A kinetic study of plutonium dioxide dissolution in hydrochloric acid using iron (II) as an electron transfer catalyst

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Effective dissolution of plutonium dioxide has traditionally been accomplished by contact with strong nitric acid containing a small amount of fluoride at temperatures of {approximately} 100 C. In spite of these aggressive conditions, PuO{sub 2} dissolution is sometimes incomplete requiring additional contact with the solvent. This work focused on an alternative to conventional dissolution in nitric acid where an electron transfer catalyst, Fe(II), was used in hydrochloric acid. Cyclic voltammetry was employed as an in-situ analytical technique for monitoring the dissolution reaction rate. The plutonium oxide selected for this study was decomposed plutonium oxalate with > 95% of the material ... continued below

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222 p.

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Fife, K.W. September 1, 1996.

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Description

Effective dissolution of plutonium dioxide has traditionally been accomplished by contact with strong nitric acid containing a small amount of fluoride at temperatures of {approximately} 100 C. In spite of these aggressive conditions, PuO{sub 2} dissolution is sometimes incomplete requiring additional contact with the solvent. This work focused on an alternative to conventional dissolution in nitric acid where an electron transfer catalyst, Fe(II), was used in hydrochloric acid. Cyclic voltammetry was employed as an in-situ analytical technique for monitoring the dissolution reaction rate. The plutonium oxide selected for this study was decomposed plutonium oxalate with > 95% of the material having a particle diameter (< 70 {micro}m) as determined by a scanning laser microscopy technique. Attempts to dry sieve the oxide into narrow size fractions prior to dissolution in the HCl-Fe(II) solvent system failed, apparently due to significant interparticle attractive forces. Although sieve splits were obtained, subsequent scanning laser microscopy analysis of the sieve fractions indicated that particle segregation was not accomplished and the individual sieve fractions retained a particle size distribution very similar to the original powder assemblage. This phenomena was confirmed through subsequent dissolution experiments on the various screen fractions which illustrated no difference in kinetic behavior between the original oxide assemblage and the sieve fractions.

Physical Description

222 p.

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INIS; OSTI as DE96013484

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  • Other Information: DN: Thesis submitted to New Mexico State Univ., Las Cruces, NM (US); TH: Thesis (Ph.D.)

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  • Other: DE96013484
  • Report No.: LA--13188-T
  • Grant Number: W-7405-ENG-36
  • DOI: 10.2172/378830 | External Link
  • Office of Scientific & Technical Information Report Number: 378830
  • Archival Resource Key: ark:/67531/metadc679199

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Office of Scientific & Technical Information Technical Reports

Reports, articles and other documents harvested from the Office of Scientific and Technical Information.

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  • September 1, 1996

Added to The UNT Digital Library

  • July 25, 2015, 2:20 a.m.

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  • Feb. 29, 2016, 9:30 p.m.

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Fife, K.W. A kinetic study of plutonium dioxide dissolution in hydrochloric acid using iron (II) as an electron transfer catalyst, report, September 1, 1996; New Mexico. (digital.library.unt.edu/ark:/67531/metadc679199/: accessed November 22, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.