Luis Montenegro

Inverse modeling of multicomponent reactive transport through single and dual porosity media

Compacted bentonite is foreseen as buffer material for high-level radioactive waste in deep geological repositories because it provides hydraulic isolation, chemical stability, and radionuclide sorption. A wide range of laboratory tests were performed within the framework of FEBEX (Full-scale Engineered Barrier EXperiment) project to characterize buffer properties and develop numerical models for FEBEX bentonite. Here we present inverse single and dual-continuum multicomponent reactive transport models of a long-term permeation test performed on a 2.5 cm long sample of FEBEX bentonite. Initial saline bentonite porewater was flushed with 5.5 pore volumes of fresh granitic water. Water flux and chemical composition of effluent waters were monitored during almost 4 years. The model accounts for solute advection and diffusion and geochemical reactions such as aqueous complexation, acid-base, cation exchange, protonation/deprotonation by surface complexation and dissolution/precipitation of calcite, chalcedony and gypsum. All of these processes are assumed at local equilibrium. Similar to previous studies of bentonite porewater chemistry on batch systems which attest the relevance of protonation/deprotonation on buffering pH, our results confirm that protonation/deprotonation is a key process in maintaining a stable pH under dynamic transport conditions. Breakthrough curves of reactive species are more sensitive to initial porewater concentration than to effective diffusion coefficient. Optimum estimates of initial porewater chemistry of saturated compacted FEBEX bentonite are obtained by solving the inverse problem of multicomponent reactive transport. While the single-continuum model reproduces the trends of measured data for most chemical species, it fails to match properly the long tails of most breakthrough curves. Such limitation is overcome by resorting to a dual-continuum reactive transport model.

A coupled THC model of the FEBEX in situ test with bentonite swelling and chemical and thermal osmosis

The performance assessment of a geological repository for radioactive waste requires quantifying the geochemical evolution of the bentonite engineered barrier. This barrier will be exposed to coupled thermal (T), hydrodynamic (H), mechanical (M) and chemical (C) processes. This paper presents a coupled THC model of the FEBEX (Full-scale Engineered Barrier EXperiment) in situ test which accounts for bentonite swelling and chemical and thermal osmosis. Model results attest the relevance of thermal osmosis and bentonite swelling for the geochemical evolution of the bentonite barrier while chemical osmosis is found to be almost irrelevant. The model has been tested with data collected after the dismantling of heater 1 of the in situ test. The model reproduces reasonably well the measured temperature, relative humidity, water content and inferred geochemical data. However, it fails to mimic the solute concentrations at the heater-bentonite and bentonite-granite interfaces because the model does not account for the volume change of bentonite, the CO(2)(g) degassing and the transport of vapor from the bentonite into the granite. The inferred HCO(3)(-) and pH data cannot be explained solely by solute transport, calcite dissolution and protonation/deprotonation by surface complexation, suggesting that such data may be affected also by other reactions.

Long-term non-isothermal reactive transport model of compacted bentonite, concrete and corrosion products in a HLW repository in clay

Radioactive waste disposal in deep geological repositories envisages engineered barriers such as carbon-steel canisters, compacted bentonite and concrete liners. The stability and performance of the bentonite barrier could be affected by the corrosion products at the canister-bentonite interface and the hyper-alkaline conditions caused by the degradation of concrete at the bentonite-concrete interface. Additionally, the host clay formation could also be affected by the hyper-alkaline plume at the concrete-clay interface. Here we present a non-isothermal multicomponent reactive transport model of the long-term (1Ma) interactions of the compacted bentonite with the corrosion products of a carbon-steel canister and the concrete liner of the engineered barrier of a high-level radioactive waste repository in clay. Model results show that magnetite is the main corrosion product. Its precipitation reduces significantly the porosity of the bentonite near the canister. The degradation of the concrete liner leads to the precipitation of secondary minerals and the reduction of the porosity of the bentonite and the clay formation at their interfaces with the concrete liner. The reduction of the porosity becomes especially relevant at t=104years. The zones affected by pore clogging at the canister-bentonite and concrete-clay interfaces at 1Ma are approximately equal to 1 and 3.3cm thick, respectively. The hyper-alkaline front (pH>8.5) spreads 2.5cm into the clay formation after 1Ma. Our simulation results share the key features of the models reported by others for engineered barrier systems at similar chemical conditions, including: 1) Pore clogging at the canister-bentonite and concrete-clay interfaces; 2) Narrow alteration zones; and 3) Limited smectite dissolution after 1Ma.

Coupled Thermo-Hydro-Geochemical Models of Engineered Barrier Systems: The Febex Project

FEBEX (Full-scale Engineered Barrier EXperiment) is a demonstration and research project dealing with the bentonite engineered barrier designed for sealing and containment of waste in a high level radioactive waste repository (HLWR). It includes two main experiments: an situ full-scale test performed at Grimsel (GTS) and a mock-up test operating since February 1997 at CIEMAT facilities in Madrid (Spain) [1,2,3]. One of the objectives of FEBEX is the development and testing of conceptual and numerical models for the thermal, hydrodynamic, and geochemical (THG) processes expected to take place in engineered clay barriers. A significant improvement in coupled THG modeling of the clay barrier has been achieved both in terms of a better understanding of THG processes and more sophisticated THG computer codes. The ability of these models to reproduce the observed THG patterns in a wide range of THG conditions enhances the confidence in their prediction capabilities. Numerical THG models of heating and hydration experiments performed on small-scale lab cells provide excellent results for temperatures, water inflow and final water content in the cells [3]. Calculated concentrations at the end of the experiments reproduce most of the patterns of measured data. In general, the fit of concentrations of dissolved species is better than that of exchanged cations. These models were later used to simulate the evolution of the large-scale experiments (in situ and mock-up). Some thermo-hydrodynamic hypotheses and bentonite parameters were slightly revised during TH calibration of the mock-up test. The results of the reference model reproduce simultaneously the observed water inflows and bentonite temperatures and relative humidities. Although the model is highly sensitive to one-at-a-time variations in model parameters, the possibility of parameter combinations leading to similar fits cannot be precluded. The TH model of the “in situ” test is based on the same bentonite TH parameters and assumptions as for the “mock-up” test. Granite parameters were slightly modified during the calibration process in order to reproduce the observed thermal and hydrodynamic evolution. The reference model captures properly relative humidities and temperatures in the bentonite [3]. It also reproduces the observed spatial distribution of water pressures and temperatures in the granite. Once calibrated the TH aspects of the model, predictions of the THG evolution of both tests were performed. Data from the dismantling of the in situ test, which is planned for the summer of 2001, will provide a unique opportunity to test and validate current THG models of the EBS.

Forward and inverse modelling of multicomponent reactive transport in single and double porosity media

The term ‘double porosity’ is generally used to represent a conceptual model in which the medium is divided into two or more domains that are coupled by an interaction term for modeling flow and solute transport. While double porosity models are available for water flow and conservative transport, there is not much experience in the fourmulation of double porosity models for multicomponent reactive species. Here we analyze the double porosity behavior in a long-term permeation and tracer test performed on a sample of FEBEX compacted bentonite. FEBEX (Full-scale Engineered Barrier EXperiment) is a demonstration and research project dealing with the bentonite engineered barrier designed for sealing and containment of waste in a high level radioactive waste repository. Hydrogeochemical modelling of porewaters indicate that the main geochemical processes controlling the chemistry of the bentonite are acid-base reactions, aqueous complexation, cation exchange, dissolution/ex-solution of CO 2 , and dissolution and precipitation of highly soluble minerals such as calcite, dolomite, chalcedony, and gypsum/anhydrite. All these processes are assumed to take place under equilibrium conditions. Water flux and chemical data of effluent waters were measured during the experiment. Inverse modelling of this experiment has been carried out using single and double porosity models. The measured breakthrough curve of chloride is consistent with a double porosity model. The model reproduces the trends of measured data except for bicarbonate and pH which are affected by uncertainties in the evolution of CO 2 (g) pressures.