"Redox Chemistry of Noninnocent Quinones Annulated To 2Fe2S Cores" by Gabriel B. Hall, Jinzhu Chen et al.
 

Redox Chemistry of Noninnocent Quinones Annulated To 2Fe2S Cores

Document Type

Article

Publication Date

11-11-2013

Department

Physical & Earth Sciences

Abstract

Noninnocent ligands that are electronically coupled to active catalytic sites can influence the redox behavior of the catalysts. A series of (μ-dithiolato)Fe2(CO)6 complexes, in which the sulfur atoms of the μ-dithiolato ligand are bridged by 5-substituted (Me, OMe, Cl, t-Bu)-1,4-benzoquinones, 1,4-naphthoquinone, or 1,4-anthraquinone, have been synthesized and characterized. In addition, the bis-phosphine complex derived from the 1,4-naphthoquinone-bridged complex has also been prepared and characterized. Cyclic voltammetry of these complexes shows two reversible one-electron reductions at potentials 0.2 to 0.5 V less negative than their corresponding parent quinones. In the presence of acetic acid two-electron reductions of the complexes result in conversion of the quinones to hydroquinone moieties. EPR spectroscopic and computational studies of the one-electron-reduced complexes show electron delocalization from the semiquinones to the 2Fe2S moieties, thereby revealing the \" noninnocent\" behavior of these ligands with these catalysts. © 2013 American Chemical Society.

DOI

10.1021/om400913p

First Page

6605

Last Page

6612

Volume

32

Issue

21

Publication Title

Organometallics

ISSN

0276-7333

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