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Kinetics of tetravalent plutonium oxidation by cerium (4)

Journal Article:

Abstract

Stoichiometry and kinetics of the Pu(4) + Ce(4) reaction is studied by spectrophotometric method at 5-30 deg C in nitric acid solutions (..mu..=(HNO/sub 3/)+(NaNO/sub 3/) = 1.0 - 5.7; (Ce(4)) = 5.10/sup -5/ - 1.2.10/sup -3/ g-ion/1, (Pu(4)) =1.10/sup -5/ - 8.5.10/sup -4/ g-ion/1. Oxidation of one Pu(4) ion to a hexavalent state requires two Ce(4) ions. The plutonium oxidation is not complicated by by-processes. Reverse Ce(3) + PuO/sub 2//sup +/ reaction does not contribute essentially to the process at (Ce(3)) 2.6.10/sup -2/ g-ion/1. The reaction rate obeys the kinetic equation - d(Pu(4))/dt = ksub(eff)(Pu(4))(Ce(4))/a sub(+-HNO/sub 3/). The thermodynamical activation parameters are found for solutions at the varied nitric acid concentrations:..delta..Gsup(not equal) = 17.0+-0.2 and ..delta..Hsup(not equal) = 21.8+-2 kcal/mole(..mu..=1.0); ..delta..Gsup(not equal) = 19.1+-0.1 and ..delta..Hsup(not equal) = 23.1+-1 kcal/mole(..mu..=4.9). The reaction mechanism is discussed in terms of the theory of absolute reaction rates and the model of long-range charge transfer.
Publication Date:
Jan 01, 1975
Product Type:
Journal Article
Reference Number:
AIX-10-425699; EDB-79-069667
Resource Relation:
Journal Name: Radiokhimiya; (USSR); Journal Volume: 17:4
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; PLUTONIUM; CHEMICAL REACTION KINETICS; OXIDATION; AQUEOUS SOLUTIONS; CERIUM COMPOUNDS; CHEMICAL COMPOSITION; EQUATIONS; NITRIC ACID; PLUTONIUM COMPOUNDS; QUANTITY RATIO; THERMODYNAMIC PROPERTIES; ACTINIDE COMPOUNDS; ACTINIDES; CHEMICAL REACTIONS; DISPERSIONS; ELEMENTS; HYDROGEN COMPOUNDS; INORGANIC ACIDS; KINETICS; METALS; MIXTURES; PHYSICAL PROPERTIES; RARE EARTH COMPOUNDS; REACTION KINETICS; SOLUTIONS; TRANSURANIUM COMPOUNDS; TRANSURANIUM ELEMENTS; 400702* - Radiochemistry & Nuclear Chemistry- Properties of Radioactive Materials
OSTI ID:
6141021
Country of Origin:
USSR
Language:
Russian
Other Identifying Numbers:
Journal ID: CODEN: RADKA
Submitting Site:
INIS
Size:
Pages: 573-580
Announcement Date:

Journal Article:

Citation Formats

Nikitina, G P, Shumakov, V G, and Egorova, V P. Kinetics of tetravalent plutonium oxidation by cerium (4). USSR: N. p., 1975. Web.
Nikitina, G P, Shumakov, V G, & Egorova, V P. Kinetics of tetravalent plutonium oxidation by cerium (4). USSR.
Nikitina, G P, Shumakov, V G, and Egorova, V P. 1975. "Kinetics of tetravalent plutonium oxidation by cerium (4)." USSR.
@misc{etde_6141021,
title = {Kinetics of tetravalent plutonium oxidation by cerium (4)}
author = {Nikitina, G P, Shumakov, V G, and Egorova, V P}
abstractNote = {Stoichiometry and kinetics of the Pu(4) + Ce(4) reaction is studied by spectrophotometric method at 5-30 deg C in nitric acid solutions (..mu..=(HNO/sub 3/)+(NaNO/sub 3/) = 1.0 - 5.7; (Ce(4)) = 5.10/sup -5/ - 1.2.10/sup -3/ g-ion/1, (Pu(4)) =1.10/sup -5/ - 8.5.10/sup -4/ g-ion/1. Oxidation of one Pu(4) ion to a hexavalent state requires two Ce(4) ions. The plutonium oxidation is not complicated by by-processes. Reverse Ce(3) + PuO/sub 2//sup +/ reaction does not contribute essentially to the process at (Ce(3)) 2.6.10/sup -2/ g-ion/1. The reaction rate obeys the kinetic equation - d(Pu(4))/dt = ksub(eff)(Pu(4))(Ce(4))/a sub(+-HNO/sub 3/). The thermodynamical activation parameters are found for solutions at the varied nitric acid concentrations:..delta..Gsup(not equal) = 17.0+-0.2 and ..delta..Hsup(not equal) = 21.8+-2 kcal/mole(..mu..=1.0); ..delta..Gsup(not equal) = 19.1+-0.1 and ..delta..Hsup(not equal) = 23.1+-1 kcal/mole(..mu..=4.9). The reaction mechanism is discussed in terms of the theory of absolute reaction rates and the model of long-range charge transfer.}
journal = {Radiokhimiya; (USSR)}
volume = {17:4}
journal type = {AC}
place = {USSR}
year = {1975}
month = {Jan}
}