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Kinetic study of the reduction of neptunium (VII) and americium (VI) by bromide ion in aqueous perchlorate media

Journal Article · · Inorg. Chem.; (United States)
DOI:https://doi.org/10.1021/ic50175a023· OSTI ID:7210488

The oxidation of Br- to bromine by the actinides, Am(VI) and Np(VII), has been found to proceed by the rate laws -/sup 1///sub 2/(d ln (Am(VI))/dt) = k/sub 1/(Br/sup -/) + k/sub 2/(Br/sup -/)/sup 2/ and -d ln (Np(VII))/dt = (Br/sup -/)(k/sub 1/(H/sup +/) + k/sub 2/(H/sup +/)/sup 2/). The apparent activation parameters are ..delta..H/sub 1//sup + +/ = 15.7 +- 0.1 kcal/mol, ..delta..H/sub 2//sup + +/ = 12.5 +- 0.1 kcal/mol, ..delta..S/sub 1//sup + +/ = 2.5 +- 2.7 eu, and ..delta..S/sub 2//sup + +/ = -1.5 +- 1.6 eu for Am(VI) and ..delta..H/sub 1//sup + +/ = 9.4 +- 0.3 kcal/mol, ..delta..H/sub 2//sup + +/ = 3.9 +- 0.5 kcal/mol, ..delta..S/sub 1//sup + +/ = -8.8 +- 1.1 eu, and ..delta..S/sub 2//sup + +/ = -26.3 +- 1.8 eu for Np(VII). The rate laws are accounted for by mechanisms consistent with other oxidations of Br/sup -/ and are compared with similar rate laws observed for the dioxo cation, VO/sub 2//sup +/.

Research Organization:
Argonne National Lab., IL
OSTI ID:
7210488
Journal Information:
Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 16:9; ISSN INOCA
Country of Publication:
United States
Language:
English