[1] Mineralogical and retardation properties of rock materials responsible for water-rock interaction in in situ migration experiments with sorbing radioactive tracers were studied in laboratory experiments. The porosity was studied by water saturation measurements and the PMMA method was used for detailed porosity characterization of heterogeneity distributions and porosity profiles toward the fracture surface. Mylonite and altered diorite sampled in the rim zone of the fracture and representative bulk rock types were investigated by batch sorption measurements with crushed materials and through-diffusion and in-diffusion experiments in intact rock pieces. Autoradiography was used for visualization of in-diffusion profiles of sorbing tracers. The use of detailed porosity information and quantitative data on heterogeneity in porosity is shown to significantly improve the interpretation and evaluation of laboratory-scale diffusion experiments. We show through the combined approach of detailed porosity characterization and laboratory sorption and diffusion investigations that we can distinguish retention properties of bulk rock and altered rock and provide qualitative and quantitative data of heterogeneous rock properties that expand the possibility for including relevant processes in the interpretation of the results of in situ tracer tests.
The results of electron-microscopy investigations of calcite precipitated in a water-conducting fracture in a ca. 1800 Ma granitic rock from 207 m below sea level at the island of Aspo on the southeastern (Baltic) coast of Sweden are compared with measurements of carbon, oxygen, and sulfur isotope composition of the calcite and embedded pyrite. Parts of the calcite had extremely low delta 13C values, indicative of biological activity, and contained bacteria-like microfossils occurring in colonies and as typical biofllms. X-ray microanalysis demonstrated these fossils to be enriched in carbon. Our results provide evidence for ancient life in deep granitic rock aquifers and suggest that the modern microbial life found there is intrinsic. Modeling historical and present geochemical processes in deep granitic aquifers should, therefore, preferably include biologically catalyzed reactions. The results also suggest that the search for life on other planets, e.g., Mars, should include subsurface material.
[1] We evaluate the breakthrough curves obtained within a comprehensive experimental program for investigating the retention properties of crystalline rock, referred to as Tracer Retention Understanding Experiments (TRUE). The tracer tests were conducted at the Äspö Hard Rock Laboratory (Sweden) in two phases jointly referred to as TRUE Block Scale (TBS); the TBS tests comprise a total of 17 breakthrough curves with nonsorbing and a range of sorbing tracers. The Euclidian length scales are between 10 and 30 m, compared to 5 m for the earlier tests TRUE-1. The unlimited diffusion model is consistent with measured breakthrough curves and is adopted here for evaluation. The model has four independent parameters, two of which are related to advection and dispersion, one which is related to diffusion-sorption, and one which is related to surface sorption; the individual retention parameters or properties cannot be inferred from breakthrough curves alone and require additional constraints. The mean water residence times for the TBS tests are in the range 15-250 h, whereas the coefficient of variation of the water residence times is in the range 0.4-0.6. A consistent trend is found in the calibrated retention parameters with the sorption affinities of the tracers involved. Using Bode sensitivity functions, it is shown that sensitivity increases for the retention parameter with increasing sorption affinity; for nonsorbing tracers, diffusion and hydrodynamic dispersion are shown to "compete," exhibiting similar effects; hence, their estimates are uncertain. The analysis presented here exposes a few fundamental limitations and sensitivities when evaluating diffusioncontrolled retention in the subsurface; it is general and applicable to any site with comparable tracer test data. In part 2, it will be shown how discrete fracture network simulations based on the hydrostructural information available can be used for further constraining individual retention parameters, in particular, the active specific surface area (s f ) and the rock matrix porosity ().
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