Chemistry, radiation, and interfaces in suspensions of nuclear waste simulants

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We focus in this report on three issues that are of central importance in the management of radioactive high-level liquid waste (HLLW). We show that the only reducing radical that lasts longer than a few ps in typical HLLW, and is capable of generating hydrogen, is NO{sub 3}{sup 2-}. We measured the lifetime of this species across the whole pH range (3 {le} pH {le} 14) and found it to be shorter than {approx}15 {mu}s, before is dissociates to give strongly oxidizing NO{sub 2} radicals. We found that it reacts with many proton donors (H{sup +} phosphate, borate, NH{sub 4}{sup ... continued below

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10 p.

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Meisel, D.; Cook, A.; Camaioni, D. & Orlando, T. August 1997.

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Description

We focus in this report on three issues that are of central importance in the management of radioactive high-level liquid waste (HLLW). We show that the only reducing radical that lasts longer than a few ps in typical HLLW, and is capable of generating hydrogen, is NO{sub 3}{sup 2-}. We measured the lifetime of this species across the whole pH range (3 {le} pH {le} 14) and found it to be shorter than {approx}15 {mu}s, before is dissociates to give strongly oxidizing NO{sub 2} radicals. We found that it reacts with many proton donors (H{sup +} phosphate, borate, NH{sub 4}{sup +}, amines) in a reaction that is not merely an acid-base equilibrium reaction. Using high-level ab initio calculations we estimate its redox potential and pK{sub a}. We have developed methodologies to study the degradation of organic additives to the HLLW (to CO{sub 2} or carbonate) by NO{sub 2}. Relative rates of degradation of several complexants were determined using competition kinetics and {sup 13}C NMR and proton NMR detection techniques. Direct absorption of the radiation (low-energy electrons as well as photons above the ionization threshold) in NaNO{sub 3} single crystal at the solid/vacuum interface led to production of NO, O, and O- as the major products.

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10 p.

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INIS; OSTI as DE97053261

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  • 192. meeting of the Electrochemical Society and 48. annual meeting of the International Society of Electrochemistry, Paris (France), 31 Aug - 5 Sep 1997

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  • Other: DE97053261
  • Report No.: ANL/CHM/CP--92698
  • Report No.: CONF-970805--
  • Grant Number: W-31109-ENG-38;AC06-76RL01830
  • Office of Scientific & Technical Information Report Number: 542071
  • Archival Resource Key: ark:/67531/metadc697438

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  • August 1997

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  • Aug. 14, 2015, 8:43 a.m.

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  • Dec. 16, 2015, 12:12 p.m.

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Meisel, D.; Cook, A.; Camaioni, D. & Orlando, T. Chemistry, radiation, and interfaces in suspensions of nuclear waste simulants, article, August 1997; Illinois. (digital.library.unt.edu/ark:/67531/metadc697438/: accessed August 19, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.