Jean-Yves Saillard

Université de Rennes 1, Roazhon, Brittany, France

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Publications (144)469.52 Total impact

  • [Show abstract] [Hide abstract]
    ABSTRACT: The first example of ligand protected Cu-Zn clusters is described. Reaction of [CpCu(CN(t)Bu)] with [Zn2Cp*2] yields [(CuCN(t)Bu)4(ZnCp*)4] () and [(CuCN(t)Bu)4(ZnCp*)3(ZnCp)] (). According to DFT calculations, the [Cu4Zn4] unit fulfils the unified superatom model for cluster valence shell closing.
    Chemical communications (Cambridge, England). 06/2014;
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    ABSTRACT: Thirteen novel dipolar and V-shaped chromophores with pyranylidene electron-donating part, diazine electron-withdrawing part and various -linkers were synthesized. The extent of intramolecular charge transfer, structure-property relationships and optical properties were further investigated by UV/Vis absorption, electrochemistry and DFT calculations.
    Tetrahedron 02/2014; · 2.80 Impact Factor
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    ABSTRACT: Three new halide-centered octanuclear silver(I) complexes, [Ag8(X){S2P(CH2CH2Ph)2}6](PF6), X = F(-), 1; Cl(-), 2; Br(-), 3; were prepared in the presence of the corresponding halide anions with silver(I) salts and dithiophosphinate ligands. Structure analyses displayed that a Ag8 cubic core can be modulated by the size effect of the central halide; however, an iodide-centered Ag8 cluster was not found under similar reaction conditions. Interestingly, a luminescent dodecanuclear silver(I) cluster, [Ag12(μ12-I)(μ3-I)4{S2P(CH2CH2Ph)2}6](I), 4; was then synthesized. The structure of 4 contains a novel μ12-I at the center of a cuboctahedral silver(I) atom cage, which is further stabilized by four additional μ3-I and six dithiophosphinate ligands. To the best of our knowledge, the μ12-I revealed in 4 is the highest coordination number for a halide ion authenticated by both experimental and computational studies. Previously, the μ12-I was only observed in [PyH][{TpMo(μ3-S)4Cu3}4(μ12-I)]. The synthetic details, spectroscopic studies including multinuclear NMR and ESI-MS, structure elucidations by single crystal X-ray diffraction, and photoluminescence of 4 are reported herein.
    Inorganic Chemistry 01/2014; · 4.59 Impact Factor
  • Journal of Organometallic Chemistry 01/2014; 761:1–9. · 2.00 Impact Factor
  • Source
    Camille Latouche, C W Liu, Jean-Yves Saillard
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    ABSTRACT: Cu(I) and Ag(I) can form with 1,1-dithio(seleno) ligands various types of clusters, the framework of which being maintained by the metal–chalcogen bonds provided by the bridging ligands. The metal centers are generally tricoordinated and consequently possess an accepting orbital of valence s and/or p character. There is no formal metal–metal bonding, but only weak d10–d10 interactions which favor the overlap between the metal accepting orbitals. Their bonding combinations are generally suited for interacting with the occupied valence orbitals of an encapsulated anion. Thus, many of these clusters are able to encapsulate anions, a situation which tends to stabilize the whole structure through building of significant host–guest bonding. Not only is the anion encapsulation effect to stabilize the cluster cage, but it can also significantly modify its structure, or act as a template in the stabilization of species which would not exist as empty clusters. This paper reviews the synthesis, structure and bonding of all the known clusters of d10 metals decorated with 1,1-dichalchogeno ligands and containing entrapped atomic anions. Their structures are analyzed with respect to size and shape. The photoluminescence properties of some of them are discussed.
    Journal of Cluster Science 12/2013; · 1.11 Impact Factor
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    ABSTRACT: Whereas stable octanuclear clusters of the type M(I)8(E(∩)E)6 (M = Cu, Ag; E(∩)E = dithio or diseleno ligand) are known for being able to encapsulate a hydride or main-group anion under some circumstances, only the related hydride-containing heptanuclear [M(I)]7(H)(E(∩)E)6 and empty hexanuclear [M(I)]6(E(∩)E)6 species have been characterized so far. In this paper we investigate by the means of theoretical calculations and experiments the viability of empty and anion-centered clusters of the type [Cu(I)]7(X)(E(∩)E)6 and [Cu(I)]6(X)(E(∩)E)6 (X = vacancy, H or a main-group atom). The theoretical prediction for the existence of anion-containing heptanuclear species, the shape of which is modulated by the anion nature and size, have been fully confirmed by the synthesis and characterization of [Cu7(X){S2P(O(i)Pr)2}6] (X = H, Br). This consistency between experiment and theory allows us to predict the stability and shape-modulated structure of a whole series of [Cu(I)]7(X)(E(∩)E)6 (X = vacancy, H, O, S, halogen) and [Cu(I)]6(X)(E(∩)E)6 (X = H, halogen) clusters.
    Inorganic Chemistry 10/2013; · 4.59 Impact Factor
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    ABSTRACT: M8L6 clusters (M = Cu(I), Ag(I); L = dichalcogeno ligand) are known for their ability to encapsulate various kinds of saturated atomic anions. Calculations on the models [M8(E2PH2)6](2+) (M = Cu(I), Ag(I); E = S, Se) and the ionic or neutral [M8(X)(E2PH2)6](q) (X = H, F, Cl, Br, O, S, Se, N, P, C) indicate that the cubic M8L6 cage adapts its shape for maximizing the host-guest bonding interaction. The interplay between size, covalent and ionic bonding favors either a cubic, tetracapped tetrahedral, or bicapped octahedral structure of the metal framework. Whereas the large third- and fourth-row main group anions maintain the cubic shape, a distortion toward a tetracapped tetrahedral arrangement of the metals occurs in the case of hydride, fluoride, and oxide. The distortion is strong in the case of hydride, weak in the case of fluoride, and intermediate in the case of oxide. Density functional theory (DFT) calculations predict a bicapped octahedral architecture in the case of nitride and carbide. These computational results are supported by X-ray structures, including those of new fluorine- and oxygen-containing compounds. It is suggested that other oxygen-containing as well as so far unknown nitride-containing clusters should be feasible. For the first time, the dynamical behavior of the encapsulated hydride has been investigated by metadynamics simulations. Our results clearly demonstrate that the interconversion mechanism between two identical tetracapped tetrahedral configurations occurs through a succession of M-H bonds breaking and forming which present very low activation energies and which involve a rather large number of intermediate structures. This mechanism is full in accordance with (109)Ag and (1)H state NMR measurements.
    Inorganic Chemistry 07/2013; 52(13):7752-7765. · 4.59 Impact Factor
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    ABSTRACT: Electro or chemical oxidation of ferrocenylmethylenepyran gave an ethanediferrocenylbispyrylium salt through the dimerization of a ferrocenylpyran radical-cation (C–C bond making). Electro or chemical reduction gave back the ferrocenylmethylenepyran (C–C bond breaking). This electrochemical reverse system constitutes an example of C–C bond making–breaking process in a metallocenyl series with rather high stability. DFT calculations and electrochemical studies were carried out in order to determine the electronic structure of the radical cation intermediate, the role of the ferrocenyl groups and the mechanism of the C–C bond making and C–C bond breaking processes. Reversible deprotonation of the ethanediferrocenylbispyrylium salt afforded an extended diferrocenylbismethylenepyran, which was subsequently reversibly oxidized to an ethenediferrocenylbispyrylium salt. X-Ray crystallographic data of diferrocenylbismethylenepyran and ethenediferrocenylbispyrylium salt allowed to determine the molecular movements, which come with the electron transfer (ET). A comparison with the behavior of the corresponding isoelectronic bisdithiafulvenes (extended TTF) and bisdithiolium salts was made.
    New Journal of Chemistry 06/2013; 37(7):2066-2081. · 2.97 Impact Factor
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    ABSTRACT: Primary and secondary amines react with ethynylcobalticinium under mild conditions in the absence of a catalyst and an additional solvent to give quantitative yields of dark-red microcrystalline cobalticinium trans-enamines that show a remarkable push-pull electronic structure.
    Chemical Communications 05/2013; · 6.38 Impact Factor
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    ABSTRACT: Full geometry optimization has been carried out for all the low-energy isomers of M(indenyl)2 (M = Sc–Ni, Y–Mo, Re, Ru–Pd). Depending on the electron-richness of the molecule, indenyl adopts various hapticities, some of them involving full or partial coordination of the C6 ring. Our results suggest that a judicious choice of substituents on the ligands should lead to the stabilization of η6-coordinated indenyl ligands. Indenyl is also shown to be quite flexible with respect to the spin ground state. Substituted iron and nickel bis-indenyl species should be characterizable in their triplet state. Thus, both from the point of view of coordination and the metal spin ground state, indenyl and cyclopentadienyl appear to behave quite differently.
    New Journal of Chemistry 05/2013; · 2.97 Impact Factor
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    ABSTRACT: An unprecedented air-stable, nanospheric polyhydrido copper cluster [Cu20(H)11(S2P(OiPr)2)9] (1H), which is the first example of elongated triangular orthobicupola copper atom array of C3h symmetry, was synthesized and characterized. Its composition is primarily determined by ESI mass spectrometry, and fully characterized by NMR (1H, 2H and 31P), and single crystal X-ray diffraction. The structure of complex 1H can be expressed by a trigonal-bipyramidal unit of [Cu2H5]3- anchored within an elongated triangular orthobicupola polyhedron of eighteen copper atoms, which is further stabilized by eighteen sulphur atoms from nine dithiophosphate ligands and six capping hydrides. The positions of eleven hydrides revealed from the low temperature X-ray diffraction was supported by a density functional theory (DFT) investigation on a simplified model [Cu20H11(S2PH2)9] of C3h symmetry. 1H is capable of releasing H2 gas under irradiation of sunlight, mild thermal condition (at 65 oC), or in the presence of acids at RT.
    Journal of the American Chemical Society 03/2013; · 10.68 Impact Factor
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    ABSTRACT: Reactions of Ag(I) salt, NH(4)(E(2)P(OR)(2)) (R = (i)Pr, Et; E = Se, S), and NaBH(4) in a 7:6:1 ratio in CH(2)Cl(2) at room temperature, led to the formation of hydride-centered heptanuclear silver clusters, [Ag(7)(H){E(2)P(OR)(2)}(6)] (R = (i)Pr, E = Se (3): R = Et; E = S(4). The reaction of [Ag(10)(E){E(2)P(OR)(2)}(8)] with NaBH(4) in CH(2)Cl(2) produced [Ag(8)(H){E(2)P(OR)(2)}(6)](PF(6)) (R = (i)Pr, E = Se (1): R = Et; E = S(2)), which can be converted to clusters 3 and 4, respectively, via the addition of 1 equiv of borohydride. Intriguingly clusters 1 and 2 can be regenerated via adding 1 equiv of Ag(CH(3)CN)(4)PF(6) to the solution of compounds 3 and 4, respectively. All complexes have been fully characterized by NMR ((1)H, (77)Se, (109)Ag) spectroscopy, UV-vis, electrospray ionization mass spectrometry (ESI-MS), FT-IR, thermogravimetric analysis (TGA), and elemental analysis, and molecular structures of 3(H) and 4(H) were clearly established by single crystal X-ray diffraction. Both 3(H) and 4(H) exhibit a tricapped tetrahedral Ag(7) skeleton, which is inscribed within an E(12) icosahedron constituted by six dialkyl dichalcogenophosphate ligands in a tetrametallic-tetraconnective (μ(2), μ(2)) bonding mode. Density functional theory (DFT) calculations on the models [Ag(7)(H)(E(2)PH(2))(6)] (E = Se: 3'; E = S: 4') yielded to a tricapped, slightly elongated tetrahedral silver skeleton, and time-dependent DFT (TDDFT) calculations reproduce satisfyingly the UV-vis spectrum with computed transitions at 452 and 423 nm for 3' and 378 nm for 4'. Intriguingly further reactions of [Ag(7)(H){E(2)P(OR)(2)}(6)] with 8-fold excess amounts of NaBH(4) produced monodisperse silver nanoparticles with an averaged particle size of 30 nm, which are characterized by scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, X-ray diffraction (XRD), and UV-vis absorption spectrum.
    Inorganic Chemistry 02/2013; · 4.59 Impact Factor
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    ABSTRACT: The structure and optical properties of several polynuclear gold(I) species, namely, diselenophosphate [Au{μ-Se(2)P(OR)(2)}](2) complexes (R = (i)Pr, Et, (n)Pr) respectively numbered 1, 2, and 3 and number 4 [Au{μ-Se(2)P(CH(2))(2)Ph)(2)}](2), exhibiting interesting structural, absorption, and emission properties have been studied. The synthesis, full characterization, and experimental spectroscopic study of 3 and 4 have first been carried out, 1 and 2 being previously studied. In the solid state, 3 gives polymers, like 1 and 2, whereas 4 exists under a dinuclear monomeric form. The absorption and phosphorescence properties of 4 have been rationalized using DFT and TDDFT computations. In particular, Au-Au bonding seems to appear in its first singlet and triplet states, whereas such a bond does not exist in the ground state. Then, the influence of polymerization through aurophilic bonding on the optical properties of 2 is investigated (1 and 3 behave as 2). It is shown using TDDFT computations that its observed UV-visible excitation spectrum in solution is due to high oligomers and not to monomers or low size oligomers. ESI-MS molecular weight measurements confirm the occurrence of such oligomers of 2 in solution. An assignment of the observed bands of 2 is proposed. The transition corresponding to the first excitation band, which is mainly a HOMO to LUMO one, exhibits metal-centered character, i.e., a gold 5d to 6p orbital transition, but concomitantly transfers significant electron density from gold to phosphorus atoms so that it is also a MLCT one.
    Inorganic Chemistry 10/2012; · 4.59 Impact Factor
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    ABSTRACT: Two luminescent, undecanuclear silver complexes [Ag(11)(μ(9)-I)(μ(3)-I)(3){E(2)P(O(i)Pr)(2)}(6)](PF(6)) [E = S (yellow), 1; Se (orange), 2], containing the first μ(9)-iodine inscribed at the center of a pentacapped trigonal-prismatic silver skeleton, were reported.
    Inorganic Chemistry 06/2012; 51(14):7439-41. · 4.59 Impact Factor
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    ABSTRACT: Reactions of Cu(I) salts with Na(S(2)CR) (R = N(n)Pr(2), NEt(2), aza-15-crown-5), and (Bu(4)N)(BH(4)) in an 8:6:1 ratio in CH(3)CN solution at room temperature yield the monocationic hydride-centered octanuclear Cu(I) clusters, [Cu(8)(H){S(2)CR}(6)](PF(6)) (R = N(n)Pr(2), 1(H); NEt(2), 2(H); aza-15-crown-5, 3(H)). Further reactions of [Cu(8)(H){S(2)CR}(6)](PF(6)) with 1 equiv of (Bu(4)N)(BH(4)) produced neutral heptanuclear copper clusters, [Cu(7)(H){S(2)CR}(6)] (R = N(n)Pr(2), 4(H); NEt(2), 5(H); aza-15-crown-5, 6(H)) and clusters 4-6 can also be generated from the reaction of Cu(BF(4))(2), Na(S(2)CR), and (Bu(4)N)(BH(4)) in a 7:6:8 molar ratio in CH(3)CN. Reformation of cationic Cu(I)(8) clusters by adding 1 equiv of Cu(I) salt to the neutral Cu(7) clusters in solution is observed. Intriguingly, the central hydride in [Cu(8)(H){S(2)CN(n)Pr(2)}(6)](PF(6)) can be oxidatively removed as H(2) by Ce(NO(3))(6)(2-) to yield [Cu(II)(S(2)CN(n)Pr(2))(2)] exploiting the redox-tolerant nature of dithiocarbamates. Regeneration of hydride-centered octanuclear copper clusters from the [Cu(II)(S(2)CN(n)Pr(2))(2)] can be achieved by reaction with Cu(I) ions and borohydride. The hydride release and regeneration of Cu(I)(8) was monitored by UV-visible titration experiments. To our knowledge, this is the first time that hydride encapsulated within a copper cluster can be released as H(2) via chemical means. All complexes have been fully characterized by (1)H NMR, FT-IR, UV-vis, and elemental analysis, and molecular structures of 1(H), 2(H), and 6(H) were clearly established by single-crystal X-ray diffraction. Both 1(H) and 2(H) exhibit a tetracapped tetrahedral Cu(8) skeleton, which is inscribed within a S(12) icosahedron constituted by six dialkyl dithiocarbamate ligands in a tetrametallic-tetraconnective (μ(2), μ(2)) bonding mode. The copper framework of 6(H) is a tricapped distorted tetrahedron in which the four-coordinate hydride is demonstrated to occupy the central site by single crystal neutron diffraction. Compounds 1-3 exhibit a yellow emission in both the solid state and in solution under UV irradiation at 77 K, and the structureless emission is assigned as a (3)metal to ligand charge transfer (MLCT) excited state. Density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations on model compounds match the experimental structures and provide rationalization of their bonding and optical properties.
    Inorganic Chemistry 06/2012; 51(12):6577-91. · 4.59 Impact Factor
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    ABSTRACT: Three copper(I) iodide clusters coordinated by different phosphine ligands formulated [Cu(4)I(4)(PPh(3))(4)] (1), [Cu(4)I(4)(Pcpent(3))(4)] (2), and [Cu(4)I(4)(PPh(2)Pr)(4)] (3) (PPh(3) = triphenylphosphine, Pcpent(3) = tricyclopentylphosphine, and PPh(2)Pr = diphenylpropylphosphine) have been synthesized and characterized by (1)H and (31)P NMR, elemental analysis and single crystal X-ray diffraction analysis. They crystallize in different space groups, namely, monoclinic P21/c, cubic Pa ̅3, and tetragonal I ̅42m for 1, 2, and 3, respectively. The photoluminescence properties of clusters 1 and 3 show reversible luminescence thermochromism with two highly intense emission bands whose intensities are temperature dependent. In accordance to Density Functional Theory (DFT) calculations, these two emission bands have been attributed to two different transitions, a cluster centered (CC) one and a mixed XMCT/XLCT one. Cluster 2 does not exhibit luminescence variation in temperature because of the lack of the latter transition. The absorption spectra of the three clusters have been also rationalized by time dependent DFT (TDDFT) calculations. A simplified model is suggested to represent the luminescence thermochromism attributed to the two different excited states in thermal equilibrium. In contrast with the pyridine derivatives, similar excitation profiles and low activation energy for these phosphine-based clusters reflect high coupling of the two emissive states. The effect of the Cu-Cu interactions on the emission properties of these clusters is also discussed. Especially, cluster 3 with long Cu-Cu contacts exhibits a controlled thermochromic luminescence which is to our knowledge, unknown for this family of copper iodide clusters. These phosphine-based clusters appear particularly interesting for the synthesis of original emissive materials.
    Inorganic Chemistry 09/2011; 50(21):10682-92. · 4.59 Impact Factor
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    ABSTRACT: DFT calculations with full geometry optimization have been performed on the series (CpM)2(as-indacene) and (CpM)2(s-indacene) (M = Mn, Fe, Co, Ni), as well as on the cations of the Fe, Co and Ni complexes. The compounds where M = Fe and Ni (as-indacene series) and M = Mn, Fe and Co (s-indacene series) were found to possess closed-shell ground states. In the mixed-valent cations as well as in the other open-shell species, the degree of metal–metal communication and the participation of the ligand into the spin density were evaluated. In general, the larger the total electron number, the larger the metal–metal communication and ligand participation to the frontier orbitals.
    New Journal of Chemistry 09/2011; 35(10):2136-2145. · 2.97 Impact Factor
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    ABSTRACT: The first elemental cluster with hexacapped trigonal bipyramidal geometry is revealed in the luminescent undecanuclear silver complex which is stabilized by nine dithiocarbamate ligands and has an interstitial hydride. The hydride position within the Ag(11) cage is confirmed by a DFT investigation.
    Chemical Communications 05/2011; 47(20):5831-3. · 6.38 Impact Factor
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    ABSTRACT: A new cluster family of the type [Ag11(S){S2P(OR)2}8]+ (R=Et, Pr, iPr) has been synthesized and characterized as their hexafluorophosphate salts. These compounds are the first silver dithiophosph(in)ato complexes exhibiting photoluminescence at ambient temperature. Their unprecedented skeletal structure describes a very distorted pentacapped trigonal-prismatic polyhedron. Geometry optimizations by DFT calculations on the R=H model reproduce the same structural arrangement in the ground state. Its electronic structure exhibits a low-lying LUMO with a large Ag(5s/5p) character whereas the highest occupied levels have a major contribution from the ligand sulfur lone pairs. The above-mentioned orbitals are shown to be responsible for the optical absorption and emission properties of these compounds. KeywordsSilver–Sulfur–Cluster–Absorption–Emission
    Journal of Cluster Science 01/2011; 22(3):381-396. · 1.11 Impact Factor
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    ABSTRACT: Density functional theory (DFT) calculations on the model [{FeCp(dpe)}(2){1,4-C(6)H(4)(CN)(2)}](2+) (3(2+); dpe = diphosphinoethane) of salts of the cations [{FeCp(dppe)}(2){1,4-C(6)H(4)(CN)(2)}](2+) (1(2+); dppe = 1,2-bis[diphenyldiphosphino]ethane) and [{FeCp*(CO)(2)}(2){1,4-C(6)H(4)(CN)(2)}](2+) (2(2+)), for which the X-ray crystal structures have been determined, as well as on its isomer [{FeCp(dpe)}(2){1,3-C(6)H(4)(CN)(2)}](2+) (4(2+)) and on the related complex [{FeCp(dpe)}(3){1,3,5-C(6)H(3)(CN)(3)}](3+) (5(2+)), indicate that the highest occupied molecular orbitals (HOMOs) of these compounds are localized on the metal centers with negligible participation of the C(6) ring. Thus, the poly(nitrile)phenylene ligand efficiently quenches the electronic communication between the metal centers. This is at variance with the related isoelectronic polyacetylene phenylene complexes, in which the iron centers have been shown to be electronically coupled. Consistently, apart from the case of 3(3+), which shows some degree of delocalization, all of the oxidized forms of 3(2+), 4(2+), and 5(2+) can be described as class II, localized mixed-valent species, in agreement with the electrochemical data showing two close oxidation potentials around 1 V vs FeCp*(2). This is at variance with the p-phenylene-bridged biethynyldiiron analogue, for which extended electronic delocalization was earlier shown to provide greater degree of delocalization of the mixed valency. Time-dependent DFT calculations on 3(2+), 4(2+), and 5(2+) indicate that the lowest-energy absorption band is associated with metal-to-ligand charge-transfer transitions involving the metallic HOMOs and the two lowest unoccupied molecular orbitals that derive from the lowest π*(phenylene) orbitals with some π*(CN) bonding admixture.
    Inorganic Chemistry 01/2011; 50(1):114-24. · 4.59 Impact Factor

Publication Stats

288 Citations
469.52 Total Impact Points

Institutions

  • 1996–2014
    • Université de Rennes 1
      • Institut des Sciences Chimiques de Rennes (ISCR) - UMR CNRS 6226
      Roazhon, Brittany, France
  • 2013
    • University of Bordeaux
      Burdeos, Aquitaine, France
  • 2009–2013
    • National Dong Hwa University
      • Department of Chemistry
      Hualian, Taiwan, Taiwan
  • 2002–2013
    • French National Centre for Scientific Research
      Lutetia Parisorum, Île-de-France, France
    • University of Santiago, Chile
      CiudadSantiago, Santiago, Chile
    • University of Chile
      • Facultad de Ciencias Químicas y Farmacéuticas
      Santiago, Region Metropolitana de Santiago, Chile
  • 1993–2013
    • Université de Rennes 2
      Roazhon, Brittany, France
  • 2007–2010
    • Pontificia Universidad Católica de Valparaíso
      • Institute of Chemistry
      Valparaíso, Region de Valparaiso, Chile
    • Universität Regensburg
      • Institut für Anorganische Chemie
      Regensburg, Bavaria, Germany
    • Universidad Andrés Bello
      • Faculty of Ecology and Natural Resources
      CiudadSantiago, Santiago, Chile
    • University of Notre Dame
      • Department of Chemistry and Biochemistry
      Indiana, PA, United States
  • 2004
    • Ecole Nationale Supérieure de Chimie de Rennes
      Roazhon, Brittany, France
  • 1994–1997
    • Rice University
      • Department of Chemistry
      Houston, Texas, United States