Evidence of ancient life at 207 m depth in a granitic aquifer

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.     

A review and comparison of fracture mineral investigations and their application to radioactive waste disposal

A compilation and comparison of fracture mineral studies from the Canadian and Fennoscandian Shields and the French Massif Central shows many similarities indicating larger external control over fracture mineral deposition, with different rock types exerting local controls. The sites investigated represent a wide range of geological settings, and host rock types ranging from felsic intrusive and extrusives to ultramafic intrusives and volcanics that span an age range from 2.5 to 0.36 Ga. Typical fracture minerals found at Canadian Shield sites include calcite, quartz, chlorite and clays, and these do not appear to be dependant on age, erosional depth or geological environment. The Fennoscandian Shield has a much larger variety of fracture filling minerals with epidote, zeolites, prehnite, fluorite, pyrrhotite, Fe oxides, serpentine, graphite, magnesite and barite in addition to the minerals typically found at Canadian Shield sites. The major control on fracture mineral type is most likely variations in rock type, and fluid chemistry and temperature.     

Detecting the near-surface redox front in crystalline bedrock using fracture mineral distribution,geochemistry and U-series disequilibrium

Oxidizing conditions normally prevail in surface waters and near-surface groundwaters, but there is usually a change to reducing conditions in groundwater at greater depth. Dissolved O₂ originally present is consumed through biogenic and inorganic reactions along the flow paths. Fracture minerals participate in these reactions and the fracture mineralogy and geochemistry can be used to trace the redox front. An important task in the safety assessment of a potential repository for the disposal of nuclear waste in crystalline bedrock, at an approximate depth of 500 m in Sweden, is to demonstrate that reducing conditions can be maintained for a long period of time. Oxygen may damage the Cu canisters that host nuclear waste; additionally, in the event of a canister failure, oxidizing conditions may increase the mobility of some radionuclides. The present study of the near-surface redox front is based on mineralogical (redox-sensitive minerals), geochemical (redox-sensitive elements) and U-series disequilibrium investigations of mineral coatings along open fractures. The fractures have been sampled along drill cores from closely spaced, 100 m deep boreholes, which were drilled during the site investigation work in the Laxemar area, south-eastern Sweden, carried out by the Swedish Nuclear Fuel and Waste Management Co. (SKB). The distribution of the redox-sensitive minerals pyrite and goethite in open fractures shows that the redox front (switch from mainly goethite to mainly pyrite in the fractures) generally occurs at about 15–20 m depth. Calcite leaching by recharging water is indicated in the upper 20–30 m and positive Ce-anomalies suggest oxidation of Ce down to 20 m depth. The U-series radionuclides show disequilibrium in most of the samples, indicating mobility of U during the last 1 Ma. In the upper 20 m, U is mainly removed (due to oxidation) or has experienced complex removal and/or deposition. At depths of 35–55 m, both deposition and removal of U are indicated. Below 55 m, recent deposition of U is generally indicated which suggests removal of U near surface (oxidation) and deposition of U below the redox front. Scattered goethite occurrences below the general redox front (down to ca 80 m) and signs of U removal at 35–55 m mostly correlate with sections of high transmissivity (and/or high fracture frequencies). This shows that highly transmissive fractures are generally required to allow oxygenated groundwaters at depth greater than ca 30 m. Removal of U (oxidation) below 55 m within the last 300 ka is not observed. Although penetration of glacial waters to great depths has been confirmed in the study area, their potential O₂ load seems to have been reduced near the surface.     

Palaeohydrogeology: A methodology based on fracture mineral studies

Two sites on the east coast of Sweden (Forsmark and Laxemar/Simpevarp) are currently being investigated as potential geologic hosts for a deep repository isolating high-level nuclear waste. In this paper, a methodology for fracture mineral studies is suggested with focus on the variation in depth of the fresh/saline water interface and location of the redox front in the bedrock. The most commonly precipitated fracture minerals in crystalline rocks are chlorite, calcite, quartz, K-feldspar, Ca–Al-silicates like epidote, prehnite and laumontite, sulphides and Fe-oxides. Of these, calcite is the mineral best suited for palaeohydrological studies since it precipitates during a wide range of conditions including low-temperature conditions during the Pleistocene and Holocene epochs. Sulphides and Fe-oxides/hydroxides provide information on the position of the redox front. In order to carry out palaeohydrological studies, a number of prerequisites are required such as; high quality drill core material, geological knowledge of the sequence of fracture mineralizations; the post-glacial (Holocene) evolution in the area; high quality groundwater chemistry, including stable isotopes; and a conceptual model of the hydrogeochemistry that is to be tested. The choice of methods used here is based on the fact that both the Forsmark and Laxemar/Simpevarp sites are situated in Palaeoproterozoic crystalline rocks with reactivation of fractures over at least 1.5 Ga, and they have been exposed to glaciations/deglaciations and transgressions/regressions of the Baltic Sea during the Quaternary. This has resulted in a palaeohydrology with a range of groundwaters of quite different chemistry and stable isotopic composition. The suggested scheme for solving the variation in depth of the fresh/saline water interface focuses on fracture calcite. It includes a step-by-step procedure with;

(1)

Initial δ¹⁸O and δ¹³C, analyses and complementary petrographic studies of thin sections and crystal morphology followed by     

Fracture-related hydrothermal alteration of metagranitic rock and associated changes in mineralogy, geochemistry and degree of oxidation: a case study at Forsmark, central Sweden

Red-staining of rocks due to fluid–rock interaction during hydrothermal circulation in fractures is a common feature in crystalline sequences. In this study, red-stained metagranitic rock adjacent to fractures in Forsmark, central Sweden, has been studied with emphasis on the mineral reactions and associated element mobility occurring during the alteration. The main mineral reactions associated with the hydrothermal alteration are an almost complete saussuritization of plagioclase accompanied by total chloritization of biotite. Magnetite has been partly replaced by hematite whereas quartz and K-feldspar were relatively unaffected by the hydrothermal alteration. We show that redistribution of elements on the whole rock scale was very limited and is mainly manifested by enrichment of Na₂O and volatiles and depletion of CaO, FeO and SiO₂ in the red-stained rock. However, on the microscale, element redistribution was more extensive, with both intragranular and intergranular migration of e.g. Ca, K, Na, Al, Si, Fe, Ba, Cs, Rb, Sr, Ti and REEs. The altered rock shows a shift towards higher total oxidation factors, but the change is smaller than 1σ and the red-staining of the rock is due to hematite dissemination rather than a significant oxidation of the rock. An increase in the connected porosity is also observed in the altered rock.     

Real system analyses/natural analogues

This paper gives an overview of the behaviour of U in two natural systems, the Forsmark site (a granitic system) in Sweden and the Ruprechtov site (a Tertiary sedimentary system) in the Czech Republic, which have been investigated in the frame of the FUNMIG project. It is not a full review paper on U geochemistry. It shows how different approaches and methods have been used to derive information on U solubility and speciation, on characteristics of key processes as well as on timescales of these processes and accordingly information on the long-term stability of U phases in the natural systems. The results are set in a wider context by relation to selected results from other sites.     

Sveconorwegian and Caledonian foreland basins in the Baltic Shield revealed by fission-track thermochronology

Fission-track thermochronology has been applied to apatite, zircon and titanite from various depths of the Baltic Shield. Burial due to Sveconorwegian (Grenville) and Caledonian foreland sedimentation is revealed.
Titanite and zircon fission-track ages from surface samples (from eastern Sweden) do not vary significantly and average ∼ 850 Myr. It is suggested that Sveconorwegian sediments reached a thickness of at least 8 km in eastern Sweden. Exhumation of these sediments was succeeded by deposition of Lower Palaeozoic cover rocks. Apatite fission-track ages along a transect from SW to NE across the shield, increase from ∼ 300 Myr to ∼ 900 Myr and yield the Phanerozoic history of subsidence and exhumation. Apatite fission tracks, in the basement of the thickest parts of the foreland basin, were totally annealed. These results suggest a > 600 km wide Caledonian foreland basin filled by Devonian sediments that were > 2.5 km thick in southern and western Sweden, thinning to the east (in Finland).     

Red-staining of the wall rock and its influence on the reducing capacity around water conducting fractures

Red-staining and alteration of wall rock is common around water conducting fractures in the Laxemar–Simpevarp area (SE Sweden), which is currently being investigated by the Swedish Nuclear Fuel and Waste Management Co. (SKB) in common with many other places. Red-staining is often interpreted as a clear sign of oxidation but relevant analyses are seldom performed. The area is dominated by Palaeoproterozoic crystalline rocks ranging in composition from quartz monzodiorite to granite. In this study wall rock samples have been compared with reference samples from within 0.1 to 1 m of the red-stained rock, in order to describe mineralogical and geochemical changes but also changes in redox conditions. A methodology for tracing changes in mineralogy, mineral and whole rock chemistry and Fe³⁺/Fe_tot ratio in silicates and oxides in the red-stained wall rock and the reference rock is reported. The results show that the red-stained rock adjacent to the fractures displays major changes in mineralogy; biotite, plagioclase and magnetite have been altered and chlorite, K-feldspar, albite, sericite, prehnite, epidote and hematite have been formed. The changes in chemistry are however moderate; K-enrichment, Ca-depletion and constant Fe_tot are documented. The Fe³⁺/Fe_tot ratio in the oxide phase is higher in the red-stained samples whereas the Fe³⁺/Fe_tot ratio in the silicate phase is largely similar in the wall rock and the reference samples. Because most of the Fe is hosted in the silicate phase the decrease in reducing capacity (Fe²⁺), if any, in the red-stained wall rock is very small and not as high as macroscopic observations might suggest. Instead, the mineralogical changes in combination with the modest oxidation and formation of minute hematite grains in porous secondary minerals in pseudomorphs after plagioclase have produced the red-staining. Increased porosity is also characteristic for the red-stained rock. Moderate alteration in the macroscopically fresh reference rock shows that the hydrothermal alteration reaches further from the fracture than the red-staining. The extent of the red-staining can therefore not be used in the same way as the extent of the alteration adjacent to a fracture. The increase in porosity in the red-stained rock may result in enhanced retention of radio-nuclides due to an increased sorptivity and diffusion close to the fracture.     

Modelling the evolution of hydrochemical conditions in the Fennoscandian Shield during Holocene time using multidisciplinary information

Three-dimensional, large-scale models for groundwater flow and solute transport are used for the low-temperature, fractured crystalline rock sites in Sweden that are being considered for the geological disposal of spent nuclear fuel. It has been suggested that comparisons between measured and simulated present-day hydrochemical data provide a means to constrain the complex influences of past climatic events and to improve the ability to understand the palaeohydrogeological evolution of the physical system studied. Here the authors demonstrate how the integration of multidisciplinary data and models from one of the sites in Sweden (Forsmark) can aid the appraisal of the hydrochemical conditions at 8000 BC, which is the selected starting point for the palaeohydrogeological modelling of the hydrochemical conditions in the Fennoscandian Shield during the Holocene (last 10 ka). Since a firm understanding of the evolution of the hydrochemical conditions is important for the long-term safety assessment, recognition of the initial hydrochemical conditions is essential for the overall build-up of confidence in the modelling process.