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Environmental Science and Pollution Research

, Volume 26, Issue 6, pp 5238–5250 | Cite as

Fate of Lu(III) sorbed on 2-line ferrihydrite at pH 5.7 and aged for 12 years at room temperature. I: insights from ICP-OES, XRD, ESEM, AsFlFFF/ICP-MS, and EXAFS spectroscopy

  • Nicolas FinckEmail author
  • Muriel BoubyEmail author
  • Kathy Dardenne
Analytical methods for characterization of nano- and micro-objects

Abstract

Two-line ferrihydrite (2LFh) was aged for 12 years under ambient conditions and sheltered from light in the presence of Lu(III) used as surrogate for trivalent actinides. 2LFh aging produced hematite rhombohedra with overgrown acicular goethite particles. Analysis of the homogeneous suspension by asymmetrical flow field-flow fractionation (AsFlFFF) coupled to ICP-MS indicated that particles have a mean hydrodynamic diameter of about 140 nm and the strong correlation of the Fe and Lu fractograms hinted at a structural association of the lanthanide with the solid phase(s). Unfortunately, recoveries were low and thus results cannot be considered representative of the whole sample. The suspension was centrifuged and X-ray absorption spectroscopy (XAS) at the Lu L3-edge on the settled particles indicated that Lu(III) is sixfold coordinated by oxygen atoms, pointing to a retention by structural incorporation within particles. This result is consistent with AsFlFFF results on the same suspension without centrifugation. The detection of next nearest Fe and O atoms were consistent with the structure of goethite, ruling out incorporation within hematite. After centrifugation of the suspension, only nanoparticulate needle-like particles, very likely goethite, could be detected in the supernatant by ESEM. AsFlFFF data of the supernatant were comparable to that obtained for the homogeneous suspension, whereas XAS indicated that Lu(III) is predominantly present as dissolved species in the supernatant. Results from both techniques can be interpreted as a major fraction of Lu present as aqueous ions and a minor fraction as structurally incorporated. Findings from this study are corroborated by STEM-HAADF data and results from DFT calculations in a companion paper.

Keywords

Ferrihydrite transformation Hematite Goethite Lutetium Flow field-flow fractionation ICP-MS X-ray absorption spectroscopy 

Notes

Acknowledgements

We thank S. Heck (KIT-INE) for ICP-OES, F. Geyer (KIT-INE) for ICP-MS analyses, and E. Soballa (KIT-INE) for SEM measurements. We acknowledge the synchrotron light source ANKA (Karlsruhe, Germany) for the provision of synchrotron radiation beamtime.

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© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Institute for Nuclear Waste Disposal (INE)Karlsruhe Institute of Technology (KIT)KarlsruheGermany

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