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1. Spotlight on the Life Cycle of Acrylamide-Based Polymers Supporting Reductions in Environmental Footprint: Review and Recent Advances

Author

Olivier Braun, Clément Coquery, Johann Kieffer, Frédéric Blondel, Cédrick Favero, Céline Besset, Julien Mesnager, François Voelker, Charlène Delorme, and Dimitri Matioszek

Subjects
water soluble polymer, sustainable process, macromolecular engineering, raw material sourcing, reduced industrial footprint, polymer fate assessment, Organic chemistry, QD241-441
Abstract

Humankind is facing a climate and energy crisis which demands global and prompt actions to minimize the negative impacts on the environment and on the lives of millions of people. Among all the disciplines which have an important role to play, chemistry has a chance to rethink the way molecules are made and find innovations to decrease the overall anthropic footprint on the environment. In this paper, we will provide a review of the existing knowledge but also recent advances on the manufacturing and end uses of acrylamide-based polymers following the “green chemistry” concept and 100 years after the revolutionary publication of Staudinger on macromolecules. After a review of raw material sourcing options (fossil derivatives vs. biobased), we will discuss the improvements in monomer manufacturing followed by a second part dealing with polymer manufacturing processes and the paths followed to reduce energy consumption and CO2 emissions. In the following section, we will see how the polyacrylamides help reduce the environmental footprint of end users in various fields such as agriculture or wastewater treatment and discuss in more detail the fate of these molecules in the environment by looking at the existing literature, the regulations in place and the procedures used to assess the overall biodegradability. In the last section, we will review macromolecular engineering principles which could help enhance the degradability of said polymers when they reach the end of their life cycle.

Published
2021
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2. Spotlight on the Life Cycle of Acrylamide-Based Polymers Supporting Reductions in Environmental Footprint: Review and Recent Advances

Author

Olivier Braun, Clément Coquery, Johann Kieffer, Frédéric Blondel, Cédrick Favero, Céline Besset, Julien Mesnager, François Voelker, Charlène Delorme, and Dimitri Matioszek

Subjects
Pharmaceutical Science, Organic chemistry, Review, sustainable process, reduced industrial footprint, Analytical Chemistry, water soluble polymer, polymer fate assessment, QD241-441, Chemistry (miscellaneous), Drug Discovery, polyacrylamide handprint, Molecular Medicine, raw material sourcing, Physical and Theoretical Chemistry, macromolecular engineering
Abstract

Humankind is facing a climate and energy crisis which demands global and prompt actions to minimize the negative impacts on the environment and on the lives of millions of people. Among all the disciplines which have an important role to play, chemistry has a chance to rethink the way molecules are made and find innovations to decrease the overall anthropic footprint on the environment. In this paper, we will provide a review of the existing knowledge but also recent advances on the manufacturing and end uses of acrylamide-based polymers following the “green chemistry” concept and 100 years after the revolutionary publication of Staudinger on macromolecules. After a review of raw material sourcing options (fossil derivatives vs. biobased), we will discuss the improvements in monomer manufacturing followed by a second part dealing with polymer manufacturing processes and the paths followed to reduce energy consumption and CO2 emissions. In the following section, we will see how the polyacrylamides help reduce the environmental footprint of end users in various fields such as agriculture or wastewater treatment and discuss in more detail the fate of these molecules in the environment by looking at the existing literature, the regulations in place and the procedures used to assess the overall biodegradability. In the last section, we will review macromolecular engineering principles which could help enhance the degradability of said polymers when they reach the end of their life cycle.

Published
2022

3. Experimental and Theoretical Comparison of Addition–Fragmentation Pathways of Diseleno- and Dithiocarbamate RAFT Agents

Author

Dimitri Matioszek, Stéphane Mazières, Ching Yeh Lin, Oleksii Brusylovets, Simon Harrisson, Michelle L. Coote, Mathias Destarac, Interactions moléculaires et réactivité chimique et photochimique (IMRCP), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD), ARC Centre of Excellence in Free Radical Chemistry and Biotechnology, affiliation inconnue, Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Institut Ecologie et Environnement (INEE), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Fédération de Recherche Fluides, Energie, Réacteurs, Matériaux et Transferts (FERMAT), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), P3R - Polymères de Précision par Procédés Radicalaires (P3R), and Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT)

Subjects
chemistry.chemical_classification, Polymers and Plastics, Organic Chemistry, Chain transfer, 02 engineering and technology, Raft, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Adduct, Inorganic Chemistry, chemistry.chemical_compound, Monomer, chemistry, Fragmentation (mass spectrometry), Polymer chemistry, Materials Chemistry, Vinyl acetate, [CHIM]Chemical Sciences, Reactivity (chemistry), 0210 nano-technology, Dithiocarbamate, ComputingMilieux_MISCELLANEOUS
Abstract

Theoretical studies suggest that identically substituted dithio- and diselenocarbamate reversible addition–fragmentation chain transfer (RAFT) agents will have similar reactivity but that diselenocarbamate RAFT agents are more likely to undergo intermediate radical termination. These results are supported by an experimental study of polymerizations of vinyl acetate mediated by Se-cyanomethyl N,N-dimethyldiselenocarbamate (1Se) and its sulfur analog, S-cyanomethyl N,N-dimethyldithiocarbamate (1S). While the two polymerizations had similar interchain transfer constants (3.2 for 1S and 3.9 for 1Se), significant retardation was observed for 1Se-mediated polymerizations. External chain transfer constants were also measured for 1S (5.4) and 1Se (45). The low apparent value of the chain transfer constant of 1S is attributed to the selective formation of a single monomer adduct in the early stages of the reaction.

Published
2019
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4. Reversible Deactivation Radical Polymerization: Mechanisms and Synthetic Methodologies

Author

Krzysztof Matyjaszewski, Haifeng Gao, Brent Sumerlin, Nicolay V. Tsarevsky, Sivaprakash Shanmugam, Nicholas S. Hill, Benjamin B. Noble, Michelle L. Coote, Atsushi Kajiwara, Joris J Haven, Matthew Hendrikx, Tanja Junkers, Pieter J Leenaers, Theodora Tsompanoglou, Cyrille Boyer, Jiangtao Xu, Almar Postma, Graeme Moad, Jason C. Morris, Jean-Louis Clément, Yohann Guillaneuf, Steven E. Bottle, Kathryn Fairfull-Smith, Didier Gigmes, Thomas G. Ribelli, S. M. Wahidur Rahaman, Rinaldo Poli, Francesca Lorandi, Marco Fantin, Francesco De Bon, Abdirisak A. Isse, Armando Gennaro, David C. McLeod, Kapil Dev Sayala, Vignesh Vasu, Joon-Sung Kim, Hyun-Seok Yu, William I. Bannerman, Mark E. Johnson, Alexandru D. Asandei, Carlos M. R. Abreu, Ana C. Fonseca, Nuno M. P. Rocha, James T. Guthrie, Arménio C. Serra, Jorge F. J. Coelho, G. Yilmaz, C. Kutahya, A. Allushi, C. Aydogan, S. Aykac, Y. Yagci, Mathias Destarac, Dimitri Matioszek, Xavier Vila, Juliette Ruchmann-Sternchuss, Samir Z. Zard, Thomas G. McKenzie, Amin Reyhani, Mitchell D. Nothling, Greg G. Qiao, Kotaro, Krzysztof Matyjaszewski, Haifeng Gao, Brent Sumerlin, Nicolay V. Tsarevsky, Sivaprakash Shanmugam, Nicholas S. Hill, Benjamin B. Noble, Michelle L. Coote, Atsushi Kajiwara, Joris J Haven, Matthew Hendrikx, Tanja Junkers, Pieter J Leenaers, Theodora Tsompanoglou, Cyrille Boyer, Jiangtao Xu, Almar Postma, Graeme Moad, Jason C. Morris, Jean-Louis Clément, Yohann Guillaneuf, Steven E. Bottle, Kathryn Fairfull-Smith, Didier Gigmes, Thomas G. Ribelli, S. M. Wahidur Rahaman, Rinaldo Poli, Francesca Lorandi, Marco Fantin, Francesco De Bon, Abdirisak A. Isse, Armando Gennaro, David C. McLeod, Kapil Dev Sayala, Vignesh Vasu, Joon-Sung Kim, Hyun-Seok Yu, William I. Bannerman, Mark E. Johnson, Alexandru D. Asandei, Carlos M. R. Abreu, Ana C. Fonseca, Nuno M. P. Rocha, James T. Guthrie, Arménio C. Serra, Jorge F. J. Coelho, G. Yilmaz, C. Kutahya, A. Allushi, C. Aydogan, S. Aykac, Y. Yagci, Mathias Destarac, Dimitri Matioszek, Xavier Vila, Juliette Ruchmann-Sternchuss, Samir Z. Zard, Thomas G. McKenzie, Amin Reyhani, Mitchell D. Nothling, Greg G. Qiao, and Kotaro

Subjects
Polymerization--Thermodynamics, Acrylates--Analysis, Alkoxides--Analysis, Vinyl chloride polymers--Analysis, Butadiene--Synthesis, Epoxy compounds--Reactivity, Copolymers--Synthesis, Lewis acids--Mechanism of action, Crosslinking (Polymerization), Polymerization, Addition polymerization, Electron paramagnetic resonance--Application, Copolymers, Polymerization--Methodology, Epoxy compounds, Hydroxyl group--Reactivity, Xanthates--Reactivity, Addition polymerization--Technological innovations, Elect
Published
2018

6. Reversible addition-fragmentation chain-transfer polymerization of vinyl monomers with N,N- dimethyldiselenocarbamates

Author

Oleksii Brusylovets, Dimitri Matioszek, Mathias Destarac, D. James Wilson, and Stéphane Mazières

Subjects
Polymers and Plastics, Chemistry, Organic Chemistry, Chain transfer, Photochemistry, Ring-opening polymerization, Vinyl polymer, Living free-radical polymerization, Anionic addition polymerization, Catalytic chain transfer, Polymer chemistry, Materials Chemistry, Living polymerization, Reversible addition−fragmentation chain-transfer polymerization
Published
2013
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7. Chalcogeno[bis(phosphaalkenyl)] Germanium and Tin Compounds

Author

Jean Escudié, Dimitri Matioszek, Ionel Haiduc, Tibor-Gabor Kocsor, Annie Castel, Nathalie Saffon, Petronela M. Petrar, and Gabriela Nemes

Subjects
Stereochemistry, chemistry.chemical_element, Germanium, Ring (chemistry), Sulfur, Inorganic Chemistry, chemistry.chemical_compound, Crystallography, Monomer, chemistry, Physical and Theoretical Chemistry, Tin, Carbene, Single crystal, Derivative (chemistry)
Abstract

The first diphosphaalkenylstannylene stabilized through complexation with a carbene NHC-Sn[C(Cl)═PMes*](2)1 (Mes* = 2,4,6-tri-tert-butylphenyl; NHC = :C{N(iPr)C(Me)}(2)) was isolated and fully characterized including single crystal X-ray diffraction analysis. Its reaction with elemental sulfur rapidly gives the cyclic Sn(2)S(2) (dithiadistannetanne) derivative 3, presumably formed by dimerization of a stannathione intermediate. By contrast, its germanium analogue NHC-Ge[C(Cl)═PMes*](2)7 leads to the corresponding monomeric germathione 4 and germaselenone 5. The germaselenone was more stable than the germathione and could be structurally characterized. An unusual thermal cyclization reaction of the last one occurs with an excess of selenium to give the Ge(2)Se(3) (triselenadigermolane) ring derivative 6.

Published
2012
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9. Halogermanium(II) Complexes Having Phenylamidinate As Supporting Ligands: Syntheses, Characterizations, and Reactivities

Author

Nadia Katir, Dimitri Matioszek, Annie Castel, and Nathalie Saffon

Subjects
Denticity, Chemistry, Ligand, Organic Chemistry, Inorganic chemistry, chemistry.chemical_element, Germanium, Carbon-13 NMR, Cycloaddition, Inorganic Chemistry, Crystallography, Octahedral molecular geometry, Salt metathesis reaction, Chelation, Physical and Theoretical Chemistry
Abstract

Novel germylenes [{Me3SiNC(Ph)NSiMe3}GeX] (X = Cl, Br, I) and [{Me3SiNC(Ph)NSiMe3}2Ge] with the bidentate phenylamidinato ligand have been synthesized in high yields by a salt metathesis reaction between Cl2Ge·dioxane or I2Ge and the lithium salt of the ligand. They were characterized by 1H and 13C NMR and mass spectrometry and single-crystal X-ray structure analyses, which confirmed N-chelation and a three-coordinate germanium center. The cycloaddition reactions with o-quinone led to cycloadducts, whose structures were determined by X-ray analyses. The chelation of the ligand to the metal center was conserved, affording penta- and hexacoordinated germanium(IV) atoms. Complexation reactions with [codW(CO)4] and [nbdMo(CO)4] resulted in trinuclear bis(germanium(II)) transition-metal complexes in “trans” octahedral geometry.

Published
2010
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10. Differential Many-Body Cooperativity in Electronic Spectra of Oligonuclear Transition-Metal Complexes

Author

Dimitri Matioszek, Christopher E. Anson, Frank Breher, Wim Klopper, Jiří Chmela, and Michael E. Harding

Subjects
010405 organic chemistry, Triphenylene, Cooperativity, 010402 general chemistry, medicine.disease_cause, 01 natural sciences, Atomic and Molecular Physics, and Optics, Spectral line, 0104 chemical sciences, Ion, chemistry.chemical_compound, Crystallography, Nuclear magnetic resonance, Transition metal, chemistry, Yield (chemistry), medicine, Physical and Theoretical Chemistry, Carbene, Ultraviolet
Abstract

In computational chemistry, non-additive and cooperative effects can be defined in terms of a (differential) many-body expansion of the energy or any other physical property of the molecular system of interest. One-body terms describe energies or properties of the subsystems, two-body terms describe non-additive but pairwise contributions and three-body as well as higher-order terms can be interpreted as a measure for cooperativity. In the present article, this concept is applied to the analysis of ultraviolet/visible (UV/Vis) spectra of homotrinuclear transition-metal complexes by means of a many-body expansion of the change in the spectrum induced by replacing each of the three transition-metal ions by another transition-metal ion to yield a different homotrinuclear transition-metal complex. Computed spectra for the triangulo-complexes [M3 {Si(mt(Me) )3}2] (M=Pd/Pt, mt(Me) =methimazole) and tritopic triphenylene-based N-heterocyclic carbene Rh/Ir complexes illustrate the concept, showing large and small differential three-body cooperativity, respectively.

Published
2015

11. Selective and Quantitative Oxidation of Xanthate End-Groups of RAFT Poly( n -butyl acrylate) Latexes by Ozonolysis

Author

Jérôme Vinas, Dimitri Matioszek, Mathias Destarac, Pierre-Emmanuel Dufils, Solvay, Laboratoire Chimie Provence (LCP), Université de Provence - Aix-Marseille 1-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Hétérochimie Fondamentale et Appliquée (LHFA), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Magnetic Resonance Spectroscopy, Polymers and Plastics, Free Radicals, Latex, Polymers, Emulsion polymerization, 010402 general chemistry, 01 natural sciences, Living free-radical polymerization, chemistry.chemical_compound, Ozone, Polymer chemistry, Materials Chemistry, Organic chemistry, [CHIM]Chemical Sciences, Reversible addition−fragmentation chain-transfer polymerization, Particle Size, ComputingMilieux_MISCELLANEOUS, Acrylate, Ozonolysis, 010405 organic chemistry, Chemistry, Organic Chemistry, Chain transfer, Raft, 0104 chemical sciences, Acrylates, Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization, Xanthate, Oxidation-Reduction
Abstract

Although various successful strategies have been reported in the past for the postpolymerization modification of the reversible addition-fragmentation chain transfer (RAFT) terminal group in homogeneous media, no solution is proposed for the tedious case of aqueous polymer dispersions where most of the thiocarbonylthio terminal group is buried into the core of the polymer particle. In this work, ozone is proposed to tackle this important academic and industrial challenge. After preliminary model ozonolysis reactions performed on a xanthate RAFT agent and a derived low molar mass poly(n-butyl acrylate) (PBA) in dichloromethane solution, it is shown that the hydrophobic nature and strong oxidant properties of ozone are responsible for its efficient diffusion in aqueous PBA latex particles obtained by RAFT and selective and complete transformation of the xanthate terminal group into a thiocarbonate end-group. In addition to the beneficial total discoloration of the final product, this chemical treatment does not generate any volatile organic compound and leaves the colloidal stability of the polymer particles unaffected, provided that a PBA latex with a sufficiently high Mn of 5000 g mol(-1) is selected.

Published
2015
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12. From rational design of organometallic precursors to optimized synthesis of core/shell Ge/GeO2 nanoparticles

Author

Heinz Gornitzka, A. Cornejo, Dimitri Matioszek, Hervé Martinez, M. Le Troedec, Wilfried-Solo Ojo, M. El Ezzi, Céline Nayral, Annie Castel, N. Katir, Fabien Delpech, Laboratoire Hétérochimie Fondamentale et Appliquée (LHFA), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées, Laboratoire de physique et chimie des nano-objets (LPCNO), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), POCTEFA Interreg project (MET-NANO EFA17/08), ANR-08-BLAN-0105,DeSiGeTin,Design de précurseurs organométalliques pour la synthèse contrôlée de nano-objets d'éléments du groupe 14(2008), Institut de Chimie de Toulouse (ICT), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), and Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Trimethylsilyl, Thermal decomposition, chemistry.chemical_element, Nanoparticle, Germanium, [CHIM.MATE]Chemical Sciences/Material chemistry, Ring strain, Inorganic Chemistry, chemistry.chemical_compound, chemistry, Reagent, Organic chemistry, Physical chemistry, [CHIM]Chemical Sciences, Reactivity (chemistry), Single crystal
Abstract

International audience; The synthesis of germanium nanoparticles has been carried out, thanks to the design of novel aminoiminate germanium(II) precursors: (ATI)GeZ (with Z = OMe, NPh2, and ATI = N,N′-diisopropyl-aminotroponiminate) and (Am)2Ge (Am = N,N′-bis(trimethylsilyl)phenyl amidinate). These complexes were fully characterized by spectroscopic techniques as well as single crystal X-ray diffraction. The thermolysis of both complexes yielded NPs which display similar features that are a Ge/GeO2 core/shell structure with a mean diameter close to 5 nm with a narrow size distribution (300 °C) classically reported in the literature for the preparation of germanium-based NPs were necessary for thermolysis of the complexes (ATI)GeZ, the use of amidinate-based precursors allows the preparation at an unprecedented low temperature (160 °C) for the thermolytic route. As suggested by a mechanistic study, the lower reactivity of (ATI)GeZ (for which the concomitant use of high temperature and acidic reagent is required) was explained in terms of lower ring strain compared to the case of (Am)2Ge.

Published
2015
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13. Synthesis and structure of some heterobimetallic complexes having a polyalkyl-s-indacenyl spacer

Author

Ivonne Chávez, Juan M. Manriquez, Dimitri Matioszek, Annie Castel, Pierre Rivière, Iván Martínez, Desmond Mac-Leod Carey, Nathalie Saffon, Cesar Morales-Verdejo, and Elies Molins

Subjects
Inorganic Chemistry, Nickel, Crystallography, chemistry.chemical_compound, chemistry, Stereochemistry, Materials Chemistry, Moiety, chemistry.chemical_element, Lithium, Manganese, Physical and Theoretical Chemistry, Derivative (chemistry)
Abstract

Three heterobimetallic complexes LmM(s-Ic′)M′Ln (M = Fe,Ru or Mn; M′ = Ni) having the same Cp∗ nickel moiety and based on a polyalkyl-s-indacenyl spacer (s-Ic′ = 2,6-diethyl-4,8-dimethyl-s-indacenyl) were synthesized by reacting Cp∗Ni(acac) with the lithium derivative of the parent monometalated complex. All three compounds were fully characterized and shown to adopt a trans geometry by X-ray crystallography.

Published
2013

14. Bis(amidinato)germylenerhodium complexes: synthesis, structure, and density functional theory calculations

Author

Jean-Marc Sotiropoulos, Dimitri Matioszek, Annie Castel, Karinne Miqueu, Jean Escudié, Nathalie Saffon, Structure Fédérative Toulousaine en Chimie Moléculaire (SFTCM), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), Institut Pluridisciplinaire de Recherche sur l'Environnement et les Matériaux (IPREM), Université de Pau et des Pays de l'Adour (UPPA)-Centre National de la Recherche Scientifique (CNRS), Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Pau et des Pays de l'Adour (UPPA), Laboratoire Hétérochimie Fondamentale et Appliquée (LHFA), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), and Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)

Subjects
Steric effects, chemistry.chemical_classification, 010405 organic chemistry, Ligand, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Oxide, chemistry.chemical_element, Germanium, Nuclear magnetic resonance spectroscopy, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, Photochemistry, 01 natural sciences, 0104 chemical sciences, Divalent, Rhodium, Inorganic Chemistry, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry.chemical_compound, Crystallography, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Density functional theory, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Physical and Theoretical Chemistry
Abstract

cited By 23; International audience; The first monogermylenerhodium complexes stabilized by bulky amidinato ligands on the divalent germanium center have been synthesized and characterized by NMR spectroscopy and X-ray crystallography. Their stability strongly depends on the steric hindrance of the amidinato ligand. With trimethysilyl groups on the nitrogen atoms of the amidinato ligand, only the germylene oxide rhodium complex could be obtained; by contrast, with t-Bu groups, the germylenerhodium complex was isolated. In both cases, the formation of amidinatorhodium complexes was observed. The donating ability of the germylene ligand has been assessed from the CO stretching frequency of the corresponding dicarbonylrhodium complex and was confirmed by density functional theory calculations. © 2012 American Chemical Society.

Published
2012
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15. Phosphaalkenyl germylenes and their gold, tungsten and molybdenum complexes

Author

Dimitri Matioszek, Gabriela Nemes, Annie Castel, Nathalie Saffon, Tibor-Gabor Kocsor, and Jean Escudié

Subjects
Denticity, Chemistry, Inorganic chemistry, Metals and Alloys, chemistry.chemical_element, Germanium, General Chemistry, Tungsten, Catalysis, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Crystallography, Molybdenum, Phosphorus atom, Atom, Materials Chemistry, Ceramics and Composites
Abstract

The new bis(phosphaalkenyl) germanium(II) compound (NHC)Ge(CCl=PMes*)(2) reacts with L(2)M(CO)(4) (M = Mo, W) to give bidentate complexes with an unexpected coordinating behaviour involving the Ge(II) centre and one phosphorus atom, and with AuI or Me(2)SAuCl to afford the monodentate complexes coordinated at the germanium(II) atom.

Published
2012

16. A new method to radical anions derived from s-indacene organobimetallic complexes, their esr characterization

Author

Annie Castel, D. Mac-Leod Carey, Alvaro Muñoz-Castro, Juan M. Manriquez, Dimitri Matioszek, Monique Rivière-Baudet, C. Adams, Pierre Rivière, Ramiro Arratia-Pérez, Iván Martínez, Juan F. Araneda, Raluca Septelean, Ivonne Chávez, and Cesar Morales-Verdejo

Subjects
Olefin fiber, Chemistry, Inorganic chemistry, Catalysis, Inorganic Chemistry, Metal, Crystallography, Hyperfine coupling, visual_art, Electrophile, Materials Chemistry, visual_art.visual_art_medium, Physical and Theoretical Chemistry, Spectroscopy
Abstract

The following organobimetallic radical anions derived from 2,6-diethyl-4,8-dimethyl- s -indacene ( s -Ic′): [CODRh( s -Ic′)RhCOD] − ( IIa ), [Cp ∗ Ru( s -Ic′)RuCp ∗ ] − ( IIb ), [Cp ∗ Ru( s -Ic′)RhCOD] − ( IIc ), [Cp ∗ Ru( s -Ic′)NiCp ∗ ] − ( IId ) [(CO) 3 Mn( s -Ic′)NiCp ∗ ] − ( IIe ) and [Cp ∗ Fe( s -Ic′)NiCp ∗ ] − ( IIf ) (COD = 1,5-cyclooctadiene; Cp ∗ = pentamethylcyclopentadienyl) were prepared by reduction of the parent complexes using a monoelectronic transfer from an electron rich olefin. The radical anions were fully characterized by ESR spectroscopy which usually gave a well resolved hyperfine coupling structure, indicating that the spin distribution in the symmetrical radical anions ( IIa , IIb ) affects mainly the organic spacer whereas in the unsymmetrical ones ( IIc – f ) it is displaced towards the most electronegative metal center and its ligands. This effect is most pronounced in IId , IIe and IIf . The calculated g tensor values of the radical anions are in good agreement with the experimental values. In heterobimetallic radical anions, the dissymmetric spin distribution shows that the two metals present different electrophile properties leading to potentially different catalytic activities.

Published
2012

17. Back Cover: Differential Many-Body Cooperativity in Electronic Spectra of Oligonuclear Transition-Metal Complexes (ChemPhysChem 1/2016)

Author

Wim Klopper, Jiří Chmela, Michael E. Harding, Dimitri Matioszek, Frank Breher, and Christopher E. Anson

Subjects
010304 chemical physics, Chemistry, Cooperativity, 010402 general chemistry, 01 natural sciences, Atomic and Molecular Physics, and Optics, Many body, Spectral line, 0104 chemical sciences, Transition metal, Chemical physics, Computational chemistry, Non additivity, 0103 physical sciences, Cover (algebra), Physical and Theoretical Chemistry, Differential (mathematics)
Published
2016
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18. Novel Stable Silyl, Germyl, and Stannyl Germanium(II) Compounds Containing an Amidinato Ligand.

Author

Dimitri Matioszek, Nadia Katir, Sonia Ladeira, and Annie Castel

Subjects
*GERMANIUM compounds, *LIGANDS (Chemistry), *CHEMICAL reactions, *CHELATES, *NUCLEAR magnetic resonance spectroscopy, *X-ray diffraction, *MAGNESIUM compounds, *CHEMICAL reagents, *MOLECULAR structure
Abstract

Reactions of the N,N′-chelated chlorogermanium(II) compound [Me3SiNC(Ph)NSiMe3]GeCl with the magnesium reagents Mg[E(SiMe3)3]2(E = Si, Ge, Sn) gave the new metallyl germylenes [Me3SiNC(Ph)NSiMe3]GeE(SiMe3)3, representing the first isolated silyl- and stannylgermylenes. These compounds have been fully characterized by multinuclear NMR spectroscopy and their structures determined by X-ray diffraction analysis. [ABSTRACT FROM AUTHOR]

Published
2011
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