Oxidation reaction of [Ni(1,4,7-triazacyclononane)2] 2+ by [Fe(o-phenanthroline)3]3+ in aqueous acidic solution at elevated pressures: Determination of the activation and reaction volumes for the Ni(III)/(II) couple

Sumitaka Itoh; Nobuyoshi Koshino; Masumi Katsuki; Toshiaki Noda; Koji Ishihara; Masahiko Inamo; Hideo D. Takagi

doi:10.1039/b401969e

Oxidation reaction of [Ni(1,4,7-triazacyclononane)₂] ²⁺ by [Fe(o-phenanthroline)₃]³⁺ in aqueous acidic solution at elevated pressures: Determination of the activation and reaction volumes for the Ni(III)/(II) couple

Sumitaka Itoh, Nobuyoshi Koshino, Masumi Katsuki, Toshiaki Noda, Koji Ishihara, Masahiko Inamo, Hideo D. Takagi^*

^*Corresponding author for this work

School of Advanced Science and Engineering

Research output: Contribution to journal › Article › peer-review

2 Citations (Scopus)

Abstract

The reaction volume corresponding to the self-exchange process of the [Ni(tacn)₂]^3+/2+ couple was determined in aqueous acidic solution. Theoretical equations on the basis of the Mean Spherical Approximation were proposed for the estimation of reaction volumes for M ^{n+1(n - 1)+} couples in solution, and the calculated reaction volumes were compared with the experimentally estimated values. The activation volume for the [Ni(tacn)₂]^3+/2+ couple was determined in the acidic condition from the cross reaction of [Ni(tacn)₂]²⁺ and [Fe(o-phen)₃]³⁺ at elevated pressures. The agreement of the experimentally estimated activation volume for the [Ni(tacn) ₂]^3+/2+ couple, -8.2 ± 2.4 cm³ mol ^-1, with the theoretically calculated value, -7.5 cm³ mol^-1, within the allowed uncertainty (±1 cm³ mol^-1) indicates that the electron self-exchange reaction of this redox couple obeys the Marcusian behavior in aqueous acidic solution.

Original language	English
Pages (from-to)	1862-1866
Number of pages	5
Journal	Dalton Transactions
Issue number	12
DOIs	https://doi.org/10.1039/b401969e
Publication status	Published - 2004 Jun 21

ASJC Scopus subject areas

Inorganic Chemistry

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Itoh, S., Koshino, N., Katsuki, M., Noda, T., Ishihara, K., Inamo, M., & Takagi, H. D. (2004). Oxidation reaction of [Ni(1,4,7-triazacyclononane)₂] ²⁺ by [Fe(o-phenanthroline)₃]³⁺ in aqueous acidic solution at elevated pressures: Determination of the activation and reaction volumes for the Ni(III)/(II) couple. Dalton Transactions, (12), 1862-1866. https://doi.org/10.1039/b401969e

Oxidation reaction of [Ni(1,4,7-triazacyclononane)₂] ²⁺ by [Fe(o-phenanthroline)₃]³⁺ in aqueous acidic solution at elevated pressures : Determination of the activation and reaction volumes for the Ni(III)/(II) couple. / Itoh, Sumitaka; Koshino, Nobuyoshi; Katsuki, Masumi et al.

In: Dalton Transactions, No. 12, 21.06.2004, p. 1862-1866.

Research output: Contribution to journal › Article › peer-review

Itoh, S, Koshino, N, Katsuki, M, Noda, T, Ishihara, K, Inamo, M & Takagi, HD 2004, 'Oxidation reaction of [Ni(1,4,7-triazacyclononane)₂] ²⁺ by [Fe(o-phenanthroline)₃]³⁺ in aqueous acidic solution at elevated pressures: Determination of the activation and reaction volumes for the Ni(III)/(II) couple', Dalton Transactions, no. 12, pp. 1862-1866. https://doi.org/10.1039/b401969e

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title = "Oxidation reaction of [Ni(1,4,7-triazacyclononane)2] 2+ by [Fe(o-phenanthroline)3]3+ in aqueous acidic solution at elevated pressures: Determination of the activation and reaction volumes for the Ni(III)/(II) couple",

abstract = "The reaction volume corresponding to the self-exchange process of the [Ni(tacn)2]3+/2+ couple was determined in aqueous acidic solution. Theoretical equations on the basis of the Mean Spherical Approximation were proposed for the estimation of reaction volumes for M n+1(n - 1)+ couples in solution, and the calculated reaction volumes were compared with the experimentally estimated values. The activation volume for the [Ni(tacn)2]3+/2+ couple was determined in the acidic condition from the cross reaction of [Ni(tacn)2]2+ and [Fe(o-phen)3]3+ at elevated pressures. The agreement of the experimentally estimated activation volume for the [Ni(tacn) 2]3+/2+ couple, -8.2 ± 2.4 cm3 mol -1, with the theoretically calculated value, -7.5 cm3 mol-1, within the allowed uncertainty (±1 cm3 mol-1) indicates that the electron self-exchange reaction of this redox couple obeys the Marcusian behavior in aqueous acidic solution.",

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AB - The reaction volume corresponding to the self-exchange process of the [Ni(tacn)2]3+/2+ couple was determined in aqueous acidic solution. Theoretical equations on the basis of the Mean Spherical Approximation were proposed for the estimation of reaction volumes for M n+1(n - 1)+ couples in solution, and the calculated reaction volumes were compared with the experimentally estimated values. The activation volume for the [Ni(tacn)2]3+/2+ couple was determined in the acidic condition from the cross reaction of [Ni(tacn)2]2+ and [Fe(o-phen)3]3+ at elevated pressures. The agreement of the experimentally estimated activation volume for the [Ni(tacn) 2]3+/2+ couple, -8.2 ± 2.4 cm3 mol -1, with the theoretically calculated value, -7.5 cm3 mol-1, within the allowed uncertainty (±1 cm3 mol-1) indicates that the electron self-exchange reaction of this redox couple obeys the Marcusian behavior in aqueous acidic solution.

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