Water, vapour and heat transport in concrete cells for storing radioactive waste

Water is collected from a drain situated at the centre of a concrete cell that stores radioactive waste at ‘El Cabril’, which is the low and intermediate level radioactive waste disposal facility of Spain. This indicates flow of water within the cell. 2D numerical models have been made in order to reproduce and understand the processes that take place inside the cell. Temperature and relative humidity measured by sensors in the cells and thermo-hydraulic parameters from laboratory test have been used. Results show that this phenomenon is caused by capillary rise from the phreatic level, evaporation and condensation within the cell produced by temperature gradients caused by seasonal temperature fluctuations outside. At the centre of the cell, flow of gas and convection also play a role. Three remedial actions have been studied that may avoid the leakage of water from the drain.Peer ReviewedPostprint (author's final draft

Modeling the organic carbon oxidation and redox sequence under the partial-equilibrium approach: a discussion by means of a semi-analytical solution

In this work, we have developed a semi-analytical solution for organic carbon oxidation coupled to the reduction-oxidation sequence assuming the Partial Equilibrium Approach (PEA) and using the decoupling procedure of De Simoni et al. (2005), https://doi.org/10.1029/2005WR004056. Our solution was applied to two very simple cases. The first assumes only advective transport and the second only diffusive transport. Comparison with a numerical solution showed the adequacy of our analytical solution to be implemented in several scenarios, for example, in organic carbon oxidation in the unsaturated zone or in highly heterogeneous advective domains. We found that for the diffusion case the PEA produced spurious reactions, such as oxidation of N2 by O2 when compared with an approach using full kinetics. These reactions do not occur in the advection case. An analysis with the semi-analytical solution revealed that they are the result of a combination of diffusive fluxes and the fact that the PEA assumes the electron acceptors to react with each other in equilibrium. Our analytical solutions are capable to quantify this shortcoming, becoming a tool to validate numerical models using PEA to describe organic carbon oxidation.This work was financially supported by MONOPOLIOS (RTI2018-101990-B-100, MINECO/FEDER), MEDISTRAESIII (Pid2019-110212RB-C22, MICINN), as well as the EU project MARADENTRO (PCI2019-103425-WW2017) and the Catalan Research Project RESTORA (ACA210/18/00,040). Additional funding was obtained from the Generalitat de Catalunya (2017 SGR1485). We also would like to thank Carlos Ayora for his constructive comments on the manuscript.Peer ReviewedPostprint (published version

Modeling the hydrogeochemical evolution of brine in saline systems: case study of the Sabkha of Oum El Khialate in South East Tunisia

We studied the effects of evaporation and groundwater flow on the formation of salt minerals in the Sabkha of Oum El Khialate in South East Tunisia, which contains large amounts of sulfate sodium mineral deposits. Due to the fact that there are no important surface water bodies present in this sabkha, transport of solutes is dominated by advection rather than mixing in lakes. For our study we used both analytical conservative and numerical reactive transport models. Results showed that salinity varies with distance and may reach very high levels near a watershed where the groundwater flux is zero. As a consequence, reactive transport simulations results showed that more minerals precipitate and water activity decreases values near this watershed. Model results also showed that a sequence of precipitating minerals could be deduced after 140,000 years. From the boundary of the sabkha towards the watershed the mineral sequence was dolomite, gypsum, magnesite, bloedite, halite and mirabilite. It was found that the amounts as well as the mineral precipitation distribution strongly depend on salinity and rates of inflowing water. (C) 2014 Elsevier Ltd. All rights reserved.Peer ReviewedPostprint (author’s final draft

Modelling of multiphase flow in evaporation tests in concrete columns

Postprint (published version

Reactive transport modelling of cement-groundwater-rock interaction at the Grimsel Test Site

An in situ experiment at the Grimsel Test Site (Switzerland) to study water-cement-rock interaction in fractured granite was modelled. It consisted of a hardened cement source in a borehole intersecting a water conducting fracture. Grimsel groundwater was injected into this borehole. Two other boreholes at about 0.56 m and 1.12 m from the emplacement borehole were used to monitor the evolution of water composition for 5 years. The modelling approach was based on a 1D radial model for the emplacement borehole and a small volume of rock (fault gouge) around it, and a 2D model for the rest of the domain. The results of the 1D model were used as input for the 2D model. Both models showed dissolution of the fault gouge minerals. Results from the 1D model showed dissolution of portlandite in the cement with an increase in porosity. The 2D model showed a reduction in porosity in the fault gouge due to mineral precipitation. Near the emplacement borehole ettringite precipitated. At the centre of the plume there was precipitation of C-A-S-H and hydrotalcite. At the edge of the hyperalkaline plume calcite, hydrotalcite and illite precipitated.Peer ReviewedPostprint (author's final draft

Application of a mixing-ratios based formulation to model mixing-driven dissolution experiments

We address the question of how one can combine theoretical and numerical modeling approaches with limited measurements from laboratory flow cell experiments to realistically quantify salient features of complex mixing-driven multicomponent reactive transport problems in porous media. Flow cells are commonly used to examine processes affecting reactive transport through porous media, under controlled conditions. An advantage of flow cells is their suitability for relatively fast and reliable experiments, although measuring spatial distributions of a state variable within the cell is often difficult. In general, fluid is sampled only at the flow cell outlet, and concentration measurements are usually interpreted in terms of integrated reaction rates. In reactive transport problems, however, the spatial distribution of the reaction rates within the cell might be more important than the bulk integrated value. Recent advances in theoretical and numerical modeling of complex reactive transport problems [De Simoni M, Carrera J, Sanchez-Vila X, Guadagnini A. A procedure for the solution of multicomponent reactive transport problems. Water Resour Res 2005;41:W11410. doi: 10.1029/2005WR004056, De Simoni M, Sanchez-Vila X, Carrera J, Saaltink MW. A mixing ratios-based formulation for multicomponent reactive transport. Water Resour Res 2007;43:W07419. doi: 10.1029/2006WR005256] result in a methodology conducive to a simple exact expression for the space–time distribution of reaction rates in the presence of homogeneous or heterogeneous reactions in chemical equilibrium. The key points of the methodology are that a general reactive transport problem, involving a relatively high number of chemical species, can be formulated in terms of a set of decoupled partial differential equations, and the amount of reactants evolving into products depends on the rate at which solutions mix. The main objective of the current study is to show how this methodology can be used in conjunction with laboratory experiments to properly describe the key processes that occur in a complex, geochemically-active system under chemical equilibrium conditions. We model three CaCO3 dissolution experiments reported in Singurindy et al. [Singurindy O, Berkowitz B, Lowell RP. Carbonate dissolution and precipitation in coastal environments: Laboratory analysis and theoretical consideration. Water Resour Res 2004;40:W04401. doi: 10.1029/2003WR002651, Singurindy O, Berkowitz B, Lowell RP. Correction to Carbonate dissolution and precipitation in coastal environments: laboratory analysis and theoretical consideration. Water Resour Res 2005;41:W11701. doi: 10.1029/2005WR004433], in which saltwater and freshwater were mixed in different proportions. The integrated reaction rate within the cell estimated from the experiments are modeled independently by means of (a) a state-of-the-art reactive transport code, and (b) the uncoupled methodology of [12, 13], both of which use dispersivity as a single, adjustable parameter. The good agreement between the results from both methodologies demonstrates the feasibility of using simple solutions to design and analyze laboratory experiments involving complex geochemical problem

Temperature driven vapor fluxes in soils cause a net recharge

Temperature gradients can drive vapor diffusion by controlling vapor pressure in the soil. We studied vapor diffusion for soils in two different climates: A semiarid climate at El Cabril (Córdoba, Spain) and a subarctic climate in the Upper Tuul River basin (Mongolia). For El Cabril vapor diffusive fluxes were studied by means of the measured temperatures and an analytical model. For the second site (Upper Tuul) a physically based soil water and energy balance model was developed accounting for relevant processes such as melting-freezing of water and vapor diffusion in the soil. Results of both sites show that vapor diffuses downwards during summer and upwards during winter, while yearly averaged fluxes diffuse downwards. The overall amount is small for El Cabril, but significant for the Upper Tuul. The latter large values can be explained by the large temperature oscillations of the Mongolian climate and the freezing/thawing of subsoil layer.Postprint (published version

Multiphase flow models of concrete cells of the radioactive waste disposal facility at El Cabril (Spain)

El Cabril is the low and intermediate level radioactive waste disposal facility for Spain. From the start of the filling (1992) until 2003, no water was collected from the drain situated at the centre of the cell. From 2003 onwards small amounts of water were collected from the drain, indicating flow of water within the cell. This occurred in summer and winter. A hypothesis had been proposed to explain this phenomenon based on multiphase flow and heat transport. We corroborate this hypothesis by means of 2D numerical models, using data measured by sensors in the cells and data from laboratory test. There is a good agreement between the data measured and the ones calculated by the models.Postprint (published version

Heat storage efficiency, ground surface uplift and thermo-hydro-mechanical phenomena for high-temperature aquifer thermal energy storage

High-temperature aquifer thermal energy storage (HT-ATES) systems can help in balancing energy demand and supply for better use of infrastructures and resources. The aim of these systems is to store high amounts of heat to be reused later. HT-ATES requires addressing problems such as variations of the properties of the aquifer, thermal losses and the uplift of the surface. Coupled thermo-hydro-mechanical (THM) modelling is a good tool to analyse the viability and cost effectiveness of HT-ATES systems and to understand the interaction of processes, such as heat flux, groundwater flow and ground deformation. The main problem of this modelling is its high computational cost. We propose a dimensional and numerical analysis of the thermo-hydro-mechanical behaviour of a pilot HT-ATES. The results of this study have provided information about the dominant thermo-hydraulic fluxes, evolution of the energy efficiency of the system and the role of the hydraulic and thermal loads generated by the injection and extraction of hot water.We acknowledge the financial support received from the ERANET project HEATSTORE (170153–4401). This project has been subsidized through the ERANET cofund GEOTHERMICA (Project n. 731117), from the European Commission, RVO (the Netherlands), DETEC (Switzerland), FZJ-PTJ (Germany), ADEME (France), EUDP (Denmark), Rannis (Iceland), VEA (Belgium), FRCT (Portugal), and MINECO (Spain). We wish to thank the Department of Research and Universities of the Generalitat de Catalunya by supporting RV with a grant (2021 FI_B 00940).Peer ReviewedPostprint (published version

Reactive transport: a review of basic concepts with emphasis on biochemical processes

Reactive transport (RT) couples bio-geo-chemical reactions and transport. RT is important to understand numerous scientific questions and solve some engineering problems. RT is highly multidisciplinary, which hinders the development of a body of knowledge shared by RT modelers and developers. The goal of this paper is to review the basic conceptual issues shared by all RT problems, so as to facilitate advancement along the current frontier: biochemical reactions. To this end, we review the basic equations to indicate that chemical systems are controlled by the set of equilibrium reactions, which are easy to model, but whose rate is controlled by mixing. Since mixing is not properly represented by the standard advection-dispersion equation (ADE), we conclude that this equation is poor for RT. This leads us to review alternative transport formulations, and the methods to solve RT problems using both the ADE and alternative equations. Since equilibrium is easy, difficulties arise for kinetic reactions, which is especially true for biochemistry, where numerous challenges are open (how to represent microbial communities, impact of genomics, effect of biofilms on flow and transport, etc.). We conclude with the basic eleven conceptual issues that we consider fundamental for any conceptually sound RT effort.This work is part of grants MEDISTRAES III funded by MCIN/AEI/ PID2019-110212RB-C22 and MCIN/AEI/PID2019-110311RB-C21 and Water JPI project MARadentro (PCI2019-103603), and by the Catalan Water Agency through the project RESTORA (CA210/18/00040). IDAEA-CSIC is a Center of Excellence Severo Ochoa (Grant CEX2018-000794-S funded by MCIN/AEI/ 10.13039/501100011033).Peer ReviewedPostprint (published version