Radiation Damage Effects in Chlorite Investigated Using Microfocus Synchrotron Techniques

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Bower , W R , Pearce , C I , Smith , A D , Pimblott , S M , Mosselmans , J F W & Pattrick , R A D 2019 , ' Radiation Damage Effects in Chlorite Investigated Using Microfocus Synchrotron Techniques ' , ACS Earth and Space Chemistry , vol. 3 , no. 4 , pp. 652-662 . https://doi.org/10.1021/acsearthspacechem.8b00205

Title: Radiation Damage Effects in Chlorite Investigated Using Microfocus Synchrotron Techniques
Author: Bower, William R.; Pearce, Carolyn I.; Smith, Andrew D.; Pimblott, Simon. M.; Mosselmans, J. Frederick W.; Pattrick, Richard A. D.
Contributor organization: Department of Chemistry
Date: 2019-04
Language: eng
Number of pages: 11
Belongs to series: ACS Earth and Space Chemistry
ISSN: 2472-3452
DOI: https://doi.org/10.1021/acsearthspacechem.8b00205
URI: http://hdl.handle.net/10138/322505
Abstract: A detailed understanding of the mechanisms and effects of radiation damage in phyllosilicate minerals is a necessary component of the evaluation of the safety case for a deep geological disposal facility (GDF) for radioactive waste. Structural and chemical changes induced by alpha-particle damage will affect the performance of these minerals as reactive barrier materials (both in the near and far-field) over time scales relevant to GDF integrity. In this study, two examples of chlorite group minerals have been irradiated at a-particle doses comparable to those predicted to be experienced by the clay buffer material surrounding high-level radioactive waste canisters. Crystallographic aberrations induced by the focused He-4(2+) ion beam are revealed via high-resolution, microfocus X-ray diffraction mapping. Interlayer collapse by up to 0.5 angstrom is prevalent across both macrocrystalline and microcrystalline samples, with the macrocrystalline specimen displaying a breakdown of the phyllosilicate structure into loosely connected, multioriented crystallites displaying variable lattice parameters. The damaged lattice parameters suggest a localized breakdown and collapse of the OH(- )rich, "brucite-like" interlayer. Microfocus Fe K-edge X-ray absorption spectroscopy illustrates this defect accumulation, manifest as a severe damping of the X-ray absorption edge. Subtle Fe2+/Fe3+ speciation changes are apparent across the damaged structures. A trend toward Fe reduction is evident at depth in the damaged structures at certain doses (8.76 X 10(15) alpha particles/cm(2)). Interestingly, this reductive trend does not increase with radiation dose; indeed, at the maximum dose (1.26 x 10(16) alpha particles/cm(2)) administered in this study, there is evidence for a slight increase in Fe binding energy, suggesting the development of a depth-dependent redox gradient concurrent with light ion damage. At the doses examined here, these damaged structures are likely highly reactive, as sorption capacity will, to an extent, be largely enhanced by lattice disruption and an increase in available "edge" sites.
Subject: 116 Chemical sciences
chlorite
radiation damage
α particles
geodisposal
bentonite
montmorillonite
synchrotron microfocus
Peer reviewed: Yes
Rights: cc_by
Usage restriction: openAccess
Self-archived version: publishedVersion


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