In 2012, the Nuclear Waste Management Organization developed a comprehensive proof test plan (PTP) to evaluate the feasibility and safety of their copper‐coated used fuel container and their novel bentonite buffer box emplacement concept to be employed in its proposed deep geological repository for the long‐term management of used nuclear fuel. Research within the PTP includes several programs to evaluate the possible extent of damage that may be caused by various copper corrosion mechanisms: oxic‐, radiolytic‐, anoxic‐, and sulfide‐induced, with particular attention being paid to the possibility of localization of any of these processes. Programs remain on track to support and refine a maximum copper corrosion allowance of <1.27 mm over a one million year emplacement in a deep geological repository.
1 March 2022 in Journal of the Electrochemical Society
The microstructures of copper (Cu) materials were investigated by electron backscatter diffraction, showing that electrodeposited (ED) Cu has a homogenous polycrystalline microstructure, while cold spray (CS) Cu has a heterogeneous microstructure with varying grain size, pores, and interfacial splat regions. The corrosion rate was examined by corrosion potential (ECORR) and polarization resistance (Rp) measurements on Cu specimens in solutions containing 0.1 M NaCl + 1 × 10−3 M Na2S. Although the as sprayed CS-Cu was the least corrosion resistant, the corrosion rate of the heat-treated CS-Cu was similar to that of the ED-Cu and wrought Cu (SKB-Cu). Electrochemical behaviours of Cu materials were investigated by either a potentiodynamic scan or a potentiostatic polarization at a more positive potential (E > ECORR) for various experiment durations up to 4 h, showing that the heat-treated CS-Cu, SKB-Cu and ED-Cu exhibited very similar behaviour while the as sprayed CS-Cu showed erratic behavior consistent with a variable surface reactivity. Nanoscale scanning transmission electron microscopy analysis has been performed at the cross-section of an anodically-oxidized CS-Cu specimen, revealing a two-layer film structure, mostly composed of Cu sulfide, with a minor diffusion of sulfur in the local area of an interfacial splat boundary tip.
Many countries are in the process of designing a deep geological repository (DGR) for long-term storage of used nuclear fuel. For several designs, used fuel containers will be placed belowground with emplacement tunnels being backfilled using a combination of highly compacted powdered bentonite clay buffer boxes surrounded by a granulated “gapfill” bentonite. To limit the potential for microbiologically influenced corrosion of used fuel containers, identifying conditions that suppress microbial growth is critical for sustainable DGR design. This study investigated microbial communities in powdered and gapfill bentonite clay incubated in oxic pressure vessels at dry densities between 1.1 g cm−3 (i.e. below repository target) and 1.6 g cm−3 (i.e. at or above repository target) as a one-year time series. Our results showed an initial (i.e. 1 month) increase in the abundance of culturable heterotrophs associated with all dry densities less than 1.6 g cm−3, which reveals transient low-pressure conditions associated with the bentonite saturation process. Following saturation, culturable heterotroph abundances decreased to those of starting material by the 6-month time point for all 1.4 and 1.6 g cm−3 pressure vessels, and most probable numbers of culturable sulfate-reducing bacteria (SRB) remained constant for all vessels and time points. The 16S rRNA gene sequencing results showed a change in microbial community composition from the starting material to the one-month time point, after which time most samples were dominated by sequences associated with Pseudomonas, Bacillus, Cupriavidus, and Streptomyces. Similar taxa were identified as dominant members of the culture-based community composition, demonstrating that the dominant members of the clay microbial communities are viable. Members of the spore-forming Desulfosporosinus genus were the dominant SRB for both clay and culture profiles. After initial microbial growth while bentonite was below target pressure in the early phases of saturation, microbial growth in pressure vessels with dry densities of at least 1.4 g cm−3 was eventually suppressed as bentonite neared saturation.
The proposed long‐term management plan for used nuclear fuel is to isolate it within a multiple‐barrier system underground in a deep geological repository (DGR). In the Canadian design, used fuel bundles will be sealed in copper‐coated carbon steel used fuel containers, encased in blocks of bentonite clay, emplaced approximately 500–800 m below ground, and surrounded by a bentonite gapfill material. A laboratory experimental campaign has been undertaken to demonstrate the integrity of the multiple‐barrier system. DGR‐relevant copper materials were embedded in bentonite clay, compacted to various densities, and sealed into a hermetic pressure vessel pressurized with demineralized water. Experiments explored the influence of bentonite compaction in the range of 1100–1600 kg/m3 on copper corrosion over durations of 1–18 months. Postexposure analysis of the copper coupons showed nonhomogeneous corrosion, with corrosion products composed of Cu2O, with some Cu2S. The average corrosion rates decreased as a function of time and increasing bentonite compaction density. In general, we observed that higher bentonite compaction density suppressed the corrosion of embedded copper.
The temperature evolution within a deep geological repository (DGR) is a key design consideration for the safe and permanent storage of the high-level radioactive waste contained inside used nuclear fuel containers (UFCs). Due to the material limitations of engineered components with respect to high temperature tolerance, the Nuclear Waste Management Organization of Canada requires the maximum temperature within a future Canadian DGR to be less than 100 °C. Densely placing UFCs within a DGR is economically ideal, but greater UFC placement density will increase the maximum temperature reached in the repository. This paper was aimed to optimize (i) the separation between UFCs, (ii) the distance between container placement rooms, and (iii) the locations of the age-dependent UFCs in the placement rooms for a conceptual DGR constructed in crystalline rock. Surrogate-based optimization reduced the amount of computationally expensive evaluations of a COMSOL Multiphysics model used to study the temperature evolution within the conceptual DGR and determined optimal repository design points. Via yield optimization, nominal design points that considered uncertainties in the design process were observed. As more information becomes available during the design process for the Canadian DGR, the methods employed in this paper can be revisited to aid in selecting a UFC placement plan and to mitigate risks that may cause repository failure.