Decomposition of Rare Earth Loaded Resin Particles

Abstract

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) fuelsmore » 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.« less