0000000001299904
AUTHOR
Narcis Avarvari
Mononuclear and One-Dimensional Cobalt(II) Complexes with the 3,6-Bis(picolylamino)-1,2,4,5-tetrazine Ligand
International audience
Magnetic Molecular Conductors Based on Bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) and the Tris(chlorocyananilato)ferrate(III) Complex
Electrocrystallization of the bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) organic donor in the presence of the [Fe(ClCNAn)3]3– tris(chlorocyananilato)ferrate(III) paramagnetic anion in different stoichiometric ratios and solvent mixtures afforded two different hybrid systems formulated as [BEDT-TTF]4[Fe(ClCNAn)3]·3H2O (1) and [BEDT-TTF]5[Fe(ClCNAn)3]2·2CH3CN (2) (An = anilato). Compounds 1 and 2 present unusual structures without the typical segregated organic and inorganic layers, where layers of 1 are formed by Λ and Δ enantiomers of the anionic paramagnetic complex together with mixed-valence BEDT-TTF tetramers, while layers of 2 are formed by Λ and Δ enantiomers of the paramagnetic…
Tetramethyl-Bis(ethylenedithio)-Tetrathiafulvalene (TM-BEDT-TTF) Revisited: Crystal Structures, Chiroptical Properties, Theoretical Calculations, and a Complete Series of Conducting Radical Cation Salts
The (S,S,S,S) and (R,R,R,R) enantiomers of tetramethyl-bis(ethylenedithio)-tetrathiafulvalene (TM-BEDT-TTF) show equatorial conformation for the four methyl groups in the solid state, according to the single-crystal X-ray analyses. Theoretical calculations at the Density Functional Theory (DFT) and time-dependent (TD) DFT levels indicate higher gas phase stability for the axial conformer than the equatorial one by 1.25kcal center dot mole-1 and allow the assignment of the UV-vis and circular dichroism transitions. A complete series of radical cation salts of 1:1 stoichiometry with the triiodide anion I3- was obtained by electrocrystallization of both enantiopure and racemic forms of the don…
Mono- and Binuclear Copper(II) and Nickel(II) Complexes with the 3,6-Bis(picolylamino)-1,2,4,5-Tetrazine Ligand
Four new compounds of formulas [Cu(hfac)2(L)] (1), [Ni(hfac)2(L)] (2), [{Cu(hfac)2}2(µ-L)]·2CH3OH (3) and [{Ni(hfac)2}2(µ-L)]·2CH3CN (4) [Hhfac = hexafluoroacetylacetone and L = 3,6-bis(picolylamino)-1,2,4,5-tetrazine] have been prepared and their structures determined by X-ray diffraction on single crystals. Compounds 1 and 2 are isostructural mononuclear complexes where the metal ions [copper(II) (1) and nickel(II) (2)] are six-coordinated in distorted octahedral MN2O4 surroundings which are built by two bidentate hfac ligands plus another bidentate L molecule. This last ligand coordinates to the metal ions through the nitrogen atoms of the picolylamine fragment. Compounds 3 and 4 are cen…
Iron( ii ) and cobalt( ii ) complexes based on anionic phenanthroline-imidazolate ligands: reversible single-crystal-to-single-crystal transformations
A series of low-spin FeII and CoII complexes based on phenanthroline-imidazolate (PIMP) ligands are reported. The FeII complex (H9O4)[Fe(PIMP)3]·(C4H10O)2(H2O) (1a) shows reversible crystalline phase transformations to afford two new phases (H9O4)[Fe(PIMP)3]·(H2O) (1b) and (H9O4)[Fe(PIMP)3]·(C8H18O)(C4H10O)(H2O) (1c) by release of diethyl ether and absorption of diethyl/dibutyl ether, respectively. This reversible uptake/release of solvent molecules is a clear example of single-crystal-to-single-crystal transformation involving a discrete metal complex. On the other hand, the corresponding CoII complex (H9O4)[Co(PIMP)3]·(C4H10O)2(H2O)2 (2) does not exhibit similar phase transformations. In …
Co-existence of ferro- and antiferromagnetic interactions in a hexanuclear mixed-valence CoIII2MnII2MnIV2 cluster sustained by a multidentate Schiff base ligand
The successful utilization of the “direct synthesis” approach yielded the unprecedented hexanuclear complex of formula [Co2MnII2MnIV2(L1)4Cl2(μ3-O)2(dmf)4]·2dmf (1) (H3L is the Schiff base derived from the condensation of salicylaldehyde and 3-aminopropane-1,2-diol). Single crystal X-ray analysis revealed that 1 crystallizes in the monoclinic system P21/c and it contains a rare mixed-valence {CoIII2MnII2MnIV2(μ2-O)8(μ3-O)2} core where all metal ions are linked through the phenolato and alkoxo groups of the L3− ligand. Besides the charge balance resulting from the X-ray structure, the oxidation state of the metal ions has been confirmed by XPS spectroscopy. Cryomagnetic studies indicate the …
Enantiopure Conducting Salts of Dimethylbis(ethylenedithio)tetrathiafulvalene (DM‐BEDT‐TTF) with the Hexachlororhenate(IV) Anion
Invited for the cover of this issue is the group of Narcis Avarvari (CIMI team) at the Laboratory MOLTECH-Anjou, UMR 6200 CNRS – Universite d'Angers, France. The cover image shows the enantiopure tetrathiafulvalene precursors used for the preparation of chiral radical cation conducting salts, together with an artwork of their packing diagrams and the suggested mirror image relationship between them.
Enantiopure Conducting Salts of Dimethylbis(ethylenedithio)tetrathiafulvalene (DM‐BEDT‐TTF) with the Hexachlororhenate(IV) Anion (Eur. J. Inorg. Chem. 24/2014)
Radical cation salts of BEDT-TTF, enantiopure tetramethyl-BEDT-TTF, and TTF-Oxazoline (TTF-Ox) donors with the homoleptic TRISPHAT anion
International audience; The synthesis and crystal structures of five radical cation salts based on the organic donors bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF), racemic ethylenedithio-methyl-oxazoline-tetrathiafulvalene (EDT-TTF-MeOx) and the enantiopure (S,S,S,S) and (R,R,R,R) tetramethyl-bis(ethylenedithio)tetrathiafulvalene (TMBEDT-TTF) and the D3-symmetric anion tris(tetrachlorobenzenediolato)phosphate(V) (TRISPHAT) are reported. The salts are formulated as [BEDT-TTF][(rac)-TRISPHAT]·CH2Cl2 (1), [BEDT-TTF][(rac)-TRISPHAT]·2CH3CN (2), [(rac)-EDT-TTF-Ox][(rac)-TRISPHAT]·CH3CN (3), [(S,S,S,S)-TMBEDT-TTF][(rac)-TRISPHAT]·2CH3CN (4), and [(R,R,R,R)-TMBEDT-TTF][(rac)-TRISPHAT]·2CH3CN (…
Ferromagnetic coupling through spin polarization in the hexanuclear [MnII(3)CuII(3)] complex.
A novel Cu(II)-Mn(II) hexanuclear complex of formula [[MnCuL](3)(tma)](ClO(4))(3).8H(2)O [H(2)L = macrocyclic Robson proligand; H(3)tma = trimesic acid] has been obtained by connecting three heterobinuclear [Cu(II)Mn(II)L](2+) cationic species through the trimesate anion. The complex exhibits a C(3) rotational symmetry, imposed by the geometry of the bridging ligand. The interaction within each Mn(II)-Cu(II) pair is antiferromagnetic (J = -16.7 cm(-1)). A weak ferromagnetic coupling among the three S = 2 resulting spins through the tricarboxylato bridge leads to a S = 6 ground spin state, for which the spin polarization mechanism is responsible.
Synthesis of μ-C2S44− Cobalt Complexes by Activation of the 1,3,4,6-tetrathiapentalene-2,5-dione, and Electrochemical Study of [(Cp*Co)2(μ-C2S4)]
The bimetallic complex [Cp(*)Co)2(μ-C2S4)] in which the two metal centres are linked by an ethylenetetrathiolate C2S44− unit, was synthesized in high yield by oxidative addition of 1,3,4,6 tetrathiapentalene-2,5-dione to [Cp(*)Co(CO)2]. The X-ray crystal structure of the intermediate product Cp*Co(dmid) (dmid2− = 4,5-disulfanyl-1,3-dithiol-2-onate) is presented. The electrochemical behaviour of the [(Cp*Co)2(μ-C2S4)] complex was studied in detail in the oxidative range. This study has shown that the nature of the product obtained after oxidation depends on the presence of complexing agent in the solution. The mechanism has been elucidated in a CH2Cl2 solution in the presence of P(OMe)3. In …
Structural Diversity and Physical Properties of Paramagnetic Molecular Conductors Based on Bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) and the Tris(chloranilato)ferrate(III) Complex
International audience; Electrocrystallization of bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) in the presence of the tris(chloranilato)ferrate(III) [Fe(Cl2An)3]3– paramagnetic chiral anion in different stoichiometric ratios and solvent mixtures afforded three different hybrid systems formulated as [BEDT-TTF]3[Fe(Cl2An)3]·3CH2Cl2·H2O (1), δ-[BEDT-TTF]5[Fe(Cl2An)3]·4H2O (2), and α‴-[BEDT-TTF]18[Fe(Cl2An)3]3·3CH2Cl2·6H2O (3). Compound 1 presents an unusual structure without the typical alternating organic and inorganic layers, whereas compounds 2 and 3show a segregated organic–inorganic crystal structure where layers formed by Λ and Δ enantiomers of the paramagnetic complex, together with…
Structural, photophysical and magnetic properties of transition metal complexes based on the dipicolylamino-chloro-1,2,4,5-tetrazine ligand
International audience; The ligand 3-chloro-6-dipicolylamino-1,2,4,5-tetrazine (Cl-TTZ-dipica) 1, prepared by the direct reaction between 3,6-dichloro-1,2,4,5-tetrazine and di(2-picolyl)-amine, afforded a series of four neutral transition metal complexes formulated as [Cl-TTZ-dipica-MCl2]2, with M = Zn(II), Cd(II), Mn(II) and Co(II), when reacted with the corresponding metal chlorides. The dinuclear structure of the isostructural complexes was disclosed by single crystal X-ray analysis, clearly indicating the formation of [MII–(μ-Cl)2MII] motifs and the involvement of the amino nitrogen atom in semi-coordination with the metal centers, thus leading to distorted octahedral coordination geome…
CCDC 2070862: Experimental Crystal Structure Determination
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CCDC 1580448: Experimental Crystal Structure Determination
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CCDC 983736: Experimental Crystal Structure Determination
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CCDC 1835925: Experimental Crystal Structure Determination
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CCDC 1580449: Experimental Crystal Structure Determination
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CCDC 1045096: Experimental Crystal Structure Determination
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CCDC 1580450: Experimental Crystal Structure Determination
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CCDC 996584: Experimental Crystal Structure Determination
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CCDC 2070865: Experimental Crystal Structure Determination
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CCDC 996582: Experimental Crystal Structure Determination
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CCDC 1045094: Experimental Crystal Structure Determination
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CCDC 1945945: Experimental Crystal Structure Determination
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CCDC 1835922: Experimental Crystal Structure Determination
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CCDC 1045095: Experimental Crystal Structure Determination
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CCDC 926042: Experimental Crystal Structure Determination
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CCDC 926041: Experimental Crystal Structure Determination
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CCDC 1045093: Experimental Crystal Structure Determination
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CCDC 1835924: Experimental Crystal Structure Determination
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CCDC 1835923: Experimental Crystal Structure Determination
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CCDC 1819913: Experimental Crystal Structure Determination
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CCDC 926044: Experimental Crystal Structure Determination
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CCDC 2070864: Experimental Crystal Structure Determination
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CCDC 1835927: Experimental Crystal Structure Determination
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CCDC 996583: Experimental Crystal Structure Determination
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CCDC 1945944: Experimental Crystal Structure Determination
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CCDC 2070863: Experimental Crystal Structure Determination
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CCDC 1045097: Experimental Crystal Structure Determination
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CCDC 1835926: Experimental Crystal Structure Determination
Related Article: Alexandre Abhervé, Samia Benmansour, Carlos José Gómez-García, Narcis Avarvari|2018|CrystEngComm|20|4141|doi:10.1039/C8CE00561C
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Related Article: Flavia Pop, Steeve Laroussi, Thomas Cauchy, Carlos J. Gomez-Garcia, John D. Wallis,Narcis Avarvari|2013|Chirality|25|466|doi:10.1002/chir.22210