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  1. This report describes the Rare Earth Crisis and the effect of rare earth elements.
  2. Summary final report for research initiated but not finished.
  3. As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O 3PC 6H 4PO 3) 1-x/2(APO 4)x·nH 2O: where M=Zr 4+, Sn 4+, A=H, Na,more » or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.« less
  4. The dissolution of unirradiated used nuclear fuel (UNF) pellets pretreated for tritium removal was demonstrated using a tributly phosphate (TBP) solvent. Dissolution of pretreated fuel in TBP could potentially combine dissolution with two cycle of solvent extraction required for separating the actinides and lanthanides from other fission products. Dissolutions were performed using UNF surrogates prepared from both uranyl nitrate and uranium trioxide produced from the pretreatment process by adding selected actinide and stable fission product elements. In laboratory-scale experiments, the U dissolution efficiency ranged from 80-99+% for both the nitrate and oxide surrogate fuels. On average, 80% of the Pumore » and 50% of the Np and Am in the nitrate surrogate dissolved; however, little of the transuranic elements dissolved in the oxide form. The majority of the 3+ lanthanide elements dissolved. Only small amounts of Sr (0-1.6%) and Mo (0.1-1.7%) and essentially no Cs, Ru, Zr, or Pd dissolved.« less
  5. Rare earth metals are critical materials in a wide variety of applications in generating and storing renewable energy and in designing more energy efficient devices. Extracting rare earth metals from geothermal brines is a very challenging problem due to the low concentrations of these elements and engineering challenges with traditional chemical separations methods involving packed sorbent beds or membranes that would impede large volumetric flow rates of geothermal fluids transitioning through the plant. We are demonstrating a simple and highly cost-effective nanofluid-based method for extracting rare earth metals from geothermal brines. Core-shell composite nanoparticles are produced that contain a magneticmore » iron oxide core surrounded by a shell made of silica or metal-organic framework (MOF) sorbent functionalized with chelating ligands selective for the rare earth elements. By introducing the nanoparticles at low concentration (≈0.05 wt%) into the geothermal brine after it passes through the plant heat exchanger, the brine is exposed to a very high concentration of chelating sites on the nanoparticles without need to pass through a large and costly traditional packed bed or membrane system where pressure drop and parasitic pumping power losses are significant issues. Instead, after a short residence time flowing with the brine, the particles are effectively separated out with an electromagnet and standard extraction methods are then applied to strip the rare earth metals from the nanoparticles, which are then recycled back to the geothermal plant. Recovery efficiency for the rare earths at ppm level has now been measured for both silica and MOF sorbents functionalized with a variety of chelating ligands. A detailed preliminary techno-economic performance analysis of extraction systems using both sorbents showed potential to generate a promising internal rate of return (IRR) up to 20%.« less
  6. There are currently zero operating suppliers of critical rare earth elements La–Lu, Sc, Y (REs), in the western hemisphere. REs are critical materials due to their importance in clean energy and defense applications, including permanent magnets in wind turbines and phosphors in energy efficient lighting. It is not economically viable to produce pure REs in the U.S. given current separations technology. REs production is dominated by suppliers in the People’s Republic of China (PRC) because of their capacity in liquid­liquid solvent extraction (SX) used to purify mixtures. Weak environmental regulations in the PRC also contribute to a competitive advantage. SXmore » is a cost, time, solvent and waste intensive process but is highly optimized and scalable. The low efficiency of SX derives from the small thermodynamic differences in solvation enthalpy between the RE3+ cations. To foster stable domestic RE production there is a critical need for fundamentally new REs chemistry that contributes to disruptive technologies in RE separations. The overall goal of this project was to develop new thermodynamic bases, and apply them, for the solution separation of rare earth metals. We have developed the chemistry of rare earth metals: La–Lu, Sc and Y, with redox active ligands. Our hypothesis for the project was that electron­hole coupling in complexes of certain lanthanide metals with redox active ligands can be used to manifest chemical distinctiveness and affect separations. We also developed separations based on unique solution equilibria from tailored ligands.« less
  7. As electronic technology continues to evolve there is a growing need to develop processes which recover valuable material from antiquated technology. This need follows from the environmental challenges associated with the availability of raw materials and fast growing generation of electronic waste. Although just present in small quantities in electronic devices, the availability of raw materials, such as rare earths and precious metals, becomes critical for the production of high tech electronic devices and the development of green technologies (i.e. wind turbines, electric motors, and solar panels). Therefore, the proper recycling and processing of increasing volumes of electronic waste presentmore » an opportunity to stabilize the market of critical materials, reducing the demand of mined products, and providing a proper disposal and treatment of a hazardous waste stream. This paper will describe development and techno-economic assessment of a comprehensive process for the recovery of value and critical materials from electronic waste. This hydrometallurgical scheme aims to selectively recover different value segments in the materials streams (base metals, precious metals, and rare earths). The economic feasibility for the recovery of rare earths from electronic waste is mostly driven by the efficient recovery of precious metals, such as Au and Pd (ca. 80 % of the total recoverable value). Rare earth elements contained in magnets (speakers, vibrators and hard disk storage) can be recovered as a mixture of rare earths oxides which can later be reduced to the production of new magnets.« less
  8. Industrial rare earth separation processes utilize PC88A, a phosphonic acid ligand, for solvent extraction separations. The separation factors of the individual rare earths, the equipment requirements, and chemical usage for these flowsheets are well characterized. Alternative ligands such as Cyanex® 572 and the associated flowsheets are being investigated at the pilot scale level to determine if significant improvements to the current separation processes can be realized. These improvements are identified as higher separation factors, reduced stage requirements, or reduced chemical consumption. Any of these improvements can significantly affect the costs associated with these challenging separation proccesses. A mid/heavy rare earthmore » element (REE) separations flowsheet was developed and tested for each ligand in a 30 stage mixer-settler circuit to compare the separation performance of PC88A and Cyanex® 572. The ligand-metal complex strength of Cyanex® 572 provides efficient extraction of REE while significantly reducing the strip acid requirements. Reductions in chemical consumption have a significant impact on process economics for REE separations. Partitioning results summarized Table 1 indicate that Cyanex® 572 offers the same separation performance as PC88A while reducing acid consumption by 30% in the strip section for the mid/heavy REE separation. Flowsheet Effluent Compositions PC88A Cyanex® 572 Raffinate Mid REE Heavy REE 99.40% 0.60% 99.40% 0.60% Rich Mid REE Heavy REE 2.20% 97.80% 0.80% 99.20% Liquor Strip Acid Required 3.4 M 2.3 M Table 1 – Flowsheet results comparing separation performance of PC88A and Cyanex® 572 for a mid/heavy REE separation.« less
  9. Colloidal synthesis and assembly provide low cost, large area routes to mesoscale structures. In particular, shape-anisotropic particles may form crystalline, plastic crystalline, complex liquid crystalline and glassy phases. Arrangements in each order class have been used to generate photonic materials. For example, large photonic band gaps have been found for photonic crystals, hyperuniform photonic glasses, and also for plastic crystals at sufficient refractive index contrast. The latter structures support highly isotropic bandgaps that are desirable for free-form waveguides and LED out-coupling. Photonic glasses with optical gain lead to self-tuned lasing by the superposition of multiply scattered light. Typically, extrinsic mediamore » such as organic dyes, rare earths, lanthanides and quantum dots are used to impart optical gain in photonic solids. The present work advances fullerene microcrystals as a new materials platform for ‘active’ light emitting in colloid-based photonic crystals. Fullerenes support singlet excited states that recombine to produce a characteristic red photoluminescence. C 60 also has a high refractive index (n ~ 2.2) and transparency (> 560 nm) 9 so that inverse structures are not required.« less
  10. This document is the final report for the Nuclear Energy Universities Program (NEUP) grant 10-910 (DE-AC07-05ID14517) “Alpha Radiolysis of Nuclear Solvent Extraction Ligands used for An(III) and Ln(III) Separations”. The goal of this work was to obtain a quantitative understanding of the impacts of both low Linear Energy Transfer (LET, gamma-rays) and high LET (alpha particles) radiation chemistry occurring in future large-scale separations processes. This quantitative understanding of the major radiation effects on diluents and ligands is essential for optimal process implementation, and could result in significant cost savings in the future.

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