Radiographic Characteristics of the Self-Magnetic Pinch Diode at RITS-6 and URSA-Minor.
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This project seeks to determine if (1) inorganic-based ion exchange materials or (2) electrochemical methods in ionic liquids can be exploited to provide effective Am and Cm separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of inorganic-based ion-exchange materials for actinide and lanthanide ions. Furthermore, we seek to determine whether ionic liquids can serve as the electrolyte that would enable formation of higher oxidation states of Am and other actinides. Experiments indicated that pH, presence of complexants and Am oxidation state exhibit significant influence on the uptake of actinides and lanthanides by layered sodium titanate and hybrid zirconium and tin phosphonate ion exchangers. The affinity of the ion exchangers increased with increasing pH. Greater selectivity among Ln(III) ions with sodium titanate materials occurs at a pH close to the isoelectric potential of the ion exchanger. The addition of DTPA decreased uptake of Am and Ln, whereas the addition of TPEN generally increases uptake of Am and Ln ions by sodium titanate. Testing confirmed two different methods for producing Am(IV) by oxidation of Am(III) in ionic liquids (ILs). Experimental results suggest that the unique coordination environment of ionic liquids inhibits the direct electrochemical oxidation of Am(III). The non-coordinating environment increases the oxidation potential to a higher value, while making it difficult to remove the inner coordination of water. Both confirmed cases of Am(IV) were from the in-situ formation of strong chemical oxidizers.
The United States Department of Energy, seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter lived fission products, thereby decreasing the volume of material requiring disposal and reducing the long-term radiotoxicity and heat load of high-level waste sent to a geologic repository. This transmutation of the long lived actinides plutonium, neptunium, americium and curium can be accomplished by first separating them from spent Light Water Reactor fuel using a pyro-metalurgical process, then reprocessing them into new fuel with fresh uranium additions, and then transmuted to short lived nuclides in a liquid metal cooled fast reactor. An important component of the technology is developing actinide-bearing fuel forms containing plutonium, neptunium, americium and curium isotopes that meet the stringent requirements of reactor fuels and materials.
The team will examine how the incorporation of actinide species important for mixed oxide (MOX) and other advanced fuel designs impacts thermodynamic quantities of the host UO 2 nuclear fuel and how Pu, Np, Cm and Am influence oxygen mobility. In many cases, the experimental data is either insufficient or missing. For example, in the case of pure NpO 2 , there is essentially no experimental data on the hyperstoichiometric form it is not even known if hyperstoichiometry NpO 2 ±x is stable. The team will employ atomistic modeling tools to calculate these quantities
This project seeks to determine if inorganic or hybrid inorganic ion-exchange materials can be exploited to provide effective americium and curium separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of the tested ion-exchange materials for actinide and lanthanide ions. During FY13, experimental work focused in the following areas: (1) investigating methods to oxidize americium in dilute nitric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium and (2) synthesis, characterization and testing of ion-exchange materials. Ion-exchange materials tested included alkali titanates, alkali titanosilicates, carbon nanotubes and group(IV) metal phosphonates. Americium oxidation testing sought to determine the influence that other redox active components may have on the oxidation of Am(III).
During FY14, experimental work focused in the following areas: (1) synthesis, characterization and testing of ion-exchange materials and (2) investigating methods to oxidize americium(III) in dilute nitric acid using peroxydisulfate. Ion-exchange materials tested at SRNL included antimony silicates. Inorganic and hybrid ion-exchange materials tested previously in this project are limited to a pH of about 2. In more concentrated acid solutions, the ion-exchange material is chemically unstable or exhibits poor ion-exchange performance for metal ions. FY14 research focused on testing antimony silicates, which had been reported to exhibit good ion-exchange in 0.2 – 1.0 M nitric acid and some ion-exchange capacity in as high as 3 M nitric acid. Performance testing of archived antimony silicate samples from Prof. R. Harjula (U. Helsinki) and freshly prepared samples showed very low affinity for lanthanide ions in 0.1, 1.0 and 3.0 M nitric acid. Tests carried out in FY14 continued work initiated the previous year to understand the effects that Pu(IV) and nitrite have on the oxidation of Am(III) by peroxydisulfate. Findings indicate that both Pu(IV) and nitrite are oxidized by peroxydisulfate. Consequently, an excess of peroxydisulfate is needed to maximize the conversion of Am(III) to Am(V).
Attached are copies of the presentations that will be given by Savannah River National Laboratory participants at the 37th Actinide Separations Conference in Spokane, Washington on June 24 – 27, 2013. This document represents the deliverable for milestone M4FT-13SR0303062, Prepare and present two papers on ion exchange separations at the 2013 Actinide Separations conference. Note that the completion of the milestone was delayed due to the rescheduling of the conference from late May 2013 to late June 2013.
This project was to use light ion beam induced charge (IBIC) to detect damage cascades generated by a single heavy ion, and thereby reveal details of the shape of the cascade and the physics of recombination of carriers that interact with the cluster. Further IBIC measurements using the hardware and software of this project will improve the accuracy of theoretical models used to predict electrical degradation in devices exposed to radiation environments. In addition, future use of light ion IBIC detection of single ion-induced damage could be used to locate single ion implantation sites in quantum computing applications. This project used Sandia's Pelletron and nanoImplanter (nI) to produce heavy ion-induced collision cascades in p-n diodes, simulating cascades made by primary knock-on atoms recoiled by neutrons. Si and Li beams from the nI were used to perform highly focused scans generating IBIC signal maps where regions of lower charge collection efficiency were observed without incurring further damage. The very first use of ion channeled beams for IBIC was explored to maximize ionization, improve contrast and provide very straight line trajectories to improve lateral resolution.
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In work supported by ORP over the past several years, VSL has collected extensive data on LAW glass formulations to increase sulfate and sodium loadings, which are the major waste loading limiting components in LAW. However, there are insufficient data to define acceptable sulfate loadings in LAW glasses in the presence of variable amounts of components such as Cl, F, P and Cr. The present work focused: a) on collecting data on acceptable sulfate loading in the presence of varying amounts of halides (Cl, F) and a fixed amount of Cr; and b) studying the effect of phosphorous on salt formation.