Large-scale modeling of reactive solute transport in fracture zones of granitic bedrocks

J Contam Hydrol. 2006 Jan 10;82(3-4):293-318. doi: 10.1016/j.jconhyd.2005.10.008. Epub 2005 Dec 5.

Abstract

Final disposal of high-level radioactive waste in deep repositories located in fractured granite formations is being considered by several countries. The assessment of the safety of such repositories requires using numerical models of groundwater flow, solute transport and chemical processes. These models are being developed from data and knowledge gained from in situ experiments such as the Redox Zone Experiment carried out at the underground laboratory of Aspö in Sweden. This experiment aimed at evaluating the effects of the construction of the access tunnel on the hydrogeological and hydrochemical conditions of a fracture zone intersected by the tunnel. Most chemical species showed dilution trends except for bicarbonate and sulphate which unexpectedly increased with time. Molinero and Samper [Molinero, J. and Samper, J. Groundwater flow and solute transport in fracture zones: an improved model for a large-scale field experiment at Aspö (Sweden). J. Hydraul. Res., 42, Extra Issue, 157-172] presented a two-dimensional water flow and solute transport finite element model which reproduced measured drawdowns and dilution curves of conservative species. Here we extend their model by using a reactive transport which accounts for aqueous complexation, acid-base, redox processes, dissolution-precipitation of calcite, quartz, hematite and pyrite, and cation exchange between Na+ and Ca2+. The model provides field-scale estimates of cation exchange capacity of the fracture zone and redox potential of groundwater recharge. It serves also to identify the mineral phases controlling the solubility of iron. In addition, the model is useful to test the relevance of several geochemical processes. Model results rule out calcite dissolution as the process causing the increase in bicarbonate concentration and reject the following possible sources of sulphate: (1) pyrite dissolution, (2) leaching of alkaline sulphate-rich waters from a nearby rock landfill and (3) dissolution of iron monosulphides contained in Baltic seafloor sediments. Based on these results, microbially mediated processes are postulated as the most likely hypothesis to explain the measured increase of dissolved bicarbonates and sulphates after tunnel construction.

MeSH terms

  • Bicarbonates / analysis
  • Bicarbonates / chemistry
  • Chemical Precipitation
  • Environmental Monitoring*
  • Finite Element Analysis
  • Geological Phenomena
  • Geology*
  • Hydrogen-Ion Concentration
  • Minerals / analysis
  • Minerals / chemistry
  • Models, Chemical
  • Oxidation-Reduction
  • Radioactive Waste*
  • Risk Assessment
  • Silicon Dioxide / analysis*
  • Silicon Dioxide / chemistry
  • Sodium Chloride / chemistry
  • Sulfates / analysis
  • Sulfates / chemistry
  • Time Factors
  • Water Movements
  • Water Pollutants, Radioactive / analysis*

Substances

  • Bicarbonates
  • Minerals
  • Radioactive Waste
  • Sulfates
  • Water Pollutants, Radioactive
  • granite
  • Sodium Chloride
  • Silicon Dioxide