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Synthesis of Uranium Fluorides from Uranium Dioxide with Ammonium Bifluoride and Ammonolysis of Uranium Fluorides to Uranium Nitrides

Synthesis of Uranium Fluorides from Uranium Dioxide with Ammonium Bifluoride and Ammonolysis of Uranium Fluorides to Uranium Nitrides


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About the Book

This work presents the chemical conversion of uranium oxides to uranium fluorides, and their subsequent conversion to uranium nitrides. Uranium dioxide reacts with ammonium bifluoride at 20C to form compound in the ammonium-uranium fluoride chemical system. This reaction occurs between solid uranium dioxide at the surface of the particles and ammonium fluoride vapor. A shrinking-sphere model demonstrated surface reaction kinetics, not mass transport by diffusion through the product layer, limit the reaction rate when the starting material consists of 100 mum uranium dioxide particles. Powder x-ray diffraction showed the reaction to be complete within 8 hours, with (NH4) 4UF8 the reaction product. High-resolution electron microcopy revealed the product is largely amorphous on a micrometer-scale, but contains well-formed crystal domains on the order of 10x10 nm. X-ray diffraction showed the reaction progresses though beta-NH4UF5, delta-(NH 4)2UF6, and gamma-(NH4)2UF6 intermediate phases before finally forming (NH4)4UF 8. Modeling the system as a series of first-order reaction suggested a fourth intermediate, possibly UF4, is likely to occur. The reaction of (NH4)4UF8 with ammonia gas at 800C forms alpha-U2N3/UN2 solid solution products with a composition of UN1.83. The x-ray powder diffraction pattern of this product is the fcc pattern commonly referenced as that of UN2 and the lattice parameter was 0.53050 nm. Surface area increased by a factor of ten during ammonolysis, consistent with the action of a hydriding agent. The alpha-U2N 3/UN2 solid solution system formed contained 1 wt% UO 2 as an impurity. Upon subsequent heating to 1150C for 4.5 hours under argon, the nitride sample formed UN with a UO2 impurity of 9 wt%. Based on the HRTEM images, oxidation in the UN product appears to be limited to within 20 nm of particle surfaces and grain boundaries.


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Product Details
  • ISBN-13: 9781243996411
  • Publisher: Proquest, Umi Dissertation Publishing
  • Publisher Imprint: Proquest, Umi Dissertation Publishing
  • Height: 246 mm
  • Weight: 249 gr
  • ISBN-10: 1243996412
  • Publisher Date: 01 Sep 2011
  • Binding: Paperback
  • Spine Width: 7 mm
  • Width: 189 mm


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Synthesis of Uranium Fluorides from Uranium Dioxide with Ammonium Bifluoride and Ammonolysis of Uranium Fluorides to Uranium Nitrides
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Synthesis of Uranium Fluorides from Uranium Dioxide with Ammonium Bifluoride and Ammonolysis of Uranium Fluorides to Uranium Nitrides
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