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Radiolytic oxidation

Abstract

Work under the Radiolytic Oxidation Contract from 1986 until April 1989 is reported. The effects of alpha- and gamma-irradiation on the chemistries of plutonium, neptunium and technetium, under conditions representative of the near fields of intermediate and high level waste repositories, were investigated. Gamma-radiolysis of Np (IV) results in oxidation in solutions below pH 12. Solutions of Tc (VII) are reduced to Tc (IV) by gamma-irradiation in contact with blast furnace slag/ordinary Portland cement under an inert atmosphere but not when in contact with pulverized fuel ash/ordinary Portland cement. Tc (IV) is shown to be susceptible to oxidation by the products of the alpha-radiolysis of water. The results of `overall effects` experiments, which combined representative components of typical ILW or HLW near fields, supported these observations and also showed enhanced plutonium concentrations in alpha-irradiated, HLW simulations. Mathematical models of the behaviour of plutonium and neptunium during gamma-radiolysis have been developed and indicate that oxidation to Pu (VI) is possible at dose rates typical of those expected for HLW. Simulations at ILW dose rates have indicated some effect upon the speciation of neptunium. Laboratory studies of the gamma-irradiation of Np (IV) in bentonite-equilibrated water have also been modelled. Computer code used:  More>>
Publication Date:
Dec 31, 1991
Product Type:
Technical Report
Report Number:
EUR-13670
Reference Number:
SCA: 052002; 400600; 400702; PA: FRD-92:000832; SN: 92000757136
Resource Relation:
Other Information: PBD: 1991
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; NEPTUNIUM; SOLUBILITY; GAMMA RADIATION; TECHNETIUM; ALPHA PARTICLES; PLUTONIUM; OXIDATION; WATER; RADIOLYSIS; RADIOACTIVE WASTE DISPOSAL; WASTE FORMS; BENCH-SCALE EXPERIMENTS; P CODES; COMPUTERIZED SIMULATION; 052002; 400600; 400702; WASTE DISPOSAL AND STORAGE; RADIATION CHEMISTRY; PROPERTIES OF RADIOACTIVE MATERIALS
OSTI ID:
10152467
Research Organizations:
Commission of the European Communities, Luxembourg (Luxembourg)
Country of Origin:
France
Language:
English
Other Identifying Numbers:
Other: ON: TI92526841; CNN: Contract Fl1W/0029-UK; TRN: FR9200832
Availability:
OSTI; NTIS (US Sales Only); INIS
Submitting Site:
FRN
Size:
110 p.
Announcement Date:
Jul 05, 2005

Citation Formats

Burns, W G, Ewart, F T, Hobley, J, Smith, A J, Walters, W S, and Williams, S J. Radiolytic oxidation. France: N. p., 1991. Web.
Burns, W G, Ewart, F T, Hobley, J, Smith, A J, Walters, W S, & Williams, S J. Radiolytic oxidation. France.
Burns, W G, Ewart, F T, Hobley, J, Smith, A J, Walters, W S, and Williams, S J. 1991. "Radiolytic oxidation." France.
@misc{etde_10152467,
title = {Radiolytic oxidation}
author = {Burns, W G, Ewart, F T, Hobley, J, Smith, A J, Walters, W S, and Williams, S J}
abstractNote = {Work under the Radiolytic Oxidation Contract from 1986 until April 1989 is reported. The effects of alpha- and gamma-irradiation on the chemistries of plutonium, neptunium and technetium, under conditions representative of the near fields of intermediate and high level waste repositories, were investigated. Gamma-radiolysis of Np (IV) results in oxidation in solutions below pH 12. Solutions of Tc (VII) are reduced to Tc (IV) by gamma-irradiation in contact with blast furnace slag/ordinary Portland cement under an inert atmosphere but not when in contact with pulverized fuel ash/ordinary Portland cement. Tc (IV) is shown to be susceptible to oxidation by the products of the alpha-radiolysis of water. The results of `overall effects` experiments, which combined representative components of typical ILW or HLW near fields, supported these observations and also showed enhanced plutonium concentrations in alpha-irradiated, HLW simulations. Mathematical models of the behaviour of plutonium and neptunium during gamma-radiolysis have been developed and indicate that oxidation to Pu (VI) is possible at dose rates typical of those expected for HLW. Simulations at ILW dose rates have indicated some effect upon the speciation of neptunium. Laboratory studies of the gamma-irradiation of Np (IV) in bentonite-equilibrated water have also been modelled. Computer code used: PHREEQE, 8 Figs.; 48 Tabs.; 38 refs.}
place = {France}
year = {1991}
month = {Dec}
}