NDLI: Spectroelectrochemical Evidence for the Nitrosyl Redox Siblings $NO^{+},$ $NO^{.},$ and $NO^{−}$ Coordinated to a Strongly Electron-Accepting $Fe^{II}$ Porphyrin: DFT Calculations Suggest the Presence of High-Spin States after Reduction of the $Fe^{II}–NO^{−}$ Complex

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Spectroelectrochemical Evidence for the Nitrosyl Redox Siblings $NO^{+},$ $NO^{.},$ and $NO^{−}$ Coordinated to a Strongly Electron-Accepting $Fe^{II}$ Porphyrin: DFT Calculations Suggest the Presence of High-Spin States after Reduction of the $Fe^{II}–NO^{−}$ Complex

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Spectroelectrochemical Evidence for the Nitrosyl Redox Siblings $NO^{+},$ $NO^{.},$ and $NO^{−}$ Coordinated to a Strongly Electron-Accepting $Fe^{II}$ Porphyrin: DFT Calculations Suggest the Presence of High-Spin States after Reduction of the $Fe^{II}–NO^{−}$ Complex

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Hübner, Ralph Pellegrino, Juan Doctorovich, Fabio Kaim, Wolfgang
Description	Author Affiliation: Pellegrino J ( Departamento de Química Inorgánica, Analítica, y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, INQUIMAE-CONICET, Ciudad Universitaria, Pab. 2, C1428EHA Buenos Aires, Argentina.)
Abstract	En este trabajo se estudia el comportamiento redox del complejo $\{FeNO\}^{7}$ con sustituyentes atractores de electrones, $[Fe(NO)(TFPPBr_{8})]=1$ $(TFPPBr_{8}=2,3,7,8,12,13,17,18-octabromo-5,10,15,20-tetrakis(pentafluorofenil)porfirina)$ mediante experimentos de espectroelectroquímica y cálculos computacionales. El complejo 1 presenta tres procesos electroquímicos de un electrón: dos reducciones reversibles y una oxidación irreversible. El considerable cambio de $ν_{NO}$ de $1715 cm^{−1}$ a ≈ $1550 cm^{−1}$ indica que la primera reducción a $1^{−}$ involucra en gran medida al ligando NO. Para la segunda reducción a $1^{2−}$ se observa, sorprendentemente, un cambio de $ν_{NO}$ a ≈ $1590 cm^{−1}.$ Este pequeño corrimiento de $ν_{NO}$ y los cambios notables de las vibraciones asociadas a modos de la porfirina, así como los cambios significativos en la banda UV/Vis de Soret, indican un proceso centrado en la porfirina; los cálculos DFT predicen el corrimiento de $ν_{NO}$ a mayores frecuencias para los estados de spin intermedio y alto de $1^{2−}.$ En cuanto a la oxidación de 1, la onda irreversible en la voltametría cíclica sugiere que la forma catiónica $1^{+}$ se disocia dando la porfirina de hierro(III) y NO; sin embargo, en el experimento espectroelectroquímico el proceso resulta reversible, recuperándose la $ν_{NO}$ de 1 al reducir. Los cálculos DFT apoyan la interpretación de los resultados experimentales.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	28
Volume Number	17
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2011-07-04
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Electrochemistry Chemistry Nitric Oxide Porphyrins Models, Chemical Molecular Structure Oxidation-Reduction Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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