One-electron redox kinetics of aqueous transition metal couples Zn2+/+, Co2+/+, and Ni2+/+ using pulse radiolysis

Lisovskaya, Alexandra; Kanjana, Kotchaphan; Bartels, David M.

doi:10.1039/d0cp03214j

Title: One-electron redox kinetics of aqueous transition metal couples Zn^2+/+, Co^2+/+, and Ni^2+/+ using pulse radiolysis

Journal Article · Mon Jul 27 00:00:00 EDT 2020 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d0cp03214j· OSTI ID:1799642

^[1]; Kanjana, Kotchaphan ^[1];

^[1]

Univ. of Notre Dame, IN (United States)

The one-electron redox potentials for aqueous metal couples Co^2+/+ and Ni^2+/+ have been investigated by using pulse radiolysis using their reactions with a series of reference compounds to establish the most positive upper limits of E⁰. Experiments with Zn⁺ were also carried out to confirm the characteristic shape of the expected reduction kinetics. Both formate ions and t-BuOH were employed to scavenge ˙OH radicals and ˙H atoms. Kinetics and fitted first and second order reaction rates have been reported for reactions with methyl viologen, fluorescein, Ru(NH₃)₆³⁺, Co(en)₃²⁺, Co(sepulcrate)³⁺, Ru(bpy)₃²⁺, Cr(bpy)33+, and Ni(Me₆[14]4,11-dieneN4)²⁺. Previous work demonstrated that both Co²⁺ and Ni²⁺ can be reduced by CO₂^˙- radicals, giving a negative E⁰ limit of -1.9 V vs. SHE. A definite reaction of Ni⁺ with fluorescein di-anions provides a new upper limit of the Ni^2+/+ couple as -0.906 V vs. SHE. The reaction of Co⁺ with Ru(bpy)₃²⁺ has been confirmed, giving E⁰ = -1.3 V vs. SHE as a rigorous upper limit of the Co^2+/+ couple. In the case of Co^2+/+, kinetics were complicated by a self-catalyzed metal clustering phenomenon. Initiation rate constants of this process have also been reported.

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Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FC02-04ER15533

OSTI ID:: 1799642

Alternate ID(s):: OSTI ID: 1648166

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 22, Issue 34; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Title: One-electron redox kinetics of aqueous transition metal couples Zn2+/+, Co2+/+, and Ni2+/+ using pulse radiolysis

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References (49)

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Title: One-electron redox kinetics of aqueous transition metal couples Zn^2+/+, Co^2+/+, and Ni^2+/+ using pulse radiolysis