Apatite- and Monazite-Bearing Glass-Crystal Composites for the Immobilization of Low-level Nuclear and Hazardous Wastes

This study demonstrates that glass-crystal composite waste forms can be produced from waste streams containing high proportions of phosphorus, transition metals, and/or halides. The crystalline phases produced in crucible-scale melts include apatite, monazite, spinels, and a Zr-Si-Fe-Ti phase. These phases readily incorporated radionuclide and toxic metals into their crystal structures, while corrosion tests have demonstrated that glass-crystal composites can be up to 300-fold more durable than simulated high-level nuclear waste glasses, such as SRL 202U

The release of technetium from defense waste processing facility glasses

Laboratory tests are being, conducted using two radionuclide-doped Defense Waste Processing, Facility (DWPF) glasses (referred to as SRL 13IA and SRL 202A) to characterize the effects of the glass surface area/solution volume (SN) ratio on the release and disposition of {Tc} and several actinide elements. Tests are being conducted at 90{degrees}C in a tuff ground water solution at SN ratios of 10, 2000, and 20,000 m{sup {minus}1} and have been completed through 1822 days. The formation of certain alteration phases in tests at 2000 and 20,000 m{sup {minus}1} results in an increase in the dissolution rates of both classes. The release of {Tc} parallels that of B and Na under most test conditions and its release increases when alteration phases form. However, in tests with SRL 202A glass at 20,000 ,{sup {minus}1}, the {Tc} concentration in solution decreases coincidentally with an increase in the nitrite/nitrate ratio that indicates a decrease in the solution Eh. This may have occurred due to radiolysis, glass dissolution, the formation of alteration phases, or vessel interactions. Technetium that was reduced from {Tc}(VII) to {Tc}(IV) may have precipitated, thou-h the amount of {Tc} was too low to detect any {Tc}-bearing phases. These results show the importance of conducting long-term tests with radioactive glasses to characterize the behavior of radionuclides, rather than relying on the observed behavior of nonradioactive surrogates

Comparison of the Corrosion Behavior of Tank 51 Sludge-Based Glass and a Nonradioactive Homologue Glass

We are conducting static dissolution tests with a glass made at the Savannah River Technology Center (SRTC) during a demonstration of the Defense Waste Processing Facility (DWPF) process control for remote vitrification [1]. The glass was made with sludge from Tank 5 1, SRL 202 frit, and added soda. This glass is similar to waste glasses being made in the current DWPF campaign. Parallel tests are being conducted with a nonradioactive glass made at ANL having the same composition as the radioactive glass, except without the radionuclides. The radioactive and nonradioactive glasses are referred to as 5lR and 5lS, respectively. The results of these tests provide information pertinent to assessing the long-term corrosion behavior of DWPF glasses, comparing the corrosion behaviors of radioactive and nonradioactive glasses, and characterizing the disposition of radionuclides as the glass corrodes

The release of cesium and the actinides from spent fuel under unsaturated conditions

Tests designed to be similar to the unsaturated and oxidizing conditions expected in the candidate repository at Yucca Mountain are in progress with spent fuel at 90{degree}C. The similarities and the differences in release behavior for {sup 137}Cs during the first 2.6 years and the actinides during the first 1.6 years of testing are presented for tests done with (1) water dripped on the fuel at a rate of 0.075 and 0.75 mL every 3.5 days and (2) in a saturated water vapor environment

Mounding Instability and Incoherent Surface Kinetics

Mounding instability in a conserved growth from vapor is analysed within the framework of adatom kinetics on the growing surface. The analysis shows that depending on the local structure on the surface, kinetics of adatoms may vary, leading to disjoint regions in the sense of a continuum description. This is manifested particularly under the conditions of instability. Mounds grow on these disjoint regions and their lateral growth is governed by the flux of adatoms hopping across the steps in the downward direction. Asymptotically ln(t) dependence is expected in 1+1- dimensions. Simulation results confirm the prediction. Growth in 2+1- dimensions is also discussed.Comment: 4 pages, 4 figure

Solution-borne colloids from drip tests using actinide-doped and fully-radioactive waste glasses

Drip tests designed to replicate the synergistic interactions between waste glass, repository groundwater, water vapor, and sensitized 304L stainless steel in the potential Yucca Mountain Repository have been ongoing in our laboratory for over ten years. Results will be presented from three sets of these drip tests: two with actinide-doped glasses, and one with a fully-radioactive glass. Periodic sampling of these tests have revealed trends in actinide release behavior that are consistent with their entrainment in colloidal material when as-cast glass is reacted. Results from vapor hydrated glass show that initially the actinides are completely dissolved in solution, but as the reaction proceeds, the actinides become suspended in solution. Sequential filtering and alpha spectroscopy of colloid-bearing leachate solutions indicate that more than 80 percent of the plutonium and americium are bound to particles that are captured by a 0. 1 gm filter, while less than 10 percent of the neptunium is stopped by a 0. 1 gm filter. Analytical transmission electron microscopy has been used to examine particles from leachate solutions and to identify several actinide-bearing phases which are responsible for the majority of actinide release during glass corrosion

Growth model with restricted surface relaxation

We simulate a growth model with restricted surface relaxation process in d=1 and d=2, where d is the dimensionality of a flat substrate. In this model, each particle can relax on the surface to a local minimum, as the Edwards-Wilkinson linear model, but only within a distance s. If the local minimum is out from this distance, the particle evaporates through a refuse mechanism similar to the Kim-Kosterlitz nonlinear model. In d=1, the growth exponent beta, measured from the temporal behavior of roughness, indicates that in the coarse-grained limit, the linear term of the Kardar-Parisi-Zhang equation dominates in short times (low-roughness) and, in asymptotic times, the nonlinear term prevails. The crossover between linear and nonlinear behaviors occurs in a characteristic time t_c which only depends on the magnitude of the parameter s, related to the nonlinear term. In d=2, we find indications of a similar crossover, that is, logarithmic temporal behavior of roughness in short times and power law behavior in asymptotic times

An Evaluation of Glass-Crystal Composites For the Disposal of Nuclear and Hazardous Waste Materials

Waste forms made of a glass-crystal composite (GCC) are being evaluated at Argonne National Laboratory for their potential use in the disposal of low-level nuclear and hazardous waste materials. This waste form is being developed within the framework strategy of DOE`s minimum Additive Waste Stabilization (MAWS) Program. The MAWS protocol involves the blending of multiple waste streams to achieve an optimal feed composition, which eliminates the need to use large amounts of additives to produce an acceptable waste form. The GCCs have a particularly useful utility in their ability to incorporate waste streams with high metal contents, including those that contain large amounts of scrap metals, and in their potential for sequestering radionuclide and hazardous constituents in corrosion-resistant mineral phases. This paper reports the results from tests conducted with simulated feeds representative of potential DOE and industry waste streams. Topics addressed include the partitioning of various radioactive and hazardous constituents between the glass and crystalline portions of the waste form, the development of secondary phases on the altered sample surfaces during corrosion testing, and the fate of waste components during corrosion testing, as indicated by elements released to solution and microanalysis of the reacted solid samples

Short-time scaling behavior of growing interfaces

The short-time evolution of a growing interface is studied within the framework of the dynamic renormalization group approach for the Kadar-Parisi-Zhang (KPZ) equation and for an idealized continuum model of molecular beam epitaxy (MBE). The scaling behavior of response and correlation functions is reminiscent of the ``initial slip'' behavior found in purely dissipative critical relaxation (model A) and critical relaxation with conserved order parameter (model B), respectively. Unlike model A the initial slip exponent for the KPZ equation can be expressed by the dynamical exponent z. In 1+1 dimensions, for which z is known exactly, the analytical theory for the KPZ equation is confirmed by a Monte-Carlo simulation of a simple ballistic deposition model. In 2+1 dimensions z is estimated from the short-time evolution of the correlation function.Comment: 27 pages LaTeX with epsf style, 4 figures in eps format, submitted to Phys. Rev.

Crossover effects in the Wolf-Villain model of epitaxial growth in 1+1 and 2+1 dimensions

A simple model of epitaxial growth proposed by Wolf and Villain is investigated using extensive computer simulations. We find an unexpectedly complex crossover behavior of the original model in both 1+1 and 2+1 dimensions. A crossover from the effective growth exponent $\beta_{\rm eff}\!\approx\!0.37$ to $\beta_{\rm eff}\!\approx\!0.33$ is observed in 1+1 dimensions, whereas additional crossovers, which we believe are to the scaling behavior of an Edwards--Wilkinson type, are observed in both 1+1 and 2+1 dimensions. Anomalous scaling due to power--law growth of the average step height is found in 1+1 D, and also at short time and length scales in 2+1~D. The roughness exponents $\zeta_{\rm eff}^{\rm c}$ obtained from the height--height correlation functions in 1+1~D ($\approx\!3/4$) and 2+1~D ($\approx\!2/3$) cannot be simultaneously explained by any of the continuum equations proposed so far to describe epitaxial growth.Comment: 11 pages, REVTeX 3.0, IC-DDV-93-00