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In situ FTIR and UV-visible spectroelectrochemical studies of iron nitrosyl porphyrins in nonaqueous media

Journal Article · · Inorganic Chemistry; (USA)
DOI:https://doi.org/10.1021/ic00299a009· OSTI ID:5439366

The techniques of in situ FTIR and UV-visible spectroelectrochemistry were combined with microvoltammetry in order to elucidate the prevailing mechanism for electrooxidation of (P)Fe(NO), where P is the dianion of tetraphenylporphyrin (TPP), meso-tetrakis(2,4,6-trimethylphenyl)porphyrin (TMP), or octaethylporphurin (OEP). Each metalloporphyrin undergoes three reversible oxidations at a Pt microelectrode of 25-{mu}m diameter. These oxidations were examined with respect to the site of electron transfer and to the fate of the NO group on the time scales of thin-layer cyclic voltammetry and bulk controlled-potential electrolysis. The NO group remains coordinated to the Fe(III) center after electrooxidation of (P)Fe(NO) and a 166-187-cm{sup {minus}1} shift in NO vibration is observed upon going from (P)Fe(NO) to ((P)Fe(NO)){sup +} in CH{sub 2}Cl{sub 2}, 0.1 M TMAP. However, the bound NO ligand dissociates from ((P)Fe(NO)){sup 2+}, which is electrogenerated at more positive potentials. The effects of bound halide ion or neutral ligand coordination on {gamma}{sub NO} of ((P)Fe(NO)){sup +} were also examined. {gamma}{sub NO} of (P)Fe(NO)X, where X = Cl{sup {minus}}, Br{sup {minus}}, or I{sup {minus}}, is linearly related to the ionization potential of HX while {gamma}{sub NO} of ((P)Fe(NO)(S)){sup +} (where S is a bound solvent molecule) is linearly correlated with the Gutmann solvent number (DN) of the trans-lighted solvent molecule in bulk CH{sub 2}Cl{sub 2}.

OSTI ID:
5439366
Journal Information:
Inorganic Chemistry; (USA), Journal Name: Inorganic Chemistry; (USA) Vol. 27:26; ISSN 0020-1669; ISSN INOCA
Country of Publication:
United States
Language:
English