Influence of dissolved silicate on rates of Fe(II) oxidation

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dc.contributor.authorKinsela, ASen_AU
dc.contributor.authorJones, AMen_AU
dc.contributor.authorBligh, MWen_AU
dc.contributor.authorPham, ANen_AU
dc.contributor.authorCollins, RNen_AU
dc.contributor.authorHarrison, JJen_AU
dc.contributor.authorWilsher, KLen_AU
dc.contributor.authorPayne, TEen_AU
dc.contributor.authorWaite, TDen_AU
dc.date.accessioned2023-01-12T00:16:13Zen_AU
dc.date.available2023-01-12T00:16:13Zen_AU
dc.date.issued2016-10-05en_AU
dc.date.statistics2022-11-03en_AU
dc.descriptionThis is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.en_AU
dc.description.abstractIncreasing concentrations of dissolved silicate progressively retard Fe(II) oxidation kinetics in the circum-neutral pH range 6.0–7.0. As Si:Fe molar ratios increase from 0 to 2, the primary Fe(III) oxidation product transitions from lepidocrocite to a ferrihydrite/silica-ferrihydrite composite. Empirical results, supported by chemical kinetic modeling, indicated that the decreased heterogeneous oxidation rate was not due to differences in absolute Fe(II) sorption between the two solids types or competition for adsorption sites in the presence of silicate. Rather, competitive desorption experiments suggest Fe(II) was associated with more weakly bound, outer-sphere complexes on silica-ferrihydrite compared to lepidocrocite. A reduction in extent of inner-sphere Fe(II) complexation on silica-ferrihydrite confers a decreased ability for Fe(II) to undergo surface-induced hydrolysis via electronic configuration alterations, thereby inhibiting the heterogeneous Fe(II) oxidation mechanism. Water samples from a legacy radioactive waste site (Little Forest, Australia) were shown to exhibit a similar pattern of Fe(II) oxidation retardation derived from elevated silicate concentrations. These findings have important implications for contaminant migration at this site as well as a variety of other groundwater/high silicate containing natural and engineered sites that might undergo iron redox fluctuations. © 2016 American Chemical Societyen_AU
dc.identifier.citationKinsela, A. S., Jones, A. M., Bligh, M. W., Pham, A. N., Collins, R. N., Harrison, J. J., Wilsher, K. L., Payne, T. E. & Waite, T. D. (2016). Influence of dissolved silicate on rates of Fe (II) oxidation. Environmental Science & Technology, 50(21), 11663-11671. doi:10.1021/acs.est.6b03015en_AU
dc.identifier.issn1520-5851en_AU
dc.identifier.issue21en_AU
dc.identifier.journaltitleEnvironmental Science & Technologyen_AU
dc.identifier.pagination11663-11671en_AU
dc.identifier.urihttps://doi.org/10.1021/acs.est.6b03015en_AU
dc.identifier.urihttps://apo.ansto.gov.au/dspace/handle/10238/14315en_AU
dc.identifier.volume50en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectAdsorptionen_AU
dc.subjectOxidationen_AU
dc.subjectOxidesen_AU
dc.subjectSilicatesen_AU
dc.subjectIronen_AU
dc.subjectKineticsen_AU
dc.titleInfluence of dissolved silicate on rates of Fe(II) oxidationen_AU
dc.typeJournal Articleen_AU
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