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5 results on '"POLE 2"'

1. Hierarchical Self-Assembly of Polyoxometalate-Based Organo Palladium(II) Metallomacrocycles via Electrostatic Interactions

Author

Raphaël Salles, Anna Proust, Aurélie Bernard, Guillaume Izzet, Christophe Desmarets, Qichun Zhang, Dalil Brouri, Etienne Derat, Benjamin Abécassis, Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Méthodes et Application en Chimie Organique (MACO), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Sorbonne Université (SU), Nanyang Technological University [Singapour], Edifices PolyMétalliques (E-POM), Architectures Moléculaires (A.R.C), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769)

Subjects
010405 organic chemistry, Small-angle X-ray scattering, POLE 2, POLE 1, Supramolecular chemistry, Solvation, chemistry.chemical_element, Ethylenediamine, 010402 general chemistry, 01 natural sciences, E-POM, ARC, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, Crystallography, chemistry, Polyoxometalate, [CHIM]Chemical Sciences, Self-assembly, Physical and Theoretical Chemistry, MACO, Protic solvent, Palladium
Abstract

International audience; The design and synthesis of a supramolecular square composed of polyoxometalate-based hybrid donors and ethylenediamine palladium(II) nodes are reported. The structure of the metallomacrocycle scaffold was inferred by diffusion NMR, small-angle X-ray scattering (SAXS), and molecular modeling. The metallomacrocycle scaffold that contains negatively and positively charged subunits can further self-assemble owing to a competition between the solvation energy of the discrete species and intermolecular electrostatic interactions. When the dissociating character of the solvent was lowered or when in the presence of a protic solvent, different types of multiscale organizations (vesicles and pseudo-1D structures) were selectively formed and were characterized by SAXS and transmission electron microscopy.

Published
2020

2. Modeling the Oxygen Vacancy at a Molecular Vanadium(III) Silica-Supported Catalyst

Author

Albert Solé-Daura, Céline Paris, Sébastien Blanchard, Yanling Li, Teng Zhang, Sarah Hostachy, Josep M. Poblet, Jorge J. Carbó, Geoffroy Guillemot, Anna Proust, Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, Edifices PolyMétalliques (E-POM), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), De la Molécule aux Nanos-objets : Réactivité, Interactions et Spectroscopies (MONARIS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Equipe de Recherche en Matériaux Moléculaires et Spectroscopies (ERMMES)

Subjects
010405 organic chemistry, Chemistry, POLE 2, Vanadium, chemistry.chemical_element, General Chemistry, 010402 general chemistry, 01 natural sciences, Biochemistry, E-POM, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, Paramagnetism, Colloid and Surface Chemistry, Physical chemistry, [CHIM]Chemical Sciences, ERMMES, Partial oxidation, Singlet state, Ground state, Tetrahydrofuran, Derivative (chemistry)
Abstract

Here we report on the use of a silanol-decorated polyoxotungstate, [SbW9O33(tBuSiOH)3]3\textendash (1), as a molecular support to describe the coordination of a vanadium atom at a single-site on silica surfaces. By reacting [V(Mes)3·thf] (Mes = 2,4,6-trimethylphenyl) with 1 in tetrahydrofuran, the vanadium(III) derivative [SbW9O33(tBuSiO)3V(thf)]3\textendash (2) was obtained. Compound 2 displays the paramagnetic behavior expected for a d2-VIII high spin complex (SQUID measurements) with a triplet electronic ground state (ca. 30 kcal·mol\textendash 1 more stable than the singlet, from DFT calculations). Compound 2 proves to be a reliable model for reduced isolated-vanadium atom dispersed on silica surfaces [(\equivSi\textemdash O)3VIII(OH2)], an intermediate that is often proposed in a Mars\textendash van Krevelen type mechanism for partial oxidation of light alcohols. Oxidation of 2 under air produced the oxo-derivative [SbW9O33(tBuSiO)3VO]3\textendash (3). In compound 2, the d2-electrons are localized in degenerated d(V) orbitals, whereas in the electronically analogous bireduced-[SbW9O33(tBuSiO)3VO]5\textendash, 3·(2e), one electron is localized on d(V) orbital and the second one is delocalized on the polyoxotungstic framework, leading to a unique case of a bireduced heteropolyanion derivative with completely decoupled d1-V(IV) and d1-W(V). Our body of experimental results (EPR, magnetic measurements, spectroelectrochemical studies, Raman spectroscopy) and theoretical studies highlights (i) the role of the apical ligand coordination, i.e., thf (σ-donor) vs oxo (π-donor), in destabilizing or stabilizing the d(V) orbitals relative to the d(W) orbitals, and (ii) a geometrical distortion of the O3VO entity that causes a splitting of the degenerated orbitals and the stabilization of one d(V) orbital in the bireduced compound 3·(2e).

Published
2018

3. Rapid Photoinduced Charge Injection into Covalent Polyoxometalate\textendash Bodipy Conjugates

Author

Black, Fiona A., Jacquart, Aurélie, Toupalas, Georgios, Alves, Sandra, Proust, Anna, Clark, Ian P., Gibson, Elizabeth A., Izzet, Guillaume, School of Chemistry, The University of Nottingham, University Park, Nottingham, NG7 2RD, UK., School of Chemistry, The University of Nottingham, University Park, Nottingham, NG7 2RD, UK. Code (UMR, EA, ...), Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Chimie Structurale Organique et Biologique (CSOB), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Edifices PolyMétalliques (E-POM), Central Laser Facility (CLF), STFC Rutherford Appleton Laboratory (RAL), and Science and Technology Facilities Council (STFC)-Science and Technology Facilities Council (STFC)

Subjects
POLE 3, POLE 2, [CHIM]Chemical Sciences, E-POM, CSOB
Published
2018

4. Photochromism and Dual-Color Fluorescence in a Polyoxometalate\textendashBenzospiropyran Molecular Switch

Author

Anna Proust, Arnaud Parrot, Guillaume Izzet, Stefano A. Serapian, Aurélie Jacquart, Anne Dolbecq, Aurélie Bernard, Carles Bo, Pierre Mialane, Olivier Oms, Rémi Métivier, Etienne Derat, Institut Parisien de Chimie Moléculaire (IPCM), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), Barcelona Institute of Science and Technology (BIST), Méthodes et Application en Chimie Organique (MACO), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Edifices PolyMétalliques (E-POM), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Universitat Rovira i Virgili, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Cachan (ENS Cachan), and Química Física i Inorgànica

Subjects
Polioxometal·lats, POLE 2, POLE 1, Population, 02 engineering and technology, 010402 general chemistry, Photochemistry, 01 natural sciences, Catalysis, Photochromism, Density functional calculations, E-POM, fluorescence, MACO, molecular photoswitches, photochromism, POLE 1, POLE 2, Polyoxometalates, [CHIM]Chemical Sciences, polyoxometalates, education, 1433-7851, Molecular switch, education.field_of_study, 010405 organic chemistry, Chemistry, Polyoxometalates, molecular photoswitches, General Medicine, General Chemistry, Química, 021001 nanoscience & nanotechnology, photochromism, Fluorescence, E-POM, Fluorescència, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Density functional calculations, Covalent bond, Polyoxometalate, density functional calculations, fluorescence, 0210 nano-technology, MACO, Two-dimensional nuclear magnetic resonance spectroscopy, Excitation, Fisicoquímica
Abstract

The photophysical properties of a Keggin-type polyoxometalate (POM) covalently bounded to a benzospir- opyran (BSPR) unit have been investigated. These studies reveal that both closed and open forms are emissive with distinct spectral features (lem (closed form) = 530 nm, lem (open form) = 670 nm) and that the fluorescence of the BSPR unit of the hybrid is considerably enhanced compared to BSPR parent compounds. While the fluorescence excitation energy of the BSPR reference compounds (370 nm) is close to the intense absorption responsible of the photochromic character (350 nm), the fluorescence excitation of the hybrid is shifted to lower energy (400 nm), improving the population of the emissive state. Combined NOESY NMR and theoretical calculations of the closed form of the hybrid give an intimate understanding of the conformation adopted by the hybrid and show that the nitroaryl moieties of the BSPR is folded toward the POM, which should affect the electronic properties of the BSPR. &nbsp

Published
2017
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5. Facile One-Pot Synthesis of Ruthenium(II) Quaterpyridine-Based Photosensitizers for Photocatalyzed Hydrogen Production

Author

Ilaria Ciofini, Elodie Rousset, Garry S. Hanan, Valérie Marvaud, Department of Chemistry [Montréal], McGill University = Université McGill [Montréal, Canada], Institut Parisien de Chimie Moléculaire (IPCM), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL), Edifices PolyMétalliques (E-POM), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
010405 organic chemistry, Chemistry, POLE 2, One-pot synthesis, Inorganic chemistry, chemistry.chemical_element, 010402 general chemistry, 01 natural sciences, 7. Clean energy, E-POM, 0104 chemical sciences, 3. Good health, Ruthenium, Catalysis, Inorganic Chemistry, chemistry.chemical_compound, Dimethylglyoxime, Excited state, Physical chemistry, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry, Cobalt, Visible spectrum, Hydrogen production
Abstract

We present here the efficient microwave-assisted synthesis and photophysical study of a family of ruthenium(II) complexes of the general formula [Ru(bpy)x(qpy)3-x]2+ (where bpy = 2,2'-bipyridine, qpy = 4,4':2',2'':4'',4'''-quaterpyridine, and x = 0, 1, 2 giving compounds 1 = [Ru(bpy)2(qpy)1]2+, 2 = [Ru(bpy)1(qpy)2]2+, and 3 = [Ru(qpy)3]2+). Compared to the standard reference, [Ru(bpy)3]2+ (τ = 870 ns, Φ = 9.5%), the complexes display longer-lived excited state lifetimes at room temperature (τ: 1 = 1440 ns, 2 = 1640 ns, 3 = 1780 ns) and improved quantum yields (Φ: 1 = 14%, 2 = 19%, 3 = 23%). Theoretical calculations were performed to support the interpretation of these photophysical properties. These complexes are excellent photosensitizers as they absorb light throughout the visible spectrum, have excellent excited state lifetimes at room temperature, and have high quantum yields. In combination with a cobalt dimethylglyoxime catalyst, they exhibit remarkable hydrogen evolution with blue light, and they are far more efficient than the reference in the field, [Ru(bpy)3]2+.

Published
2017

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