Chemistry, radiation, and interfaces in suspensions of nuclear waste simulants
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.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States); Battelle Memorial Inst., Columbus, OH (United States)
- Sponsoring Organization:
- USDOE Office of Energy Research, Washington, DC (United States)
- DOE Contract Number:
- W-31109-ENG-38; AC06-76RL01830
- OSTI ID:
- 542071
- Report Number(s):
- ANL/CHM/CP-92698; CONF-970805-; ON: DE97053261; TRN: 98:008447
- Resource Relation:
- Conference: 192. meeting of the Electrochemical Society and 48. annual meeting of the International Society of Electrochemistry, Paris (France), 31 Aug - 5 Sep 1997; Other Information: PBD: 1997
- Country of Publication:
- United States
- Language:
- English
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