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Multielectron redox chemistry of lanthanide Schiff-base complexes

Content Provider	Royal Society of Chemistry (RSC)
Author	Camp, Clément Biswas, Biplab Dubois, Lionel Mazzanti, Marinella Guidal, Valentin Pécaut, Jacques
Copyright Year	2012
Abstract	Multielectron redox chemistry, which is essential in metal catalysed chemical transformations, is not easily accessible in lanthanide complexes. Here we explored the reductive chemistry of lanthanide complexes with tetradentate Schiff bases acting as redox-active ligands with the objective of identifying new pathways to lanthanide multielectron redox transfer. The chemical reduction with alkali metals of heteroleptic [Nd(salophen)X] (salophen = N,N′-bis(salicylidene)phenylenediamine, X = I, OTf) and of a series of homoleptic K[Ln(Rsalophen)2] complexes of trivalent lanthanides has resulted respectively in the synthesis of the new dinuclear Nd(III) complex K2[Nd2(cyclo-salophen)(THF)2] and in the synthesis of a series of mononuclear lanthanide(III) complexes of general formula K3[Ln(bis-Rsalophen)] (R = H, Me, tBu). Ligand reduction and C–C bond formation are supported by X-ray crystal structures. Proton NMR studies demonstrate that the K2[Nd2(cyclo-salophen)(py)2] complex can transfer four electrons in the reaction with oxidizing agents such as AgOTf through the breaking of the two C–C bonds. Moreover the electrochemistry and reactivity of the mononuclear complexes K3[Ln(bis-Rsalophen)] show that they can act as formal two electron reductants and that their oxidation potential can be tuned by changing the substituents on the ligand. These results illustrate that Schiff bases provide a new way to introduce multielectron redox events at lanthanide centers and a new route to highly reactive mono- and polynuclear complexes of lanthanides.
Starting Page	2433
Ending Page	2448
Page Count	16
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	3
Issue Number	8
Journal	Chemical Science
DOI	10.1039/c2sc20476b
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Lanthanide Ligand Chemical bond Redox Proton nuclear magnetic resonance Alkali metal Rsalophen Proton NMR X-ray crystallography Organic chemistry Phenylenediamine Schiff Homoleptic Electrochemistry Potassium
Content Type	Text
Resource Type	Article
Subject	Chemistry

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