Removal of Technetium, Carbon Tetrachloride, and Metals from DOE Properties

The objective of this research is to prepare, characterize, and evaluate new materials for the removal of technetium (Tc) compounds, halogenated organics, and other troublesome metals from DOE waste streams and contaminated areas. This work follows the discovery that a nanoscale form of zero-valent iron, dispersed on high surface area supports, reduces metal ions (Cr, Hg, Pb, Cd) and Re (as a surrogate for Tc) to insoluble forms much faster than does unsupported iron. The scientific goals of the project are to better understand the mechanism of the reduction process, to develop supports that are compatible with a variety of mixed waste compositions, and to develop surface modifiers for supported iron that will optimize selectivity for the contaminants of interest. The support composition is of particular interest in the case of Tc separation and stabilization in the Hanford tank wastes. While tests with tank waste simulants have shown that pertechnetate is reduced insoluble TcO2, the support material must be compatible with the vitrification process used in the final waste disposition. The surface modifications are also a focal point for Hanford applications because of the complex and variable makeup of the tank wastes

Zirconia-Based Compositions for Use in Passive NO\u3csub\u3ex\u3c/sub\u3e Adsorber Devices

A passive NOx adsorbent includes: palladium, platinum or a mixture thereof and a mixed or composite oxide including the following elements in percentage by weight, expressed in terms of oxide: 10-90% by weight zirconium and 0.1-50% by weight of least one of the following: a transition metal or a lanthanide series element other than Ce. Although the passive NOx adsorbent can include Ce in an amount ranging from 0.1 to 20% by weight expressed in terms of oxide, advantages are obtained particularly in the case of low-Ce or a substantially Ce-free passive NOx adsorbent

Sulfur Partitioning During Vitrification of INEEL Sodium Bearing Waste: Status Report

The sodium bearing tank waste (SBW) at Idaho National Engineering and Environmental Laboratory (INEEL) contains high concentrations of sulfur (roughly 5 mass% of SO3 on a nonvolatile oxide basis). The amount of sulfur that can be feed to the melter will ultimately determine the loading of SBW in glass produced by the baseline (low-temperature, joule-heated, liquid-fed, ceramic-lined) melter. The amount of sulfur which can be fed to the melter is determined by several major factors including: the tolerance of the melter for an immiscible salt layer accumulation, the solubility of sulfur in the glass melt, the fraction of sulfur removed to the off-gas, and the incorporation of sulfur into the glass up to it?s solubility limit. This report summarizes the current status of testing aimed at determining the impacts of key chemical and physical parameters on the partitioning of sulfur between the glass, a molten salt, and the off-gas

Removal of pertechnetate from simulated nuclear waste streams using supported zerovalent

The application of nanoparticles of predominantly zerovalent iron (nanoiron), either unsupported or supported, to the separation and reduction of pertechnetate anions (TcO 4 -) from complex waste mixtures was investigated as an alternative approach to current waste-processing schemes. Although applicable to pertechnetate-containing waste streams in general, the research discussed here was directed at two specific potential applications at the U.S. Department of Energy's Hanford Site: (1) the direct removal of pertechnetate from highly alkaline solutions, typical of those found in Hanford tank waste, and (2) the removal of dilute pertechnetate from near-neutral solutions, typical of the eluate streams from commercial organic ion-exchange resins that may be used to remediate Hanford tank wastes. It was envisioned that both applications would involve the subsequent encapsulation of the loaded sorbent material into a separate waste form. A high surface area (>200 m 2 /g) base-stable, nanocrystalline zirconia was used as a support for nanoiron for tests with highly alkaline solutions, while a silica gel support was used for tests with near-neutral solutions. It was shown that after 24 h of contact time, the high surface area zirconia supported nanoiron sorbent removed about 50% (K d ) 370 L/kg) of the pertechnetate from a pH 14 tank waste simulant containing 0.51 mM TcO 4 -and large concentrations of Na + , OH -, NO 3 -, and CO 3 2-for a phase ratio of 360 L simulant per kg of sorbent. It was also shown that after 18 h of contact time, the silica-supported nanoiron removed >95% pertechnetate from a neutral pH eluate simulant containing 0.076 mM TcO 4 -for a phase ratio of 290 L/kg. It was determined that in all cases, nanoiron reduced the Tc(VII) to Tc(IV), or possibly to Tc(V), through a redox reaction. Finally, it was demonstrated that a mixture of 20 mass % of the solid reaction products obtained from contacting zirconia-supported nanoiron with an alkaline waste solution containing Re(VII), a surrogate for Tc(VII), with 80 mass % alkali borosilicate based frit heat-treated at 700°C for 4 h sintered into an easily handled glass composite waste form