Decomposition of Rare Earth Loaded Resin Particles

The Fuel Cycle R and D (FCR and D) program within the Department of Energy Office of Nuclear Energy (DOE-NE) is evaluating nuclear fuel cycle options, including once-through, modified open, and fully closed cycles. Each of these scenarios may utilize quite different fuel management schemes and variation in fuel types may include high thermal conductivity UO{sub 2}, thoria-based, TRISO, metal, advanced ceramic (nitride, carbide, composite, etc.), and minor actinide (MA) bearing fuels and targets. Researchers from the US, Europe, and japan are investigating methods of fabricating high-specific activity spherical particles for fuel and target applications. The capital, operating, and maintenance costs of such a fuel fabrication facility can be significant, thus fuel synthesis and fabrication processes that minimize waste and process losses, and require less footprint are desired. Investigations have been performed at the Institute for Transuranium Elements (ITU) and the French Atomic Energy Commission (CEA) studying the impact of americium and curium on the fuel fabrication process. proof of concept was demonstrated for fabrication of MA-bearing spherical particles, however additional development will be needed for engineering scale-up. Researchers at the Paul Scherer Institute (PSI) and the Japan Atomic Energy Association (JAEA) have collaborated on research with ceramic-metallic (CERMET) fuels using spherical particles as the ceramic component dispersed in the metal matrix. Recent work at the CEA evaluates the burning of MA in the blanket region of sodium fast reactors. There is also interest in burning MA in Canada Deuterium Uranium (CANDU) reactors. The fabrication of uranium-MA oxide pellets for a fast reactor blanket or MA-bearing fuel for CANDU reactors may benefit from a low-loss dedicated footprint for producing MA-spherical particles. One method for producing MA-bearing spherical particles is loading the actinide metal on a cation exchange resin. The AG-50W resin is made of sulfonic acid functional groups attached to a styrene divinylbenzene copolymer lattice (long chained hydrocarbon). The metal cation binds to the sulfur group, then during thermal decomposition in air the hydrocarbons will form gaseous species leaving behind a spherical metal-oxide particle. Process development for resin applications with radioactive materials is typically performed using surrogates. For americium and curium, a trivalent metal like neodymium can be used. Thermal decomposition of Nd-loaded resin in air has been studied by Hale. Process conditions were established for resin decomposition and the formation of Nd{sub 2}O{sub 3} particles. The intermediate product compounds were described using x-ray diffraction (XRD) and wet chemistry. Leskela and Niinisto studied the decomposition of rare earth (RE) elements and found results consistent with Hale. Picart et al. demonstrated the viability of using a resin loading process for the fabrication of uranium-actinide mixed oxide microspheres for transmutation of minor actinides in a fast reactor. For effective transmutation of actinides, it will be desirable to extend the in-reactor burnup and minimize the number of recycles of used actinide materials. Longer burn times increases the chance of Fuel Clad Chemical or Mechanical Interaction (FCCI, FCMI). Sulfur is suspected of contributing to Irradiation Assisted Stress Corrosion Cracking (IASCC) thus it is necessary to maximize the removal of sulfur during decomposition of the resin. The present effort extends the previous work by quantifying the removal of sulfur during the decomposition process. Neodymium was selected as a surrogate for trivalent actinide metal cations. As described above Nd was dissolved in nitric acid solution then contacted with the AG-50W resin column. After washing the column, the Nd-resin particles are removed and dried. The Nd-resin, seen in Figure 1 prior to decomposition, is ready to be converted to Nd oxide microspheres

Crystallography of Functional Materials

The goal of this special issue is to obtain new insights into the roles of crystallography in functional materials. This special issue consists of eight papers illustrating the structure and property relationships, as well as applications of selected classes of materials that deal with various aspects of functional materials, ranging from battery, magnetic, photocatalysis, and waveguide materials, to luminescent metal-organic frameworks and borates, semiconductors, and inorganic electrides. This issue provides further evidence of the importance of crystallography in understanding and improving various properties of functional materials, whether they are single crystals, bulk polycrystalline materials, or thin films

Insights into the structure of mixed CO2/CH4 in gas hydrates

The exchange of carbon dioxide for methane in natural gas hydrates is an attractive approach to harvesting CH4 for energy production while simultaneously sequestering CO2. In addition to the energy and environmental implications, the solid solution of clathrate hydrate (CH4)1–x(CO2)x·5.75H2O provides a model system to study how the distinct bonding and shapes of CH4 and CO2 influence the structure and properties of the compound. High-resolution neutron diffraction was used to examine mixed CO2/CH4 gas hydrates. CO2-rich hydrates had smaller lattice parameters, which were attributed to the higher affinity of the CO2 molecule interacting with H2O molecules that form the surrounding cages, and resulted in a reduction in the unit-cell volume. Experimental nuclear scattering densities illustrate how the cage occupants and energy landscape change with composition. These results provide important insights on the impact and mechanisms for the structure of mixed CH4/CO2 gas hydrate

Nanoporous Metal Porphyrin Frameworks (MPFs)

The investigation of nanoporous Metal Porphyrin Frameworks (MPFs) for on-board vehicular hydrogen storage is a research project spanning two colleges and four departments at the University of Tennessee. In the Chemistry Department, Dr. Peter Zhang and a post-doctoral researcher, Dr. Ying Chen, are synthesizing MPFs. In the Chemical Engineering Department, Dr. David Keffer, Dr. Brian Edwards, and Ruichang Xiong, a Ph.D. student, are modeling the hydrogen adsorptive capacity of MPFs using molecular simulation. In the Materials Science and Engineering Department, Dr. Claudia Rawn, who holds a joint appointment at ORNL, is using state-of-the-art diffraction facilities at ORNL to characterize the MPF\u27s created by Drs. Zhang and Chen. In the Civil and Environmental Engineering Department, Dr. Sandeep Agnihotri, plans to measure the hydrogen adsorptive capacity of the synthesized MPFs