Publications

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Deep boreholes could be a relatively inexpensive, safe, and rapidly deployable strategy for disposing Americaś nuclear waste. To study this approach, Sandia invested in a three year LDRD project entitled “Radionuclide Transport from Deep Boreholes.” In the first two years, the borehole reference design and backfill analysis were completed and the supporting modeling of borehole temperature and fluid transport profiles were done. In the third year, some of the logistics of implementing a deep borehole waste disposal system were considered. This report describes what was learned in the third year of the study and draws some conclusions about the potential bottlenecks of system implementation.

This document summarizes a three year Laboratory Directed Research and Development (LDRD) program effort to improve our understanding of algal flocculation with a key to overcoming harvesting as a techno-economic barrier to algal biofuels. Flocculation is limited by the concentrations of deprotonated functional groups on the algal cell surface. Favorable charged groups on the surfaces of precipitates that form in solution and the interaction of both with ions in the water can favor flocculation. Measurements of algae cell-surface functional groups are reported and related to the quantity of flocculant required. Deprotonation of surface groups and complexation of surface groups with ions from the growth media are predicted in the context of PHREEQC. The understanding of surface chemistry is linked to boundaries of effective flocculation. We show that the phase-space of effective flocculation can be expanded by more frequent alga-alga or floc-floc collisions. The collision frequency is dependent on the floc structure, described in the fractal sense. The fractal floc structure is shown to depend on the rate of shear mixing. We present both experimental measurements of the floc structure variation and simulations using LAMMPS (Large-scale Atomic/Molecular Massively Parallel Simulator). Both show a densification of the flocs with increasing shear. The LAMMPS results show a combined change in the fractal dimension and a change in the coordination number leading to stronger flocs.

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The effects of algae concentration, ferric chloride dose, and pH on the flocculation efficiency of the freshwater algae Chlorella zofingiensis can be understood by considering the nature of the electrostatic charges on the algae and precipitate surfaces. Two critical conditions are identified which, when met, result in flocculation efficiencies in excess of 90% for freshwater algae. First, a minimum concentration of ferric chloride is required to overcome the electrostatic stabilization of the algae and promote bridging of algae cells by hydroxide precipitates. At low algae concentrations, the minimum amount of ferric chloride required increases linearly with algae concentration, characteristic of flocculation primarily through electrostatic bridging by hydroxide precipitates. At higher algae concentrations, the minimum required concentration of ferric chloride for flocculation is independent of algae concentration, suggesting a change in the primary flocculation mechanism from bridging to sweep flocculation. Second, the algae must have a negative surface charge. Experiments and surface complexation modeling show that the surface charge of C. zofingiensis is negative above a pH of 4.0±0.3 which agrees well with the minimum pH required for effective flocculation. These critical flocculation criteria can be extended to other freshwater algae to design effective flocculation systems. © 2011 Wiley Periodicals, Inc.

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A coordination chemistry analysis of oil-calcite adhesion allows waterflood chemistry controls over enhanced oil recovery from limestones to be understood. The model relies on temperature-dependent surface complexation models of calcite and oil. The primary electrostatic bridges holding oil to calcite are calculated to be [-COO^-][>CaOH₂⁺], [-COO^-][>COOCa⁺], [>CaSO₄^-][-COOCa⁺] and [-COOCa⁺][>COO^-] (“>” denotes calcite surface groups; “-” denotes polar oil surface groups; Mg²⁺ can substitute for Ca⁺²). The [-COO^-][>CaOH₂⁺] bridge between oil carboxylate and protonated calcite calcium sites is most sensitive to changes in waterflood chemistry. Model calculations predict that increased levels of Ca⁺², Mg⁺², and SO₄^-2, alone or in combination, will increase oil recovery from limestones by decreasing the number of [-COO^-][>CaOH₂⁺] bridges. Divalent cations decrease the local interfacial potential by decreasing the net negative charge on oil carboxylate groups; SO₄^-2 coordinates to protonated calcite calcium sites to decrease charge and electrostatic attraction. Increases in ionic strength should increase adhesion by increasing the net charge on each surface, though the effect will be less on calcite. The model presented here requires no fitting parameters yet accurately reproduces observed oil mobilization trends suggesting the model to be a potentially valuable tool for designing chemistries of waterfloods employed in limestones.

A reference design and operational procedures for the disposal of high-level radioactive waste in deep boreholes have been developed and documented. The design and operations are feasible with currently available technology and meet existing safety and anticipated regulatory requirements. Objectives of the reference design include providing a baseline for more detailed technical analyses of system performance and serving as a basis for comparing design alternatives. Numerous factors suggest that deep borehole disposal of high-level radioactive waste is inherently safe. Several lines of evidence indicate that groundwater at depths of several kilometers in continental crystalline basement rocks has long residence times and low velocity. High salinity fluids have limited potential for vertical flow because of density stratification and prevent colloidal transport of radionuclides. Geochemically reducing conditions in the deep subsurface limit the solubility and enhance the retardation of key radionuclides. A non-technical advantage that the deep borehole concept may offer over a repository concept is that of facilitating incremental construction and loading at multiple perhaps regional locations. The disposal borehole would be drilled to a depth of 5,000 m using a telescoping design and would be logged and tested prior to waste emplacement. Waste canisters would be constructed of carbon steel, sealed by welds, and connected into canister strings with high-strength connections. Waste canister strings of about 200 m length would be emplaced in the lower 2,000 m of the fully cased borehole and be separated by bridge and cement plugs. Sealing of the upper part of the borehole would be done with a series of compacted bentonite seals, cement plugs, cement seals, cement plus crushed rock backfill, and bridge plugs. Elements of the reference design meet technical requirements defined in the study. Testing and operational safety assurance requirements are also defined. Overall, the results of the reference design development and the cost analysis support the technical feasibility of the deep borehole disposal concept for high-level radioactive waste.

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Deep boreholes have been proposed for many decades as an option for permanent disposal of high-level radioactive waste and spent nuclear fuel. Disposal concepts are straightforward, and generally call for drilling boreholes to a depth of three to five kilometers into crystalline basement rocks. Waste is placed in the lower portion of the hole, and the upper several kilometers of the hole are sealed to provide effective isolation from the biosphere. The potential for excellent long-term performance has been recognized in many previous studies. This paper reports updated results of what is believed to be the first quantitative analysis of releases from a hypothetical disposal borehole repository using the same performance assessment methodology applied to mined geologic repositories for high-level radioactive waste. Analyses begin with a preliminary consideration of a comprehensive list of potentially relevant features, events, and processes (FEPs) and the identification of those FEPs that appear to be most likely to affect long-term performance in deep boreholes. Performance assessment model estimates of releases from deep boreholes, and the annual radiation doses to hypothetical future humans associated with those releases, are extremely small, indicating that deep boreholes may be a viable alternative to mined repositories for disposal of both high-level radioactive waste and spent nuclear fuel.

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