution offers a unique remedy. However, HTC do not provide a robust repository for actinide isolation over the long term. In this study, we formed HTC by in-situ precipitation in a barren lixiviant from a uranium mine and thermally transformed the resulting radionuclide-laden, nanoscale HTC. Atomic-scale forensic examination of the amorphized/recrystallised product reveals segregation of U to nanometre-wide mineral interfaces and the local formation of interface-hosted mineral grains. This U-phase is enriched in rare earth elements, a geochemical analogue of actinides such as Np and Pu, and represents a previously unreported radionuclide interfacial segregation. U-rich phases associated with the mineral interfaces record a U concentration factor of ~ 50,000 relative to the original solute demonstrating high extraction and concentration efficiencies. In addition, the co-existing host mineral suite of periclase, spinel-, and olivine-group minerals that equate to a lower mantle, high P–T mineral assemblage have geochemical and geotechnical properties suitable for disposal in a nuclear waste repository. Our results record the efficient sequestering of radionuclides from contaminated water and this novel, broad-spectrum, nanoscale HTC capture and concentration process constitutes a rapid solute decontamination pathway and solids containment option in perpetuity.
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spelling curtin-20.500.11937-924222023-06-29T06:38:20Z Engineered mineralogical interfaces as radionuclide repositories Douglas, Grant B. Reddy, Steven Saxey, David MacRae, C.M. Webster, N.A.S. Beeching, L.J. Effective capture of fugitive actinides and daughter radionuclides constitutes a major remediation challenge at legacy or nuclear accident sites globally. The ability of double-layered, anionic clay minerals known as hydrotalcites (HTC) to contemporaneously sequester a range of contaminants from solution offers a unique remedy. However, HTC do not provide a robust repository for actinide isolation over the long term. In this study, we formed HTC by in-situ precipitation in a barren lixiviant from a uranium mine and thermally transformed the resulting radionuclide-laden, nanoscale HTC. Atomic-scale forensic examination of the amorphized/recrystallised product reveals segregation of U to nanometre-wide mineral interfaces and the local formation of interface-hosted mineral grains. This U-phase is enriched in rare earth elements, a geochemical analogue of actinides such as Np and Pu, and represents a previously unreported radionuclide interfacial segregation. U-rich phases associated with the mineral interfaces record a U concentration factor of ~ 50,000 relative to the original solute demonstrating high extraction and concentration efficiencies. In addition, the co-existing host mineral suite of periclase, spinel-, and olivine-group minerals that equate to a lower mantle, high P–T mineral assemblage have geochemical and geotechnical properties suitable for disposal in a nuclear waste repository. Our results record the efficient sequestering of radionuclides from contaminated water and this novel, broad-spectrum, nanoscale HTC capture and concentration process constitutes a rapid solute decontamination pathway and solids containment option in perpetuity. 2023 Journal Article http://hdl.handle.net/20.500.11937/92422 10.1038/s41598-023-29171-1 eng http://creativecommons.org/licenses/by/4.0/ fulltext
spellingShingle Douglas, Grant B.
Reddy, Steven
Saxey, David
MacRae, C.M.
Webster, N.A.S.
Beeching, L.J.
Engineered mineralogical interfaces as radionuclide repositories
title Engineered mineralogical interfaces as radionuclide repositories
title_full Engineered mineralogical interfaces as radionuclide repositories
title_fullStr Engineered mineralogical interfaces as radionuclide repositories
title_full_unstemmed Engineered mineralogical interfaces as radionuclide repositories
title_short Engineered mineralogical interfaces as radionuclide repositories
title_sort engineered mineralogical interfaces as radionuclide repositories
url http://hdl.handle.net/20.500.11937/92422