Influence of tectonic perturbations on the migration of long-lived radionuclides from an underground repository of radioactive waste

We studied the influence of tectonic perturbations on the transport of potentially mobilized radionuclides in groundwater from a deep-mined repository of solid high-level radioactive waste. The study was carried out by the method of mathematical modeling. Key parameters of the model correspond to the site of a potential federal repository in Russia. The groundwater flow domain is delimited on one side by a water divide (i.e., boundary of the catchment basin) and on the other side by the river bank. 2D simulations of groundwater flow and radionuclide migration are carried out along a vertical cross-section normal to the water divide. The groundwater flows through the rock massif, which encloses the repository, and discharges into the adjacent river. It is supposed that tectonic activity may form a fault which is parallel to the river bank. We analyzed how repository safety depends on the time of the fault emergence and on the distance between the repository and the fault. The results of our simulations suggest that: (1) emergence of a fault due to tectonic perturbations is not inevitably associated with a substantial growth of radionuclides released from the repository to the environment; (2) influence of the fault on the repository safety depends on the distance between the fault and the repository as well as on the time interval between the repository development and the fault emergence; (3) the influence of the fault on the repository safety can depend substantially on local elevations of the relief at the repository site

Calibration of Hydrodynamic Models of Groundwater Flow in Aquifers Polluted by Liquid Radioactive Waste

Pollution of aquifers by liquid radioactive waste is especially hazardous due to high permeability of aquifer rocks. Pollution can take place as a result of deep injection disposal of liquid waste or due to its leakage from a surface reservoir. The ecological hazard depends on distribution of aquifer permeability, which can be highly heterogeneous. The only source of data for determination of such distribution is measurements in exploratory boreholes at the polluted site. A technique is proposed for determination of spatial distribution of aquifer transmissibility on the basis of hydrological measurements in a limited number of boreholes. The problem is reduced to a minimization problem which was solved numerically

Modification of Pulse Decay Method for Determination of Permeability of Crystalline Rocks

An improvement of the pulse decay method of rock permeability measurement is presented. The technique is based on fitting experimental data to analytical and numerical solutions of the filtration equations derived with regard to the variation of flowing gas properties with temperature and pressure. A special apparatus and software for the implementation of this method were developed. A single experiment in which gas is used as a flowing medium enables determining both the permeability of a sample to water and the Klinkenberg constant. The permeability measurements on the samples of different types of rock with various reservoir properties were carried out and demonstrated satisfactory accuracy and efficiency of the method. An effective method for anisotropic permeability measurement is proposed as a development of this technique

Thermal Effects and Glass Crystallization in Composite Matrices for Immobilization of the Rare-Earth Element–Minor Actinide Fraction of High-Level Radioactive Waste

The current policy of managing high-level waste (HLW) derived in the closed nuclear fuel cycle consists in their vitrification into B-Si or Al-P vitreous forms. These compounds have rather limited capacity with respect to the HLW (5–20 wt%), and their properties change over time due to devitrification of the glasses. Cardinal improvement in the management of HLW can be achieved by their separation onto groups of elements with similar properties, followed by their immobilization in robust waste forms (matrices) and emplacement in deep disposal facilities. One of the possible fractions contains trivalent rare-earth elements (REEs) and minor actinides (MAs = Am and Cm). REEs are the fission products of actinides, which are mainly represented by stable isotopes of elements from La to Gd as well as Y. This group also contains small amounts of short-lived radionuclides with half-lives (T1/2) from 284 days (144Ce) to 90 years (151Sm), including 147Pm (T1/2 = 2.6 years), 154Eu (T1/2 = 8.8 years), and 155Eu (T1/2 = 5 years). However, the main long-term environmental hazard of the REE–MA fraction is associated with Am and Cm, with half-lives from 18 years (244Cm) to 8500 years (245Cm), and their daughter products: 237Np (T1/2 = 2.14 × 106 years), 239Pu (T1/2 = 2.41 × 104 years), 240Pu (T1/2 = 6537 years), and 242Pu (T1/2 = 3.76 × 105 years), which should be immobilized into a durable waste form that prevents their release into the environment. Due to the heat generated by decaying radionuclides, the temperature of matrices with an REE–MA fraction will be increased by hundreds of centigrade above ambient. This process can be utilized by selecting a vitreous waste form that will crystallize to form durable crystalline phases with long-lived radionuclides. We estimated the thermal effects in a potential REE–MA glass composite material based on the size of the block, the content of waste, the time of storage before immobilization and after disposal, and showed that it is possible to select the waste loading, size of blocks, and storage time so that the temperature of the matrix during the first decades will reach 500–700 °C, which corresponds to the optimal range of glass crystallization. As a result, a glass–ceramic composite will be produced that contains monazite ((REE,MA)PO4) in phosphate glasses; britholite (Cax(REE,MA)10-x(SiO4)6O2) or zirconolite ((Ca,REE,MA)(Zr,REE,MA)(Ti,Al,Fe)2O7), in silicate systems. This possibility is confirmed by experimental data on the crystallization of glasses with REEs and actinides (Pu, Am). The prospect for the disposal of glasses with the REE–MA fraction in deep boreholes is briefly considered

Influence of Rock Structure on Migration of Radioactive Colloids from an Underground Repository of High-Level Radioactive Waste

Studies of leaching of vitrified simulated high-level radioactive waste (HLW) evidence that most of actinides or their simulators enter leaching water in a colloidal form. In this paper, we consider a mechanism of colloid-facilitated migration of radionuclides from an underground repository of HLW located at a depth of a few hundreds of meters in fractured crystalline rocks. The comparison between data of field and laboratory measurements showed that the bulk permeability of the rock massif in field tests is much greater than the permeability of rock samples in laboratory experiments due to an influence of a network of fractures in the rock massif. Our theoretical analysis presents evidence that this difference can take place even in a case when the network is not continuous, and the fractures are isolated with each other through a porous low-permeable matrix of the rock. Results of modelling revealed a possibility of mechanical retention of radionuclide-bearing colloid particles in the frame of rock during their underground migration

Zirconolite Matrices for the Immobilization of REE–Actinide Wastes

The structural and chemical properties of zirconolite (ideally CaZrTi2O7) as a host phase for separated REE–actinide-rich wastes are considered. Detailed analysis of both natural and synthetic zirconolite-structured phases confirms that a selection of zirconolite polytype structures may be obtained, determined by the provenance, crystal chemistry, and/or synthesis route. The production of zirconolite ceramic and glass–ceramic composites at an industrial scale appears most feasible by cold pressing and sintering (CPS), pressure-assisted sintering techniques such as hot isostatic pressing (HIP), or a melt crystallization route. Moreover, we discuss the synthesis of zirconolite glass ceramics by the crystallization of B–Si–Ca–Zr–Ti glasses containing actinides in conditions of increased temperatures relevant to deep borehole disposal (DBD)