Seismogeological acceptance criteria for geological repositories for spent nuclear fuel

Qualitative geological acceptance criteria and quantitative seismological acceptance criteria for radioactive waste disposals are developed. The background material for the initiation of site selection and for its earthquake hazard assessment is discussed. The recent movements of the Earth's surface as well as the other mechanical properties of geological media, hydrological conditions of geological blocks, their groundwater chemistry, geochemical rheology, petrological analyses of rocks, etc., have to be taken into account. A new comprehensive integrated safety analysis of the final underground disposal of spent nuclear fuel has been underway in the Czech Republic since 1991. In accordance with these seismogeological acceptance criteria regions for building underground final radioactive waste disposals are singled out in the Czech Republic.     

Site selection criteria for the disposal of spent nuclear fuel in Romania

 Common opinion today is that the only practicable way for the disposal of hazardous waste is in deep-laying bedrock deposits. A set of general site selection criteria for spent nuclear fuel were developed, and are presented and discussed in this paper. Four widespread geological formations in Romania appropriate as geological barriers for underground disposal (salt, granite, volcanic tuff and green schists) were analyzed, and sites were proposed on the basis of the geological criteria defined for each of the four formations. Received: 18 July 1996 · Accepted: 27 September 1996     

The uranium ore from Mina Fe (Salamanca, Spain) as a natural analogue of processes in a spent fuel repository

In the frame of the ENRESA natural analogue programme, the uranium ore from the “Mina Fe” (Salamanca, Spain) has been studied as a natural analogue of radioactive spent fuel behaviour. This uranium mine is hosted in highly fractured schistose rocks, a geological setting that has not been envisaged in the Spanish options for radioactive waste burial. However, some analogies with the processes that might be involved in the evolution of these geological repositories suggested this investigation.

The pitchblende–pyrite–carbonate paragenesis has been studied “in situ” as natural analogue of the nuclear spent fuel behaviour under extremely oxidative dissolution conditions. Similarly, secondary Fe oxyhydroxides and clay minerals have also been considered as relevant analogue materials for the retention of uranium and other analogous trace metals. A multidisciplinary characterisation of the site has been performed in order to study these processes.

Though the intense mining activities in the site hindered precise determination of the original hydrogeological and hydrochemical features of the investigated zone (Boa fault zone), the mineralogy and geochemistry of fracture fillings, mineralisation and associated clayey materials have allowed the geochemical evolution of the system to be established. Three geochemical zones have been clearly differentiated: (i) the oxidised zone, from the surface to approximately 20 m depth, (ii) the redox transition zone, from 20 to 50 m depth, and (iii) the reduced zone, located below the transition zone.

The oxidised zone is characterised by the presence of the typical mineral association resulting from the strong acid conditions caused by the total oxidation of pyrite and other sulphides. The total oxidation, dissolution and leaching of U(IV), as uranyl–sulphate aqueous complexes, prevailed in this oxidised zone. The redox transition zone is characterised by the coexistence of the primary uranium paragenesis, oxidised minerals, as well as numerous secondary solid phases as a result of the physico-chemical changes in the environment. The optimal physico-chemical conditions for the coffinitisation of pitchblende and the co-precipitation of Fe(III)–U(VI) took place in this zone. In the reduced zone, where the primary uranium paragenesis is present, we currently find the necessary physico-chemical conditions to stabilise pitchblende, pyrite and carbonates.

The physico-chemical conditions of the oxidised zone are not relevant to disposal conditions. In the transition zone, two main geochemical processes take place: (i) the coffinitisation of pitchblende, which may be an important process for the stability of spent fuel in reducing conditions, and (ii) the co-precipitation of the Fe(III) and U(VI) as oxyhydroxides, another relevant mechanism for the retention of uranium. The physico-chemical conditions that prevail below 50 m depth should be sufficient to stabilise a spent nuclear fuel repository, in the same way as they have been able to preserve the 34-Ma-old uranium deposit of the Mina Fe.     

Implementation of microbial processes in the performance assessment of spent nuclear fuel repositories

Present strategies for the long-term disposal of high-level nuclear wastes are based on the construction of repositories hundreds of meters below the earth surface. Although the surrounding host-rocks are relatively isolated from the light at the earth surface they are by no means lifeless. Microorganisms rule the deep part of the biosphere and it is well established that their activity can alter chemical and physical properties of these environments. Microbial processes can directly and indirectly affect radionuclide migration in multiple ways. Within 6th FP IP FUNMIG the interplay between microbial biofilms and radionuclides and the effect of microbially induced redox transformations of Fe on radionuclide mobility have been investigated. For the first time, formation of U(V) as a consequence of microbial U(VI) reduction in a multi-species biofilm was detected in vivo by combining laser fluorescence spectroscopy and confocal laser scanning microscopy. Furthermore, it was demonstrated that addition of U(VI) can lead to increased respiratory activity in a biofilm. Increased respiration in a biofilm can create microenvironments with lower redox potential, and hence induce reduction of radionuclides. Transient mobilization of U was observed in experiments with Fe oxides containing adsorbed U(VI) in which the activity of SO₄-reducing organisms was mimicked by sulfide addition. Faster reaction of sulfide with Fe oxides compared to U(VI) reduction, and decreasing U(VI) adsorption due to the transformation of Fe oxides into FeS can explain the observed intermittent U mobilization. The presented research on microbe-radionuclide interactions performed within FUNMIG addresses only a few aspects of the potential role of microorganisms in the performance assessment of nuclear waste repositories. For this reason, additionally, this article provides a cursory overview of microbial processes which were not studied within the FUNMIG project but are relevant in the context of performance assessment. The following aspects are presented: (a) the occurrence and metabolic activity of microorganisms of several proposed types of host-rocks, (b) the potential importance of microorganisms in the near-field of nuclear waste repositories, (c) indirect effects of microbial processes on radionuclide mobility in the repository far-field, (d) binding of radionuclides to microbial biomass, (e) microbial redox transformations of radionuclides, and (f) the implementation of microbial processes in reactive transport models for radionuclide migration.     

Scoping analyses of the coupled thermal-hydrological-mechanical behaviour of the rock mass around a nuclear fuel waste repository

Scoping calculations were performed in order to assess the influence of radiogenic heat on the performance of the rock mass around a nuclear fuel waste repository. The full coupling between the thermal, mechanical and hydrological processes involved was considered by using the finite element code, FRACON, developed through an extension of Biot's classical theory of soil consolidation. By considering the full T---H---M coupling, several important safety features, which would otherwise be omitted in uncoupled analyses, were detected in the present study. In particular, it was shown that the heat-induced pore pressure increase around the repository has the potential to significantly increase the rate of groundwater flow, and affect the structural integrity of the rock mass.     

A case study on the influence of THM coupling on the near field safety of a spent fuel repository in sparsely fractured granite

In order to demonstrate the feasibility of geological disposal of spent CANDU fuel in Canada, a safety assessment was performed for a hypothetical repository in the Canadian Shield. The assessment shows that the maximum long term radionuclide release from such repository would meet international criteria for dose rate; however, uncertainties in the assumed evolution of the repository were identified. Such uncertainties could be resolved by the consideration of coupled Thermal-Hydro-Mechanical-Chemical (THMC) processes. In Task A of the DECOVALEX-THMC project, THM models were developed within the framework of the theory of poroelasticity. Such model development was performed in an iterative manner, using experimental data from laboratory and field tests. The models were used to perform near-field simulations of the evolution of the repository in order to address the above-mentioned uncertainties. This paper presents the definition and rationale of task A and the results of the simulations. From a repository safety point of view, the simulations predict that the maximum temperature would be well below the design target of 100°C; however, the stress on the container can marginally exceed the design value of 15 MPa. However, the most important finding from the simulations is that a rock damage zone could form around the emplacement borehole. Such damage zone can extend a few metres from the walls of the emplacement holes, with permeability values that are orders of magnitude higher than the initial values. The damage zone has the potential to increase the radionuclide transport flux from the geosphere; the effect of such an increase should be taken into account in the safety assessment and mitigated if necessary by the provision of sealing systems. Prepared for publication in Environmental Geology. DECOVALEX-THMC Special Issue.     

Geologic uncertainty in a regulatory environment: An example from the potential Yucca Mountain nuclear waste repository site

Regulatory geologists are concerned with predicting the performance of sites proposed for waste disposal or for remediation of existing pollution problems. Geologic modeling of these sites requires large-scale expansion of knowledge obtained from very limited sampling. This expansion induces considerable uncertainty into the geologic models of rock properties that are required for modeling the predicted performance of the site.One method for assessing this uncertainty is through nonparametric geostatistical simulation. Simulation can produce a series of equiprobable models of a rock property of interest. Each model honors measured values at sampled locations, and each can be constructed to emulate both the univariate histogram and the spatial covariance structure of the measured data. Computing a performance model for a number of geologic simulations allows evaluation of the effects of geologic uncertainty. A site may be judged acceptable if the number of failures to meet a particular performance criterion produced by these computations is sufficiently low. A site that produces too many failures may be either unacceptable or simply inadequately described.The simulation approach to addressing geologic uncertainty is being applied to the potential high-level nuclear waste repository site at Yucca Mountain, Nevada, U.S.A. Preliminary geologic models of unsaturated permeability have been created that reproduce observed statistical properties reasonably well. A spread of unsaturated groundwater travel times has been computed that reflects the variability of those geologic models. Regions within the simulated models exhibiting the greatest variability among multiple runs are candidates for obtaining the greatest reduction in uncertainty through additional site characterization.     

Vertical distribution, stability and evolution of groundwater composition in granite suitable for storage of spent nuclear fuel

Granite with extremely low permeability has been selected to host a repository of spent nuclear fuel in the Czech Republic. Three boreholes were drilled in a test site of the Podlesi granite stock in the Krusne hory Mts. The holes were located 10 m apart. After hydraulic tests, four sections in one of the boreholes were separated by packers at depth of 69-111, 111-161, 161-220 and 220-300 m. Samples of groundwater from each section were periodically collected for chemical and isotopic analysis. Groundwater from fractures in the granite stock does not belong to a single and uniform groundwater body in spite of that the granite is chemically and mineralogically homogeneous. There are three water bodies, which are only partly hydraulically connected. They are： （1） The groundwater in the oxidation zone to a depth of about 111 m. （2） The groundwater of the zone of hydrolysis of alumosilicates from 111 to 220 m. （3） The groundwater of the zone of hydrolysis of alumosilicates below the depth of 220 m from a different fracture system than the water from the above sections. The total dissolved solids of water increase with depth. The Ca-SO4 component predominates in the near surface water body while Na-HCO3 component predominates in the two deeper water bodies. Water from the oxidation zone contains higher concentrations of iron and other trace metals. The chemical composition of water in the three water bodies changed during the 14 months of sampling. No steady state was reached during this time. The changes displayed systematic trends. The ratio Ca/Na increased and the ratio HCO3/SO4 decreased with time in the shallow water body. In contrast, the ratio CafNa decreased and HCO3/SO4 fluctuated without an obvious trend in the deeper water bodies. An unusually high concentration of dissolved organic carbon （DOC） was found in the lowest section of the test borehole. The concentration of DOC was 150 mg/L at the beginning of sampling. The isotopic composition was δ^13C=-27.6 ‰. The concentration of DOC dropped both towards the surface and with time.     

核废料储库周边介质热力耦合数值分析

以热力学和热弹性理论为基础,分析热-力相互耦合作用及其对热特性参数和力特性参数的影响。建立了非等温条件下的耦合作用控制方程,给出了相应的空间离散和时间离散形式。利用有限元法对一核废料储库的平面问题进行了计算,讨论了储库周围粘性土介质内温度场、应力场等的动态发展变化规律,并分析了耦合效应对计算结果的影响。研究表明,随时间的增长,热能由储库边壁不断向远处传导和扩散,而在空间上又处于不断变化的非等温状态,这一动态变化过程必然会诱致周围土介质内应力的产生和发展,并随温度的变化而不断变化。     

Modelling groundwater contamination above a nuclear waste repository at Gorleben, Germany

The candidate repository for high-level nuclear waste in the Gorleben salt dome, Germany, is expected to host 8,550 tonnes of uranium in burnt fuel. It has been proposed that 5,440 waste containers be deposited at a depth of about 800?m. There is 260?C280?m of siliciclastic cover sediments above the proposed repository. The potential groundwater contamination in the siliciclastic aquifer is simulated with the TOUGHREACT and TOUGH2-MP codes for a three-dimensional model with 290,435 elements. Two deterministic cases are simulated. The single-phase case considers the transport of radionuclides in the liquid phase only. The two-phase case accounts for hydrogen gas generated by the corrosion of waste containers and release of gaseous C-14. The gas release via a backfilled shaft is assumed to be steady (non-explosive). The simulation period is 2,000,000 years for the single-phase case and 7,000 years for the two-phase case. Only the radioactive dose in the two-phase case is higher than the regulatory limit (0.1?mSv/a).     

On persistent primary variables for numerical modeling of gas migration in a nuclear waste repository

Numerical simulation of gas migration driven by compressible two-phase partially miscible flow in porous media is of major importance for safety assessment of deep geological repositories for long-lived high-level nuclear waste. We present modeling of compositional liquid and gas flow for numerical simulations of hydrogen migration in deep geological radioactive waste repository based on persistent primary variables. Two-phase flow is considered, with incompressible liquid and compressible gas, which includes capillary effects, gas dissolution, and diffusivity. After discussing briefly the existing approaches to deal with phase appearance and disappearance problem, including a persistent set of variables already considered in a previous paper (Bourgeat et al., Comput Geosci 13(1):29–42, 2009), we focus on a new variant of the primary variables: dissolved hydrogen mass concentration and liquid pressure. This choice leads to a unique and consistent formulation in liquid saturated and unsaturated regions, which is well adapted to heterogeneous media. We use this new set of variable for numerical simulations and show computational evidences of its adequacy to simulate gas phase appearance and disappearance in different but typical situations for gas migration in an underground radioactive waste repository.     

Corrosion-induced gas generation in a nuclear waste repository: Reactive geochemistry and multiphase flow effects

Corrosion of steel canisters, stored in a repository for spent fuel and high-level nuclear wastes, leads to the generation and accumulation of H₂ gas in the backfilled emplacement tunnels, which may significantly affect long-term repository safety. Previous studies have used H₂ generation rates based on the volume of the waste or canister material and the stoichiometry of the corrosion reaction. However, Fe corrosion and H₂ generation rates vary with time, depending on factors such as amount of Fe, water availability, water contact area and aqueous and solid chemistry. To account for these factors and feedback mechanisms, a chemistry model was developed related to Fe corrosion, coupled with two-phase (liquid and gas) flow phenomena that are driven by gas-pressure buildup associated with H₂ generation and water consumption. Results indicate that by dynamically calculating H₂ generation rates based on a simple model of corrosion chemistry, and by coupling this corrosion reaction with two-phase flow processes, the degree and extent of gas-pressure buildup could be much smaller compared to a model that neglects the coupling between flow and reactive transport mechanisms. By considering the feedback of corrosion chemistry, the gas pressure increases initially at the canister, but later decreases and eventually returns to a stabilized pressure that is slightly higher than the background pressure. The current study focuses on corrosion under anaerobic conditions for which the coupled hydrogeochemical model was used to examine the role of selected physical parameters on H₂ gas generation and corresponding pressure buildup in a nuclear waste repository. The developed model can be applied to evaluate the effect of water and mineral chemistry of the buffer and host rock on the corrosion reaction for future site-specific studies.     

The potential effect of cementitious colloids on radionuclide mobilisation in a repository for radioactive waste

Colloid-facilitated transport of contaminants could enhance the release rate of radionuclides from the cementitious near field of a repository for radioactive waste. In the current design of the planned Swiss repository for intermediate-level radioactive waste, a gas-permeable mortar is employed as backfill material for the engineered barrier. The main components of the material are hardened cement paste (HCP) and quartz aggregates. The chemical condition in the backfill mortar is controlled by the highly alkaline cement pore water present in the large pore space. The interaction of pore water with the quartz aggregates is expected to be the main source for colloids. Colloid transport is facilitated due to the high porosity of the backfill mortar. Batch-type studies have been performed to generate colloidal material in systems containing crushed backfill mortar or quartz in contact with artificial cement pore water (ACW) at pH 13.3. The chemical composition of the colloidal material corresponds to that of calcium silicate hydrates (CSH). Batch flocculation tests show that, after about 20 days reaction time, the concentration of the CSH-type colloids is typically below 0.1 mg l⁻¹ due to reduced colloid stability in ACW. Uptake studies with Cs(I), Sr(II) and Th(IV) on a CSH phase (initial C:S ratio=1.09) have been carried out to assess the sorption properties of the colloidal material. The influence of uptake by colloids on radionuclide mobilisation is expressed in terms of sorption reduction on the immobile phase (HCP). Sorption reduction factors can be estimated on the assumption that the sorption properties of the colloidal material are either similar to those of the CSH phase or HCP, and that sorption is linear and reversible. A scaling factor accounts for the higher specific surface area of the colloidal material compared to the CSH phase and HCP. At colloid concentration levels typically encountered in highly alkaline cement pore waters, colloid-induced sorption reduction is predicted to be negligibly small even for strongly sorbing radionuclides, such as Th(IV). Thus, no significant impact of cementitious colloids on radionuclide mobilisation in the porous backfill mortar is anticipated.