NDLI: Structural bases of oxygen-sensitivity in Fe(II) complexes with tripodal ligands . Steric effects, Lewis acidity and the role of ancillary ligands

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Structural bases of oxygen-sensitivity in Fe(II) complexes with tripodal ligands . Steric effects, Lewis acidity and the role of ancillary ligands

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Benhamou, Laila Thibon, Aurore Brelot, Lydia Mandon, Dominique Lachkar, Mohammed
Description	Author Affiliation: Benhamou L ( Laboratoire de Chimie Biomimétique des Métaux de Transition, UMR CNRS n° 7177, Institut de Chimie de Strasbourg et Université de Strasbourg, Bâtiment Le Bel, 4 rue Blaise Pascal, CS 90032, F-67081 Strasbourg cedex, France.)
Abstract	The complexation of $Fe(SO_{3}CF_{3})_{2}$ to the series of fluoro α-substituted tris-(2-aminomethylpyridyl)amine tripods $F_{1–3}TPA$ yields the triflato $F_{1–3}TPAFe(SO_{3}CF_{3})_{2}$ complexes which have firstly been characterized in solution. As expected, bis-acetonitrile charged species are present in $CH_{3}CN,$ and neutral bis-triflato complexes in $CH_{2}Cl_{2}.$ The X-ray diffraction analyses of $F_{1}TPAFe(SO_{3}CF_{3})_{2}$ and $F_{2}TPAFe(SO_{3}CF_{3})_{2}$ crystallized from $CH_{2}Cl_{2}$ solutions show that their structure in solution is retained in the solid state, with coordination of both triflate ions and the $κ^{4}$ coordination mode of the tripod in each complex. The solid state structure of the $[F_{2}TPAFe(NCMe)(SO_{3}CF_{3})](SO_{3}CF_{3})$ complex obtained from crystallization in acetonitrile of the bis-triflato precursor is also reported. The presence of a bound triflate in the solid state is unexpected and interpreted as the result of solid-state stabilization by a metal center which displays some Lewis acidity character because of its coordination to an electron-deficient tripod. The fourth compound whose solid state structure is reported is $[F_{2}TPAFe(H_{2}O)_{2}](SO_{3}CF_{3})_{2},$ fortuitously obtained after the bis-triflato precursor was handled under aerobic conditions. In $CH_{3}CN,$ all complexes are oxygen stable. The gain in stability of the bis-acetonitrile adducts is certainly responsible for the lack of reactivity of all complexes in this solvent . In $CH_{2}Cl_{2},$ the parent $TPAFe(SO_{3}CF_{3})_{2}$ complex reacts with $O_{2}$ to yield a compound belonging to the well-known class of μ-oxo diferric compounds. Whereas $F_{1}TPAFe(SO_{3}CF_{3})_{2}$ is poorly reactive, $F_{2}TPAFe(SO_{3}CF_{3})_{2}$ and $F_{3}TPAFe(SO_{3}CF_{3})_{2}$ turn out to be completely inert. This strongly contrasts with the behavior of the known $F_{1–3}TPAFeCl_{2}$ complexes for which an increased reactivity is observed upon ligand substitution. In $CH_{2}Cl_{2},$ conductimetry measurements indicate extremely weak (if any!) dissociation of the ancillary ligands in all complexes. Comparative analysis of the structures reveals relatively invariant structural parameters within the series of $Fe(SO_{3}CF_{3})_{2}$ complexes, whereas $FeCl_{2}$ complexes display important metal to ligand elongations upon tripod substitution. The reactivity increase upon fluorination of the ligand in the $FeCl_{2}$ complexes is interpreted as resulting from sterically-induced pyridine flexibility. The opposite situation with $Fe(SO_{3}CF_{3})_{2}$ complexes is due to the lock of the coordination polyhedron in the absence of important steric stress, especially when the metal center becomes electron-deficient.
ISSN	14779226
Issue Number	47
Volume Number	41
e-ISSN	13645447
Journal	Dalton Trans.
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2012-12-21
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Ferrous Compounds Chemistry Lewis Acids Oxygen Crystallization Ligands Models, Molecular Stereoisomerism Journal Article Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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