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Macro- and micro-scale studies on U(VI) immobilization in hardened cement paste

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Abstract

Wet chemistry and synchrotron-based (micro-)spectroscopic investigations have been carried out to determine the uptake and speciation of U(VI) in hardened cement paste (HCP). The wet chemistry experiments included kinetic studies and the determination of the sorption isotherm. The latter measurements allowed conditions for linear sorption to be distinguished from those where precipitation occurred. Micro-X-ray fluorescence and X-ray absorption spectroscopy (μ-XRF/XAS) were used to determine the elemental distribution and the coordination environment of U(VI) in an intact HCP sample at the atomic level. The sample was prepared by in-diffusion of U(VI) into HCP over 9 months. Micro-XRF maps revealed a heterogeneous distribution of U(VI) in a ten micron thick layer on the surface of the HCP disk. Micro-XAS measurements on a U(VI) hot spot showed that the coordination environment of U(VI) is similar to that in U(VI) doped HCP and in C-S-H sorption samples. To the best of our knowledge this is the first synchrotron-based micro-spectroscopic study on the speciation of diffusing uranyl ions with micro-scale spatial resolution.

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Acknowledgments

The micro-spectroscopic studies were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the US Department of Energy, Office of Basic Energy Sciences. Sam Webb (BL 2-3/SSRL) is thanked for the experimental assistance during the measurements. Thanks are extended to the staff of BM 20 (ROBL) at the European Synchrotron Radiation Facility (ESRF) (Grenoble, France) for assistance with the bulk-EXAFS measurements. Prof. F. P. Glasser is gratefully acknowledged for provision of Ca-uranate and uranophane samples. The study was carried out within the framework of a Marie Curie Fellowship with a grant to N.M. financed by the European Community (EC). Partial financial support was provided by the EC through the 6th framework programme “ACTINET” and by the National Cooperation for the Disposal of Radioactive Waste (Nagra), Switzerland.

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  1. N. Macé

    Present address: CEA Saclay, DEN/DANS/DPC/SECR, 91191, Gif-sur-Yvette Cedex, France

Authors and Affiliations

  1. Laboratory for Waste Management, Nuclear Energy and Safety Research Department, Paul Scherrer Institut, 5232, Villigen PSI, Switzerland

    E. Wieland, N. Macé, R. Dähn, D. Kunz & J. Tits

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  1. E. Wieland
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  2. N. Macé
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  3. R. Dähn
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  4. D. Kunz
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  5. J. Tits
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Correspondence to E. Wieland.

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Wieland, E., Macé, N., Dähn, R. et al. Macro- and micro-scale studies on U(VI) immobilization in hardened cement paste. J Radioanal Nucl Chem 286, 793–800 (2010). https://doi.org/10.1007/s10967-010-0742-y

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  • DOI: https://doi.org/10.1007/s10967-010-0742-y

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