Radiolytic and Radiolytically Induced Generation of Gases from Synthetic Wastes : Final Report

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To better understand the processes leading to the generation and release of gases from waste tanks, the authors studied the radiolytic and thermal generation of H2, N2O, N2, O2, and NH3 in nonradioactive waste simulant solutions and slurries. The radiolytic sources for H2 are e(sub aq)⁻ and its predecessors and H atoms. Radiolysis of the water generates some H2 and an additional amount comes from the hydrogen abstraction reaction H + RH(yields) H2+R(center_dot). Nitrate scavenges e(sub aq)(sup (minus) and its predecessors whereas nitrite is the major H-atom scavenger. Computer modeling shows that if [NO3⁻] is above 0.5 M, and [NO2⁻] ... continued below

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x, 92 p. : charts, tables

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Meisel, Dan; Jonah, Charles D.; Kapoor, S.; Matheson, Max S. & Sauer, M. C. October 1993.

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  • Main Title: Radiolytic and Radiolytically Induced Generation of Gases from Synthetic Wastes : Final Report
  • Added Title: ANL (Series)
  • Added Title: Argonne National Laboratory Report ANL-93/43
  • Series Title: Argonne National Laboratory Reports

Description

To better understand the processes leading to the generation and release of gases from waste tanks, the authors studied the radiolytic and thermal generation of H2, N2O, N2, O2, and NH3 in nonradioactive waste simulant solutions and slurries. The radiolytic sources for H2 are e(sub aq)⁻ and its predecessors and H atoms. Radiolysis of the water generates some H2 and an additional amount comes from the hydrogen abstraction reaction H + RH(yields) H2+R(center_dot). Nitrate scavenges e(sub aq)(sup (minus) and its predecessors whereas nitrite is the major H-atom scavenger. Computer modeling shows that if [NO3⁻] is above 0.5 M, and [NO2⁻] is above 2M, the addition of other scavengers will have little effect on the yield of H2. In the presence of organic molecules O2 is efficiently destroyed. Small yields of ammonia were measured and the yields increase linearly with dose. The nitrogen in NH3 comes from organic chelators. The yields of gases in solution depend only weakly on temperature. The rate of thermal generation of gases increases upon preirradiation, reaches a maximum, and then declines. The known radiolytic degradation products of chelators, NTA, IDA, glycolate, glyoxylate, formaldehyde, formate, oxalate, and hydroxylainine were examined for their roles in the thermal generation of H2 and N2O at 60 C. In solution or slurry only radiolytically produced Pd intermediate strongly retains H2. Radiolytic yields of N2O are strongly reduced by Cr(III). In irradiated slurry, loose and tight gas were found. The loose gas could be removed by bubbling from the slurry, but the tight gas could be released only by dissolution of the slurry.

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x, 92 p. : charts, tables

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  • October 1993

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  • Aug. 4, 2015, 8:33 a.m.

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Meisel, Dan; Jonah, Charles D.; Kapoor, S.; Matheson, Max S. & Sauer, M. C. Radiolytic and Radiolytically Induced Generation of Gases from Synthetic Wastes : Final Report, report, October 1993; Argonne, Illinois. (https://digital.library.unt.edu/ark:/67531/metadc283156/: accessed July 18, 2019), University of North Texas Libraries, Digital Library, https://digital.library.unt.edu; crediting UNT Libraries Government Documents Department.