Emerging investigator series: a holistic approach to multicomponent EXAFS: Sr and Cs complexation in clayey soils

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dc.contributor.authorBots, Pen_AU
dc.contributor.authorComarmond, MJen_AU
dc.contributor.authorPayne, TEen_AU
dc.contributor.authorGückel, Ken_AU
dc.contributor.authorLunn, RJen_AU
dc.contributor.authorRizzo, Len_AU
dc.contributor.authorSchellenger, AEPen_AU
dc.contributor.authorRenshaw, JCen_AU
dc.date.accessioned2024-10-03T23:31:30Zen_AU
dc.date.available2024-10-03T23:31:30Zen_AU
dc.date.issued2021-06-21en_AU
dc.date.statistics2024-05-09en_AU
dc.description.abstractStrontium and caesium are fission products of concern at many nuclear legacy sites and Cs is additionally a significant consideration at sites in the aftermath of nuclear accidents and incidents. Such sites require long-term management to minimize the risk of such contaminants to the environment and the public. Understanding the geochemical speciation of Sr and Cs in situ in the soils and groundwater is essential to develop engineered management strategies. Here we developed and utilized a comprehensive approach to fitting the EXAFS of Sr and Cs adsorption to single mineral phases and a composite clayey soil. First, a shell-by-shell fitting strategy enabled us to determine that Sr surface complexes involve the formation of bidentate edge sharing complexes with anatase and illite-smectite, and form at the silicon vacancy sites at the kaolinite basal surfaces. Cs surface complexes form at the silicon vacancy sites at the illite-smectite and kaolinite basal surfaces. Second, using a subsequent holistic approach we determined the predominance of these complexes within a composite clayey soil. Sr was dominated by complexation with illite-smectite (72–76%) and to a lesser extent with kaolinite (25–30%) with negligible complexation with anatase, while Cs complexed roughly equally to both illite-smectite and kaolinite. The presented approach to fitting EXAFS spectra will strengthen predictive modelling on the behaviour of elements of interest. For example, the details on Sr and Cs speciation will enable predictive modelling to characterise their long-term behaviour and the design and validation of evidence-based engineering options for long-term management of nuclear legacy sites. © Royal Society of Chemistry 2024 - Open Access CC-BYen_AU
dc.description.sponsorshipWe would like to acknowledge Diamond Light Source for awarding us with XAS beamtime at the Core XAS beamline (B18) under grant number: SP17114 and Dr Gianantonio Cibin for his assistance during XAS beamtime. We would also like to acknowledge the EPSRC ICASE award: EP/L505663/1 with financial support from the Nuclear Decommissioning Authority to support L. Rizzo and the EPSRC funded DISTINCTIVE consortium: EP/L014041/1. Finally, we thank Sangeeth Thiruvoth for assistance with tracer stock preparations, Lida Mokhber Shahin and Jennifer Harrison for their assistance with the radiochemical analyses, Jennifer Harrison and Pichamon Sarakan for their assistance with the adsorption experiments to ‘CH30 1.0–1.2 m’, Henri Wong for the ICP-AES analyses, Dr Dioni Cendón for the mineralogical assessment of the CH30 sample, and Dr Vinzenz Brendler for the preliminary discussions on the adsorption of radionuclides to clay minerals and requirements for potential surface complexation modelling.en_AU
dc.format.mediumPrint-Electronicen_AU
dc.identifier.citationBots, P., Comarmond, M. J., Payne, T. E., Gückel, K., Lunn, R. J., Rizzo, L., Schellenger, A. E. P., & Renshaw, J. C. (2021). Emerging investigator series: a holistic approach to multicomponent EXAFS: Sr and Cs complexation in clayey soils. Environmental Science: Processes & Impacts, 23(8), 1101-1115. doi:10.1039/D1EM00121Cen_AU
dc.identifier.issn2050-7887en_AU
dc.identifier.issn2050-7895en_AU
dc.identifier.issue8en_AU
dc.identifier.journaltitleEnvironmental Science Processes & Impactsen_AU
dc.identifier.pagination1101-1115en_AU
dc.identifier.urihttps://doi.org/10.1039/d1em00121cen_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15724en_AU
dc.identifier.volume23en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherRoyal Society of Chemistryen_AU
dc.subjectChromiumen_AU
dc.subjectStrontiumen_AU
dc.subjectSoilsen_AU
dc.subjectGround wateren_AU
dc.subjectNuclear materials managementen_AU
dc.subjectGeochemical surveysen_AU
dc.titleEmerging investigator series: a holistic approach to multicomponent EXAFS: Sr and Cs complexation in clayey soilsen_AU
dc.typeJournal Articleen_AU
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