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Kinetics of the oxidation of selenium(IV) by neptunium(VII) in aqueous acidic perchlorate media

Journal Article · · Inorg. Chem.; (United States)
DOI:https://doi.org/10.1021/ic50165a061· OSTI ID:7230599

The Np(VII) oxidation of Se(IV) proceeds with two-to-one stoichiometry to yield Np(VI) and Se(VI) according to the empirical rate law -d(ln(Np(VII)))/dt = k/sub 1/(Se(IV)) + k/sub 2/(Se(IV))/sup 2/ with no detectable acid dependence. The apparent activation parameters are ..delta..H/sub 1/* = 7.43 +- 0.14 and ..delta..H/sub 2/* = 3.70 +- 0.65 kcal/mol and ..delta..S/sub 1/* = 19.7 +- 0.5 and ..delta..S/sub 2/* = -28.9 +- 2.2 eu. This rate law is accounted for by a mechanism involving the known dimerization of Se(IV) in acidic media and parallel paths for the oxidation of both monomeric and dimeric forms. At 25/sup 0/ and ..mu.. = 1.00 M, the specific rate constants for oxidation of the monomer (k/sub M/) and dimer (k/sub D/) are (1.07 +- 0.02) x 10/sup 3/ and (4.37 +- 0.17) x 10/sup 3/ M/sup -1/s/sup -1/, respectvely. The observed rate law and rate parameters are discussed in terms of, and are found to be consistent with, the established reactivity pattern exhibited by Np(VII) when oxidizing aquometal ions.

OSTI ID:
7230599
Journal Information:
Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 15:11; ISSN INOCA
Country of Publication:
United States
Language:
English