Reactive Transport Model of Steel/Bentonite Interactions in the FEBEX in Situ Test

Steel corrosion plays a major role in the geochemical evolution at the canister/bentonite interface of the engineered barrier systems of geological radioactive waste repositories. The interactions between corrosion products and bentonite can significantly affect bentonite properties and performance. These interactions have been investigated by resorting to in situ tests conducted in underground laboratories, such as the FEBEX (Full-scale Engineered Barrier Experiment) test. The FEBEX in situ test, which was conducted at the Grimsel underground research laboratory in Switzerland from 1997 to 2015, demonstrated substantial corrosion of the steel liner in areas without a heater, primarily due to the presence of O2. Here we report a reactive transport model that simulates steel corrosion products and their interactions with bentonite. The model builds on a previously published conceptual geochemical model and addresses its limitations by integrating a more detailed representation of temperature and unsaturated flow conditions, leveraging prior thermo–hydrodynamic–mechanical–chemical (THMC) models. Given the prevailing uncertainties in O2 and redox conditions during the test and the limited data on liner corrosion and gas conditions at the liner–bentonite interface, liner corrosion was modeled by using a prescribed time-dependent function for the corrosion rate. Goethite, hematite, and magnetite were the Fe minerals allowed to precipitate in the model. The corrosion rate and the specific surface area of the hematite and magnetite were calibrated based on the profiles of goethite, hematite, and total Fe (including dissolved, exchanged and sorbed forms) observed at the post mortem analysis of the FEBEX in situ test. The model reproduces the observed goethite and hematite precipitation near the liner but underestimates the measured values at greater distances from the liner. The pattern of total calculated Fe concentrations reproduce the measured values except at a distance between 15 and 50 mm from the liner. Goethite is the predominant corrosion product in the model results, even under reducing conditions, owing to kinetic constraints on magnetite and hematite precipitation and to the enhanced stability of goethite driven by pH increase and thermal evolution.