Chemistry, microstructure, and alpha decay damage of natural brannerite

dc.contributor.authorLumpkin, GRen_AU
dc.contributor.authorLeung, SHFen_AU
dc.contributor.authorFerenczy, Jen_AU
dc.date.accessioned2022-11-04T03:12:47Zen_AU
dc.date.available2022-11-04T03:12:47Zen_AU
dc.date.issued2012-01-06en_AU
dc.date.statistics2022-10-20en_AU
dc.description.abstractTo investigate the long-term stability of brannerite with respect to alpha decay damage and interaction with aqueous fluids, we have undertaken a study of twelve natural samples from a range of geological environments. Our results indicate that seven of the samples exhibit only minor alteration, usually located within veinlets or around the rim of the sample. The remaining five samples consist of variable amounts of unaltered and altered brannerite. Based on a total of 3 metal cations, the Ti and U contents of unaltered brannerite range from 1.8 to 2.1 and 0.4 to 0.9 atoms per formula unit (apfu), respectively. Maximum amounts of the other major cations on the A-site are 0.48 Ca, 0.22 Th, 0.14 Y, and 0.07 Ln (lanthanide = Ce, Nd, Gd, Sm) atoms pfu. Maximum values of other cations on the B-site are 0.15 Fe, 0.14 Si, 0.09 Al, 0.06 Nb, 0.04 Mn, and 0.04 Ni atoms pfu. Altered regions of brannerite contain significant amounts of Si and other elements incorporated from an aqueous fluid phase, and up to 40–90% of the original amount of U has been lost as a result of alteration. SEM-EDX results also provide evidence for TiO2 phases, galena, and a thorite-like phase as alteration products. Electron diffraction patterns of all samples typically consist of two broad, diffuse rings that have equivalent d-spacings of 0.31 nm and 0.19 nm, indicating that brannerite is rendered completely amorphous by alpha decay damage. Many of the grains also exhibit weak diffraction spots due to fine-grained inclusions of a uranium oxide phase and galena. Using the available age data, these samples have accumulated alpha decay doses in the range of 0.7–200 × 1016 α mg−1. Although imprecise, the U–Th–Pb chemical ages determined by microanalysis are generally consistent with the known ages and geological histories of the brannerite host rocks. To a first approximation, it is possible to understand the results of chemical and isotopic dating of brannerite by treating each sample as a complex system composed of nominally unaltered, altered, and recrystallised areas. The dominant effects are U loss from altered areas and Pb loss from unaltered brannerite and, to a lesser extent, altered brannerite, the structure of which approximates to a Ti–Si–O glass-like network wherein Pb is more comfortable as a network modifier. Crown Copyright © 2011 Published by Elsevieren_AU
dc.description.sponsorshipThis work was performed at the Australian Nuclear Science and Technology Organisation, partly funded under contract with Lawrence Livermore National Laboratory as part of the Plutonium Immobilization Project.en_AU
dc.identifier.citationLumpkin, G. R., Leung, S. H. F., & Ferenczy, J. (2012). Chemistry, microstructure, and alpha decay damage of natural brannerite. Chemical Geology, 291, 55-68. doi:10.1016/j.chemgeo.2011.09.008en_AU
dc.identifier.issn0009-2541en_AU
dc.identifier.journaltitleChemical Geologyen_AU
dc.identifier.pagination55-68en_AU
dc.identifier.urihttps://doi.org/10.1016/j.chemgeo.2011.09.008en_AU
dc.identifier.urihttps://apo.ansto.gov.au/dspace/handle/10238/13984en_AU
dc.identifier.volume291en_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.subjectAlpha decayen_AU
dc.subjectPegmatitesen_AU
dc.subjectBranneriteen_AU
dc.subjectSouth Australiaen_AU
dc.subjectGeochemistryen_AU
dc.subjectAge estimationen_AU
dc.subjectMicrostructureen_AU
dc.titleChemistry, microstructure, and alpha decay damage of natural branneriteen_AU
dc.typeJournal Articleen_AU
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