Characterization of a paramagnetic mononuclear nonheme iron-superoxo complex

Chien Wei Chiang; Scott T. Kleespies; Heather D. Stout; Katlyn K. Meier; Po Yi Li; Emile L. Bominaar; Lawrence Que; Eckard Münck; Way Zen Lee

doi:10.1021/ja504410s

Characterization of a paramagnetic mononuclear nonheme iron-superoxo complex

Chien Wei Chiang, Scott T. Kleespies, Heather D. Stout, Katlyn K. Meier, Po Yi Li, Emile L. Bominaar, Lawrence Que, Eckard Münck, Way Zen Lee

Chemistry (Twin Cities)

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

64 Scopus citations

Abstract

O₂ bubbling into a THF solution of Fe^II(BDPP) (1) at -80 °C generates a reversible bright yellow adduct 2. Characterization by resonance Raman and Mössbauer spectroscopy provides complementary insights into the nature of 2. The former shows a resonance-enhanced vibration at 1125 cm^-1, which can be assigned to the ν(O-O) of a bound superoxide, while the latter reveals the presence of a high-spin iron(III) center that is exchange-coupled to the superoxo ligand, like the Fe^III-O ₂^- pair found for the O₂ adduct of 4-nitrocatechol-bound homoprotocatechuate 2,3-dioxygenase. Lastly, 2 oxidizes dihydroanthracene to anthracene, supporting the notion that Fe ^III-O₂^- species can carry out H atom abstraction from a C-H bond to initiate the 4-electron oxidation of substrates proposed for some nonheme iron enzymes.

Original language	English (US)
Pages (from-to)	10846-10849
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	136
Issue number	31
DOIs	https://doi.org/10.1021/ja504410s
State	Published - Aug 6 2014

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Characterization of a paramagnetic mononuclear nonheme iron-superoxo complex. / Chiang, Chien Wei; Kleespies, Scott T.; Stout, Heather D.; Meier, Katlyn K.; Li, Po Yi; Bominaar, Emile L.; Que, Lawrence; Münck, Eckard; Lee, Way Zen.

In: Journal of the American Chemical Society, Vol. 136, No. 31, 06.08.2014, p. 10846-10849.

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

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title = "Characterization of a paramagnetic mononuclear nonheme iron-superoxo complex",

abstract = "O2 bubbling into a THF solution of FeII(BDPP) (1) at -80 °C generates a reversible bright yellow adduct 2. Characterization by resonance Raman and M{\"o}ssbauer spectroscopy provides complementary insights into the nature of 2. The former shows a resonance-enhanced vibration at 1125 cm-1, which can be assigned to the ν(O-O) of a bound superoxide, while the latter reveals the presence of a high-spin iron(III) center that is exchange-coupled to the superoxo ligand, like the FeIII-O 2- pair found for the O2 adduct of 4-nitrocatechol-bound homoprotocatechuate 2,3-dioxygenase. Lastly, 2 oxidizes dihydroanthracene to anthracene, supporting the notion that Fe III-O2- species can carry out H atom abstraction from a C-H bond to initiate the 4-electron oxidation of substrates proposed for some nonheme iron enzymes.",

author = "Chiang, {Chien Wei} and Kleespies, {Scott T.} and Stout, {Heather D.} and Meier, {Katlyn K.} and Li, {Po Yi} and Bominaar, {Emile L.} and Lawrence Que and Eckard M{\"u}nck and Lee, {Way Zen}",

year = "2014",

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language = "English (US)",

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T1 - Characterization of a paramagnetic mononuclear nonheme iron-superoxo complex

AU - Chiang, Chien Wei

AU - Kleespies, Scott T.

AU - Stout, Heather D.

AU - Meier, Katlyn K.

AU - Li, Po Yi

AU - Bominaar, Emile L.

AU - Que, Lawrence

AU - Münck, Eckard

AU - Lee, Way Zen

PY - 2014/8/6

Y1 - 2014/8/6

N2 - O2 bubbling into a THF solution of FeII(BDPP) (1) at -80 °C generates a reversible bright yellow adduct 2. Characterization by resonance Raman and Mössbauer spectroscopy provides complementary insights into the nature of 2. The former shows a resonance-enhanced vibration at 1125 cm-1, which can be assigned to the ν(O-O) of a bound superoxide, while the latter reveals the presence of a high-spin iron(III) center that is exchange-coupled to the superoxo ligand, like the FeIII-O 2- pair found for the O2 adduct of 4-nitrocatechol-bound homoprotocatechuate 2,3-dioxygenase. Lastly, 2 oxidizes dihydroanthracene to anthracene, supporting the notion that Fe III-O2- species can carry out H atom abstraction from a C-H bond to initiate the 4-electron oxidation of substrates proposed for some nonheme iron enzymes.

AB - O2 bubbling into a THF solution of FeII(BDPP) (1) at -80 °C generates a reversible bright yellow adduct 2. Characterization by resonance Raman and Mössbauer spectroscopy provides complementary insights into the nature of 2. The former shows a resonance-enhanced vibration at 1125 cm-1, which can be assigned to the ν(O-O) of a bound superoxide, while the latter reveals the presence of a high-spin iron(III) center that is exchange-coupled to the superoxo ligand, like the FeIII-O 2- pair found for the O2 adduct of 4-nitrocatechol-bound homoprotocatechuate 2,3-dioxygenase. Lastly, 2 oxidizes dihydroanthracene to anthracene, supporting the notion that Fe III-O2- species can carry out H atom abstraction from a C-H bond to initiate the 4-electron oxidation of substrates proposed for some nonheme iron enzymes.

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