Conflicting Role of Water in the Activation of H2O2 and the Formation and Reactivity of Non-Heme FeIII-OOH and FeIII-O-FeIII Complexes at Room Temperature

Sandeep K. Padamati; Apparao Draksharapu; Duenpen Unjaroen; Wesley R. Browne

doi:10.1021/acs.inorgchem.5b02976

Conflicting Role of Water in the Activation of H₂O₂ and the Formation and Reactivity of Non-Heme Fe^III-OOH and Fe^III-O-Fe^III Complexes at Room Temperature

Sandeep K. Padamati
, Apparao Draksharapu
, Duenpen Unjaroen
, Wesley R. Browne

Chemistry (Twin Cities)

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

22 Scopus citations

Abstract

The formation of an Fe^III-OOH species by reaction of complex 1 ([(MeN3Py)Fe^II(CH₃CN)₂]²⁺) with H₂O₂ at room temperature is reported and is studied by a combination of UV/vis absorption, EPR, and resonance Raman spectroscopies. The formation of the Fe^III-OOH species, and its subsequent conversion to relatively inert Fe^III-O-Fe^III species, is shown to be highly dependent on the concentration of water, with excess water favoring the formation of the latter species, which is studied by UV/vis absorption spectroelectrochemistry also. The presence of acetic acid increases the rate and extent of oxidation of 1 to its iron(III) state and inhibits the wasteful decomposition of H₂O₂ but does not affect significantly the spectroscopic properties of the Fe^III-OOH species formed.

Original language	English (US)
Pages (from-to)	4211-4222
Number of pages	12
Journal	Inorganic chemistry
Volume	55
Issue number	9
DOIs	https://doi.org/10.1021/acs.inorgchem.5b02976
State	Published - May 2 2016

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© 2016 American Chemical Society.

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10.1021/acs.inorgchem.5b02976

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title = "Conflicting Role of Water in the Activation of H2O2 and the Formation and Reactivity of Non-Heme FeIII-OOH and FeIII-O-FeIII Complexes at Room Temperature",

abstract = "The formation of an FeIII-OOH species by reaction of complex 1 ([(MeN3Py)FeII(CH3CN)2]2+) with H2O2 at room temperature is reported and is studied by a combination of UV/vis absorption, EPR, and resonance Raman spectroscopies. The formation of the FeIII-OOH species, and its subsequent conversion to relatively inert FeIII-O-FeIII species, is shown to be highly dependent on the concentration of water, with excess water favoring the formation of the latter species, which is studied by UV/vis absorption spectroelectrochemistry also. The presence of acetic acid increases the rate and extent of oxidation of 1 to its iron(III) state and inhibits the wasteful decomposition of H2O2 but does not affect significantly the spectroscopic properties of the FeIII-OOH species formed.",

author = "Padamati, \{Sandeep K.\} and Apparao Draksharapu and Duenpen Unjaroen and Browne, \{Wesley R.\}",

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T1 - Conflicting Role of Water in the Activation of H2O2 and the Formation and Reactivity of Non-Heme FeIII-OOH and FeIII-O-FeIII Complexes at Room Temperature

AU - Padamati, Sandeep K.

AU - Draksharapu, Apparao

AU - Unjaroen, Duenpen

AU - Browne, Wesley R.

PY - 2016/5/2

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N2 - The formation of an FeIII-OOH species by reaction of complex 1 ([(MeN3Py)FeII(CH3CN)2]2+) with H2O2 at room temperature is reported and is studied by a combination of UV/vis absorption, EPR, and resonance Raman spectroscopies. The formation of the FeIII-OOH species, and its subsequent conversion to relatively inert FeIII-O-FeIII species, is shown to be highly dependent on the concentration of water, with excess water favoring the formation of the latter species, which is studied by UV/vis absorption spectroelectrochemistry also. The presence of acetic acid increases the rate and extent of oxidation of 1 to its iron(III) state and inhibits the wasteful decomposition of H2O2 but does not affect significantly the spectroscopic properties of the FeIII-OOH species formed.

AB - The formation of an FeIII-OOH species by reaction of complex 1 ([(MeN3Py)FeII(CH3CN)2]2+) with H2O2 at room temperature is reported and is studied by a combination of UV/vis absorption, EPR, and resonance Raman spectroscopies. The formation of the FeIII-OOH species, and its subsequent conversion to relatively inert FeIII-O-FeIII species, is shown to be highly dependent on the concentration of water, with excess water favoring the formation of the latter species, which is studied by UV/vis absorption spectroelectrochemistry also. The presence of acetic acid increases the rate and extent of oxidation of 1 to its iron(III) state and inhibits the wasteful decomposition of H2O2 but does not affect significantly the spectroscopic properties of the FeIII-OOH species formed.

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