Abstract
Tomographic studies of granite from the Äspö Underground Laboratory in Sweden are performed to understand the observed release of natural uranium in column studies upon application of groundwater flow. X-ray phase-sensitive tomography images reconstructed from in-line X-ray phase contrasted radiographs were compared with scanning fluorescence tomography reconstructions. The latter are based on sinograms of X-ray emission lines recorded with spatial resolution on a nanometer scale for a granite rock containing U after being subjected to a radionuclide tracer experiment. The results show that the U distribution follows microfissures or pores in the granite. Naturally occurring Th is revealed to be intimately associated with what appears to be feldspar, suggesting its being present as a dopant ion in the mineral structure. Neptunium tracer was not found in a sample prepared using FIB lift-out techniques, although the presence of Np was identified in the original granite piece during screening experiments prior to FIB-ing. The Np-containing part of the sample broke off during the preparation. Although this case study was limited to only three samples, initial interpretation of results confirm that Th is less likely than U to become mobile in groundwater upon drilling and excavation of emplacement caverns and shafts for a nuclear waste repository in granite bedrock.
This is a preview of subscription content, log in via an institution.
Buying options
Tax calculation will be finalised at checkout
Purchases are for personal use only
Learn about institutional subscriptionsReferences
Kienzler, B, Vejmelka, P, Römer, J, Jansson, M (2009) Actinide migration in fractures of granite host rock: laboratory and in situ investigations. Nucl. Technol. 165:223–240
Denecke, MA, Brendebach, B, De Nolf, W, Falkenberg, G, Janssens, K, Simon, R (2009) Spatially resolved μ-XRF and μ-XAFS study of a fractured granite bore core following a radiotracer experiment. Spectrochim. Acta B 64:791–795
Overwijk, MHF, van den Heuvel, FC, Bulle-Lieuwma, CWT (1993) Novel scheme for the preparation of transmission electron microscopy specimens with a focused ion beam. J. Vac. Sci. Technol. B11:2021–2024
Falkenberg, G, Rickers, K, Bilderback, DH, Huang, R (2003) A Single-bounce Capillary for Focusing of Hard X-rays. http://hasyweb.desy.de/science/annual_reports/2003_report/part1/intern/11062.pdf
Huang, R, Bilderback, DH (2006) Single-bounce monocapillaries for focusing synchrotron radiation: modeling, measurements and theoretical limits. J. Synchrotron Radiat. 13:74–84
Vekemans, B, Janssens, K, Vincze, L, Adams, F, Van Espen, P (1994) Analysis of X-ray spectra by iterative least squares (AXIL): new developments. X-ray Spectrom. 23:278
Bleuet, P, Simionovici, A, Lemelle, L, Ferroir, T, Cloetens, P, Tucoulou, R, Susini, J (2008) Hard X-rays nanoscale fluorescence imaging of earth and planetary science samples. Appl. Phys. Lett. 92:213111
Ortega, R, Cloetens, P, Devès, G, Carmona, A, Bohic, S (2007) Iron storage within dopamine neurovesicles revealed by chemical nano-imaging. PLoS ONE 2(9):e925
Bleuet, P, Cloetens, P, Gergaud, P, Mariolle, D, Chevalier, N, Tucoulou, R, Susini, J, Chabli, A (2009) A hard X-ray nanoprobe for scanning and projection nanotomography. Rev. Sci. Instrum. 80:056101
Somogyi, A, Tucoulou, R, Martinez-Criado, G, Homs, A, Bleuet, P, Simionovici, A (2005) ID22: a multitechnique hard X-ray microprobe beamline at the European Synchrotron Radiation Facility. J. Synchrotron Radiat. 12:208–215
Labiche, J-C, Mathon, O, Pascarelli, S, Newton, MA, Ferre, GG, Curfs, C, Vaughan, G, Homs, A, Carreiras, DF (2007) The fast readout low noise camera as a versatile X-ray detector for time resolved dispersive extended X-ray absorption fine structure and diffraction studies of dynamic problems in materials science, chemistry, and catalysis. Rev. Sci. Instrum. 78: 0901301
Lange, K, Carson, R (1984) EM reconstruction algorithms for emission and transmission tomography. J. Comput. Assist. Tomogr. 8(2):306
De Nolf, W, Janssen, K (2010) Micro X-ray diffraction and fluorescence tomography for the study of multilayered automotive paints. Surf. Interf. Anal. 42:411–418
Sole, VA, Papillon, E, Cotte, M, Walter, P, Susini, J (2007) A multiplatform code for the analysis of energy-dispersive X-ray fluorescence spectra. Spectrochim. Acta B62:63
Paganin, D, Mayo, SC, Gureyev, TE, Miller, PR, Wilkins, SW (2002) Simultaneous phase and amplitude extraction from a single defocused image of a homogeneous object. J. Microsc. 206:33–40
Cloetens, P, Ludwig, W, Baruchel, J, Van Dyck, D, Van Landuyt, J, Guigay, JP, Schlenker, M (1999) Holotomography: quantitative phase tomography with micrometer resolution using hard synchrotron radiation X-rays. Appl. Phys. Lett. 75:2912–2914
Weitzel, H, Schrocke, H (1980) Kristallstrukturverfeinerungen von euxenit, Y(Nb0.5Ti0.5)2O6, und M-fergusonit, YNbO4. Zeitschrift für Kristallographie 152:69–82
Abolhassani, S, Gasser, P (2006) Preparation of TEM samples of metal-oxide interface by focused ion beam. J. Microsc. doi: 10.1111/j.1365-2818.2006.01599
Schroer, CG, Boye, P, Feldkamp, JM, Patommel, J, Samberg, D, Schropp, A, Schwab, A, Stephan, S, Falkenberg, G, Wellenreuther, G, Reimers, N (2010) Hard X-ray nanoprobe at beamline P06 at PETRA III. Nucl. Instrum. Methods Phys. Res. A 616:93–97
Denecke, MA, Janssens, K, Proost, K, Rothe, J, Noseck, U (2005) Confocal micro-XRF and micro-XAFS studies of uranium speciation in a tertiary sediment from a waste disposal natural analogue site. Environ. Sci. Technol. 39(7):2049–2058
Schoch, AE, Scheepers, R (1990) The distribution of uranium and thorium in the cape columbine granite from the southwestern cape province, South Africa. Ore Geol. Rev. 5:223–246
Acknowledgments
We thank HASYLAB and the ESRF for awarding us beamtime. We also are grateful to E. Sobolla (KIT-INE) and Julijana Krbanjevic (PSI) for preparation of the ground and FIB-ed samples and J. Göttlicher (KIT) for expert improvement of this manuscript. We acknowledge financial support as a Joint Research Group between the German Helmholtz Society and the Russian Basic Research Foundation (HRJRG-011 and 07-03-92280-SIG_a).
Author information
Authors and Affiliations
Corresponding author
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2011 Springer-Verlag Berlin Heidelberg
About this chapter
Cite this chapter
Denecke, M.A. et al. (2011). Speciation of Actinides in Granite Subjected to Tracer Studies. In: Kalmykov, S., Denecke, M. (eds) Actinide Nanoparticle Research. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-11432-8_16
Download citation
DOI: https://doi.org/10.1007/978-3-642-11432-8_16
Published:
Publisher Name: Springer, Berlin, Heidelberg
Print ISBN: 978-3-642-11431-1
Online ISBN: 978-3-642-11432-8
eBook Packages: Chemistry and Materials ScienceChemistry and Material Science (R0)