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Np(V) Retention at the Illite du Puy Surface

1 август 2023

Schacherl, B., Joseph, C., Beck, A., Lavrova, P., Schnurr, A., Dardenne, K., Geyer, F., Cherkezova-Zheleva, Z., Göttlicher, J., Geckeis, H., Vitova, T..
     ( Зара Черкезова-Желева; )

Abstract

In this study, Np­(V) retention on Illite du Puy (IdP) was investigated since it is essential for understanding the migration behavior of Np in argillaceous environments. The presence of structural Fe­(III) and Fe­(II) in IdP was confirmed by Fe K-edge X-ray absorption near-edge structure (XANES) and 57Fe Mössbauer spectroscopy. In batch sorption experiments, a higher Np sorption affinity to IdP was found than to Wyoming smectite or iron-free synthetic montmorillonite. An increase of the relative Np­(IV) ratio sorbed onto IdP with decreasing pH was observed by solvent extraction (up to (24 ± 2)% at pH 5, c0(Np) = 10–6 mol/L). Furthermore, up to (33 ± 5)% Np­(IV) could be detected in IdP diffusion samples at pH 5. Respective Np M5-edge high-energy resolution (HR-) XANES spectra suggested the presence of Np­(IV/V) mixtures and weakened axial bond covalency of the NpO2+ species sorbed onto IdP. Np L3-edge extended X-ray absorption fine structure (EXAFS) analysis showed that significant fractions of Np were coordinated to FeO entities at pH 9. This highlights the potential role of Fe­(II/III) clay edge sites as a strong Np­(V) surface complex partner and points to the partial reduction of sorbed Np­(V) to Np­(IV) via structural Fe­(II).

Environmental Science and Technology, 57, 30, American Chemical Society, 2023, ISSN:0013936X, DOI:10.1021/acs.est.2c09356, 11185-11194. SJR (Scopus):3.12 Q1, не оглавява ранглистата (Scopus)

https://www.scopus.com/pages/publications/85166385133


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