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Rock Matrix Diffusion as a Mechanism for Radionuclide Retardation: Natural Radioelement Migration in Relation to the Microfractography and Petrophysics of Fractured Crystalline rock: Phase I

Objective

Rock matrix diffusion is an important element in radionuclide migration models: diffusion from water-conducting fractures into the rock matrix provides a potentially important mechanism for the retardation of nuclide migrating from a repository. Recent studies of crystalline rocks have shown, however, that free diffusion of nuclide from fractures into the rock matrix does not always take place and that very little of the rock adjacent to fractures may be available for diffusion. Although mathematical models describing diffusion have been developed in the past, they have never been furnished with complete physical and chemical data from actual sites. The aims of the study are: 1) to observe evidence of past diffusion of uranium and its daughters from fractures into the rock adjacent to fractures; 2) to relate observed diffusion phenomena to the physical properties of the rock; 3) to construct physicochemical profiles across fractures and into the adjacent rock to allow complete characterisation of past diffusion and assess the potential for future diffusion; and 4) to develop a mathematical diffusion model that can be validated by reference to geo-logical evidence and be incorporated reliably into overall radionuclide migration models.
Rock matrix diffusion is an important element in radionuclide migration models: diffusion from water conducting fractures into the rock matrix provides a potentially important mechanism for the retardation of nuclides migrating from a repository. Recent studies of crystalline rocks have shown, however, that free diffusion of nuclides from fractures into the rock matrix does not always take place and that very little of the rock adjacent to fractures may be available for diffusion. Although mathematical models describing diffusion have been developed in the past, they have never been furnished with complete physical and chemical data from actual sites. The aims of the study are: to observe evidence of past diffusion of uranium and its daughters from fractures into the rock adjacent to fractures; to relate observed diffusion phenomena to the physical properties of the rock; to construct physicochemical profiles across fractures and into the adjacent rock to allow complete characterisation of past diffusion and assess the potential for future diffusion; and to develop a mathematical diffusion model that can be validated by reference to geological evidence and be incorporated reliably into overall radionuclide migration models. Preliminary studies of the 3-dimensional microfractographic network of granite have been undertaken under laser scanning microscopy in confocal mode (LSM-CM). A preliminary petrographic study has been carried out using 2 different methods: digital image analysis and stereology. Polished thin sections of granite have also been studied under acoustic microscopy. The images obtained make possible the detailed identification of intergranular structures in the rock forming minerals. Thin sections of granite, impregnated with fluorescent resin, have been studied in Besancon using fluorescence optical microscopy. The feldspars appear highly altered; quartz grians show intragranular and intergranular cracks and the mica sometimes shows a loss of cohesion between grains. The data being acquired in the various studies described above will provide the input for a mathematical diffusion model.
Work programme:

(1) Determination of rock properties and examination of evidence for past diffusion in a series of rock slices at distance of up to 50 cm from hydrogeologically-active fractures;
(2) Quantitative petrophysical analysis and the determination of key physical properties (accessible porosity, dry density, void index, kinetic water behaviour, dynamic properties);
(3) Quantitative microstructural analysis using optical, fluorescence, acoustic and confocal laser microscopy, digital image processing and stereological techniques;
(4) Geochemical analysis (major elements, iron chemistry, uranium and thorium, Rare Earth Elements, selected trace elements);
(5) Uranium disequilibrium studies by alpha spectrometry;
(6) Uranium microcartography by autoradiographic, fission track and SEM/EDX techniques;
(7) The development of a mathematical diffusion model based upon real geological/geochemical data.

Funding Scheme

CSC - Cost-sharing contracts

Coordinator

University of Exeter
Address
Laver Building North Park Road
EX4 4QE Exeter
United Kingdom

Participants (4)

Commissariat à l'Energie Atomique (CEA)
France
Address
Centre D'études De Fontenay-aux-roses 60-68 Avenue Du Général Leclerc
92265 Fontenay-aux-roses
UNIVERSIDAD DE OVIEDO
Spain
Address
C/. Jesús Arias De Velasco, S/n
33005 Oviedo
University of Liverpool
United Kingdom
Address
Brownlow Street
L69 3BX Liverpool
Université de Franche-Comté
France
Address
16 Route De Gray
25030 Besançon