Uranium(VI) sorption on iron oxides in Hanford Site sediment: Application of a surface complexation model

• Published in: Applied geochemistry 2008-09, Vol.23 (9), p.2649-2657
• Main Authors: Um, Wooyong, Serne, R. Jeffrey, Brown, Christopher F., Rod, Kenton A.
• Format: Article
• Language: English
• Subjects: Earth sciences; Earth, ocean, space; Engineering and environment geology. Geothermics; Exact sciences and technology; Freshwater; Geochemistry; GEOSCIENCES; HANFORD RESERVATION; Hanford Site; IRON OXIDES; MATHEMATICAL MODELS; NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Pollution, environment geology; remediation; SAND; SEDIMENTS; SORPTION; SORPTIVE PROPERTIES; surface complexation model; transport; URANIUM
• ISSN: 0883-2927; 1872-9134
• DOI: 10.1016/j.apgeochem.2008.05.013

Sorption of U(VI) on Hanford fine sand (HFS) with varying Fe-oxide (especially ferrihydrite) contents showed that U(VI) sorption increased with the incremental addition of synthetic ferrihydrite into HFS, consistent with ferrihydrite being one of the most reactive U(VI) sorbents present in natural sediments. Surface complexation model (SCM) calculations for U(VI) sorption, using only U(VI) surface-reaction constants obtained from U(VI) sorption data on freshly synthesized ferrihydrite at different pHs, were similar to the measured U(VI) sorption results on pure synthetic ferrihydrite and on HFS with high contents of ferrihydrite (5 wt%) added. However, the SCM prediction using only U(VI) sorption reactions and constants for synthetic ferrihydrite overestimated U(VI) sorption on the natural HFS or HFS with addition of low amounts of added ferrihydrite (1 wt% added). Over-predicted U(VI) sorption was attributed to reduced reactivity of natural ferrihydrite present in Hanford Site sediments, compared to freshly prepared synthetic ferrihydrite. Even though the SCM general composite (GC) approach is considered to be a semi-quantitative estimation technique for contaminant sorption, which requires systematic experimental data on the sorbent–sorbate system being studied to obtain credible SCM parameters, the general composite SCM model was still found to be a useful technique for describing U(VI) sorption on natural sediments. Based on U(VI) batch sorption results, two simple U(VI) monodentate surface species, SO_UO 2HCO 3 and SO_UO 2OH on ferrihydrite and phyllosillicate in HFS, respectively, can be successfully used to describe U(VI) sorption onto Hanford Site sediment contacting varying geochemical solutions.