科研之友
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摘要
The aim of this study was to obtain evidences regarding the physical and geochemical processes occurring as a result of the combined effects of cementitious materials from the concrete degradation and magnetite from steel corrosion on the bentonite barrier during disposal of high-level radioactive waste. A series of six experiments were done that attempt to reproduce the repository conditions prevailing from 1000 to 3000 years after emplacement of wastes. A lime mortar was used as the source of calcium and alkalinity as this is the presumed reactive product produced during concrete degradation at long-term. Magnetite powder was used to simulate the final corrosion product of cast iron and C-steel under anaerobic conditions. Either a natural FEBEX bentonite or a pretreated "aged" sample, depleted in exchangeable Mg and enriched in K, were used as the swelling clay component. Experiments, with both types of bentonite, were performed simultaneously in cylindrical specimens (50 mm diameter, 25 mm length), confined in a Teflon (R) sleeve/steel case cells. These specimens were composed of cement mortar in contact with compacted bentonite, which was in turn in contact with compressed magnetite powder. They were hydrated with an artificial Na+-Ca(2+)xSO(2)(4-) type Spanish reference clayey formation water for 18 months at 60 degrees C and constant hydraulic pressure applied through the base of the mortar. After dismantling and sampling the specimens, distribution of soluble ions, exchangeable cations and mineralogy were studied in the bentonite by different instrumental techniques. Iron migration or any impact of the corrosion products in the bentonite was not noticeable in the clay. Both, mortar and magnetite acted as sinks of chloride and sulfate. Small quantities of Ca-Al-sulfates and carboaluminates, which can allocate chlorides, were determined near the mortar-bentonite interface. Portlandite dissolved near the bentonite interface and induced the formation of calcium silicates hydrates (C-S-H) phases cementing the clay interface, characterizing a calcium front that was developed from the mortar towards the bentonite. Magnesium silicate hydrates (M-S-H) phases were also concentrated at the interface with mortar in the natural bentonite. It was also determined that natural bentonite has potentially higher buffering capacity attenuating the calcium alkaline front than the pretreated clay. In both cases, a low porosity bentonite-mortar zone was experimentally created at the interface. This type of material should be carefully studied in order to predict the potential for further development of a diffusive alkaline alteration, the radionuclides retention and the consequences in the hydration rate of the unaffected bentonite buffer.
- 出版日期2016-5
