A Nonheme, High-Spin {FeNO}(8) Complex that Spontaneously Generates N2O

One-electron reduction of [Fe(NO)(N3PyS)]BF4 (1) leads to the production of the metastable nonheme {FeNO}(8) complex, [Fe(NO)(N3PyS)] (3). Complex 3 is a rare example of a high-spin (S = 1) {FeNO}(8) and is the first example, to our knowledge, of a mononuclear nonheme {FeNO}(8) species that generate...

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Bibliographic Details
Published inJournal of the American Chemical Society Vol. 139; no. 31; pp. 10621 - 10624
Main Authors Confer, Alex M., McQuilken, Alison C., Matsumura, Hirotoshi, Moenne-Loccoz, Pierre, Goldberg, David P.
Format Journal Article
LanguageEnglish
Published WASHINGTON Amer Chemical Soc 09.08.2017
Subjects
Chemistry
Chemistry, Multidisciplinary
Physical Sciences
Science & Technology
HEME MODEL
DIOXYGEN
NITRIC-OXIDE REDUCTASE
MECHANISM
NITROXYL
REACTIVITY
CHEMISTRY
REDOX
PORPHYRIN
INSIGHTS
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Summary:One-electron reduction of [Fe(NO)(N3PyS)]BF4 (1) leads to the production of the metastable nonheme {FeNO}(8) complex, [Fe(NO)(N3PyS)] (3). Complex 3 is a rare example of a high-spin (S = 1) {FeNO}(8) and is the first example, to our knowledge, of a mononuclear nonheme {FeNO}(8) species that generates N2O. A second, novel route to 3 involves addition of Piloty's acid, an HNO donor, to an Fe-II precursor. This work provides possible new insights regarding the mechanism of nitric oxide reductases.
Bibliography:NIH RePORTER
National Science Foundation
ISSN:0002-7863
DOI:10.1021/jacs.7b05549