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In Sweden the encapsulated nuclear waste will be surrounded by compacted bentonite in the granitic host rock. In contact with water-bearing fractures the bentonite barrier may release montmorillonite colloids that may be further transported in groundwater. If large amounts of material are eroded from the barrier, the buffer functionality can be compromised. Furthermore, in the scenario of a leaking canister, strongly sorbing radionuclides, can be transported by montmorillonite colloids towards the biosphere. This thesis addresses the effects of groundwater chemistry on the generation, stability, sorption and transport of montmorillonite colloids in water bearing rock fractures. To be able to predict quantities of montmorillonite colloids released from the bentonite barrier in contact with groundwater of varying salinity, generation and sedimentation test were performed. The aim is first to gain understanding on the processes involved in colloid generation from the bentonite barrier. Secondly it is to test if concentration gradients of montmorillonite colloids outside the barrier determined by simple sedimentation experiments are comparable to generation tests. Identical final concentrations and colloid size distributions were achieved in both types of tests. Colloid stability is strongly correlated to the groundwater chemistry. The impact of pH, ionic strength and temperature was studied. Aggregation kinetics experiments revealed that for colloid aggregation rate increased with increasing ionic strength. The aggregation rate decreased with increasing pH. The temperature effect on montmorillonite colloid stability is pH-dependent. At pH≤4, the rate constant for colloid aggregation increased with increasing temperature, regardless of ionic strength. At pH≥10, the aggregation rate constant decreased with increasing temperature. In the intermediate pH interval, the aggregation rate constant decreased with increasing temperature except at the highest ionic strength, where it increased. The relationship between the rate constant and the ionic strength allowed the critical coagulation concentration (CCC) for Na- and Ca-montmorillonite to be determined. In order to distinguish the contribution of physical filtration and sorption to colloid retention in transport, the different retention mechanisms were quantified. Sorption on different representative minerals in granite fractures was measured for latex colloids (50, 100, 200 nm) and montmorillonite colloids as a function of ionic strength and pH. Despite of the negative charge in mineral surfaces and colloids, sorption was detected. The sorption is correlated to the mineral point of zero charge and the zeta potential of the colloids, and increases with increasing ionic strength and decreasing pH. In transport experiments with latex colloids in columns packed with fracture filling material, the retention by sorption could clearly be seen. In particular at low flow rates, when the contact time for colloids with the mineral surfaces were the longest, sorption contributed to retention of the transport significantly. The retention of latex colloids appeared to be irreversible in contrary to the reversible montmorillonite colloid retention. Generation, stability and sorption of the montmorillonite colloids are controlled by electrostatic forces; hence, the results were in qualitative agreement with DLVO.

Doctoral Dissertation, Ph.D., University of California, Berkeley, Berkeley, California, USA. / Published through the Information Bridge: DOE Scientific and Technical Information. "LBNL--56749" Folden III, Charles Marvin. USDOE Director. Office of Science. Office of Nuclear Physics 11/04/2004. Report is also available in paper and microfiche from NTIS.

This thesis pertains to two R&D objectives associated with deploying TMFD sensor technology for meeting AARST-NRPP metrics for Radon (Rn) in-air detection, as well as for monitoring of ultra-trace actinides in air, amidst other Rn-progeny alpha emitting radionuclides. A challenge has persisted over the past 40+ years for detecting trace actinides in air amidst a 100-1000x higher Rn-progeny background. This thesis had a primary aim for addressing this challenge, and developing and assessing for a novel technology solution. Both objectives were successfully met. Methods, designs, and experimental effects of apparatus are discussed for successful Rn and progeny detection for 1-100 pCi/L concentration levels, as well as for Rn-progeny “blind” spectroscopic detection of 10-12 μCi/cc concentrations of actinides (Pu/U/Am) in air. The resulting CTMFD based technology was compared with the state-of-art “Alpha Sentry” CAM system and found to offer superior performance in multiple categories, and ~18x improvement in time to detect (e.g. at 0.02 DAC in 3 hrs vs ~70 hrs for state-of-art) for actinides while also remaining ~100% blind to ~102x higher Rn-progeny background; and, with 1 keV energy resolution vs ~300-400 keV for Alpha Sentry.

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Thesis (Ph.D.); Submitted to the UNIVERSITY OF CALIFORNIA, BERKELEY, CA (US); 9 Dec 2004. / Published through the Information Bridge: DOE Scientific and Technical Information. "LBNL--56744" Guo, Fanqing. USDOE Director. Office of Science. Office of Nuclear Physics (US) 12/09/2004. Report is also available in paper and microfiche from NTIS.