The study of solid hydrogen storage and o-dihydrogen complexes / Sameh Dhaher  

Public ISBD Titre : The study of solid hydrogen storage and o-dihydrogen complexes Type de document : texte imprimé Auteurs : Sameh Dhaher, Auteur ; Grellier, Mary, Directeur de thèse ; Sylviane Sabo-Etienne, Directeur de thèse Langues : Anglais (eng) Tags : HYDROGEN STORAGE  HYDROGENATION  DEHYDROGENATION  SYNTHESIS  CHARACTERIZATION  APPLICATION  DOPING OF MATERIALS  ENERGY VECTOR  SIGMA DIHYDROGEN COMPLEXES Résumé : "Adopting clean and emission- free energy cycle using hydrogen as an energy carrier could be the solution in order to curb the ill effects of energy crisis and global warming on the planet. Thus, the lack of efficient hydrogen storage devices has stimulated the search of new systems. In this manuscript, the dehydrogenation of the bis-dihydrogen ruthenium complex without additives at the ruthenium center has been reported in Chapter II. The unusual and rare dimeric complex bearing two phosphido bridges was accessed from thermolysis of the bis(dihydrogen) complex RuH2(H2)2(PCyp3)2. The complex was characterized by NMR, IR, UV-Visible, X-ray, neutron structure and DFT calculations. Surprisingly, the complex shows a reversible up take and release of H2 at room temperature in solution as well as in the solid state. This is one major criteria for designing a solid hydrogen storage material. The activation of the H-H bond has been subjected to a detailed study in Chapter III. Several novel ruthenium complexes bearing fac-coordinating ligands, 1,3,5-triaminocyclohexane (tach) and 1,4,7-triazacyclononane (tacn) and different anions have been prepared. DFT investigation has been deployed throughout these studies for a fine-level examination of H-H bond activation. An attractive goal in the context of hydrogen storage is to combine magnesium hydride, MgH2 or MOFs to organometallic complexes. This is the purpose of the fourth chapter. Doping magnesium hydride with ruthenium or nickel precursors shows promising results." Document : Thèse de Doctorat Etablissement_delivrance : Université deToulouse 3 Date_soutenance : 13/12/2019 Ecole_doctorale : Sciences de la Matière (SdM) (Toulouse) Domaine : Chimie Organométallique et de Coordination En ligne : http://thesesups.ups-tlse.fr/4555/ The study of solid hydrogen storage and o-dihydrogen complexes [texte imprimé] / Sameh Dhaher, Auteur ; Grellier, Mary, Directeur de thèse ; Sylviane Sabo-Etienne, Directeur de thèse . - [s.d.]. Langues : Anglais (eng) Tags : HYDROGEN STORAGE  HYDROGENATION  DEHYDROGENATION  SYNTHESIS  CHARACTERIZATION  APPLICATION  DOPING OF MATERIALS  ENERGY VECTOR  SIGMA DIHYDROGEN COMPLEXES Résumé : "Adopting clean and emission- free energy cycle using hydrogen as an energy carrier could be the solution in order to curb the ill effects of energy crisis and global warming on the planet. Thus, the lack of efficient hydrogen storage devices has stimulated the search of new systems. In this manuscript, the dehydrogenation of the bis-dihydrogen ruthenium complex without additives at the ruthenium center has been reported in Chapter II. The unusual and rare dimeric complex bearing two phosphido bridges was accessed from thermolysis of the bis(dihydrogen) complex RuH2(H2)2(PCyp3)2. The complex was characterized by NMR, IR, UV-Visible, X-ray, neutron structure and DFT calculations. Surprisingly, the complex shows a reversible up take and release of H2 at room temperature in solution as well as in the solid state. This is one major criteria for designing a solid hydrogen storage material. The activation of the H-H bond has been subjected to a detailed study in Chapter III. Several novel ruthenium complexes bearing fac-coordinating ligands, 1,3,5-triaminocyclohexane (tach) and 1,4,7-triazacyclononane (tacn) and different anions have been prepared. DFT investigation has been deployed throughout these studies for a fine-level examination of H-H bond activation. An attractive goal in the context of hydrogen storage is to combine magnesium hydride, MgH2 or MOFs to organometallic complexes. This is the purpose of the fourth chapter. Doping magnesium hydride with ruthenium or nickel precursors shows promising results." Document : Thèse de Doctorat Etablissement_delivrance : Université deToulouse 3 Date_soutenance : 13/12/2019 Ecole_doctorale : Sciences de la Matière (SdM) (Toulouse) Domaine : Chimie Organométallique et de Coordination En ligne : http://thesesups.ups-tlse.fr/4555/

COORDINATION DES LIAISONS SI-H ET GE-H AU CENTRE METALLIQUE RUTHENIUM : STRUCTURE, REACTIVITE ET APPLICATIONS CATALYTIQUES / Aswin Chandran  

Public ISBD Titre : COORDINATION DES LIAISONS SI-H ET GE-H AU CENTRE METALLIQUE RUTHENIUM : STRUCTURE, REACTIVITE ET APPLICATIONS CATALYTIQUES Type de document : texte imprimé Auteurs : Aswin Chandran, Auteur ; Grellier, Mary, Directeur de thèse ; Jason M Lynam, Directeur de thèse Langues : Français (fre) Document : thèse de Doctorat Etablissement_delivrance : Université Toulouse 3 en cotutelle avec UNIVERSITY OF YORK Date_soutenance : 13/12/2023 Ecole_doctorale : Sciences de la matière (SdM) ( Toulouse) Domaine : Aspects moleculaires et cellulaires de la biologie En ligne : https://theses.fr/s295624 COORDINATION DES LIAISONS SI-H ET GE-H AU CENTRE METALLIQUE RUTHENIUM : STRUCTURE, REACTIVITE ET APPLICATIONS CATALYTIQUES [texte imprimé] / Aswin Chandran, Auteur ; Grellier, Mary, Directeur de thèse ; Jason M Lynam, Directeur de thèse . - [s.d.]. Langues : Français (fre) Document : thèse de Doctorat Etablissement_delivrance : Université Toulouse 3 en cotutelle avec UNIVERSITY OF YORK Date_soutenance : 13/12/2023 Ecole_doctorale : Sciences de la matière (SdM) ( Toulouse) Domaine : Aspects moleculaires et cellulaires de la biologie En ligne : https://theses.fr/s295624

Ruthenium silane and germane complexes : synthesis, electrochemical and catalytic studies / Smart, Katharine  

Public ISBD Titre : Ruthenium silane and germane complexes : synthesis, electrochemical and catalytic studies Type de document : texte imprimé Auteurs : Smart, Katharine, Auteur ; Grellier, Mary, Directeur de thèse ; Sylviane Sabo-Etienne, Directeur de thèse Année de publication : 2013 Langues : Anglais (eng) Tags : RUTHENIUM  SILANE  GERMANE  SILAZANE  DEUTERATION  ELECTROCHEMISTRY  NEUTRON DIFFRACTION  CATALYSIS Résumé : "The activation of E - H bonds (E = Si, Ge, H) by ruthenium complexes is subjected to detailed study. The first chapter describes the preparation of novel N-heterocycle-silane compounds, their employment as ligands to ruthenium and the properties of the resulting complexes. Several classes of ruthenium-N-heterocycle-silane species were isolated including a series bearing the motif RuSi3H comprising heptacoordinated moieties with three N-heterocycle-silane ligands and a hydride. As explored in chapter 2, two degenerate systems are encountered for RuSi3H; with the hydride located equidistant from the three silicon atoms or with the hydride closer to two silicon atoms than the third. Protonation of RuSi3H led to RuSi3H2+ bearing hydride, silyl and ??-(H??Si) ligands. In chapter 3, the wide range in oxidation potentials of the RuSi3H complexes is correlated to the electronic properties of the ligands. Chemical and electrochemical oxidation of a RuSi3H species gave rise to RuSi3H2+ and possible routes accounting for the transformation are examined. The focus shifts in chapter 4 to the activation of Ge - H bonds. Complexes of the type Ru(diphosphine)2(GeH3)(H) were accessed by the photochemical reaction of GeH4 with Ru(diphosphine)2H2. Study of germane systems continued with the reaction of Ph2GeH2 and the polyhydride complex Ru(H)2(?2-H2)2(PCy3)2 giving rise to a unique dihydrogen-germylene-ruthenium complex, Ru(H)2(=GePh2)(?2-H2)(PCy3)2. It was also possible to prepare (Ph2HGe)2O from the coupling of Ph2GeH2 and water in the presence of a catalytic amount of ruthenium. The complex Ru(H)4{(Ph2Ge)2O}(PCy3)2 was also isolated and identified as a key intermediate in the generation of (Ph2HGe)2O. The final chapter describes the selective catalytic deuteration of hydridosilanes with deuterium gas. It was possible to achieve the successful deuteration of a range of silanes with very low catalyst loading." Document : Thèse de Doctorat Etablissement_delivrance : Université de Toulouse 3 Date_soutenance : 11/10/2013 Ecole_doctorale : Sciences de la matière (SdM) Domaine : Chimie Organométallique et de Coordination En ligne : http://thesesups.ups-tlse.fr/2186/ Ruthenium silane and germane complexes : synthesis, electrochemical and catalytic studies [texte imprimé] / Smart, Katharine, Auteur ; Grellier, Mary, Directeur de thèse ; Sylviane Sabo-Etienne, Directeur de thèse . - 2013. Langues : Anglais (eng) Tags : RUTHENIUM  SILANE  GERMANE  SILAZANE  DEUTERATION  ELECTROCHEMISTRY  NEUTRON DIFFRACTION  CATALYSIS Résumé : "The activation of E - H bonds (E = Si, Ge, H) by ruthenium complexes is subjected to detailed study. The first chapter describes the preparation of novel N-heterocycle-silane compounds, their employment as ligands to ruthenium and the properties of the resulting complexes. Several classes of ruthenium-N-heterocycle-silane species were isolated including a series bearing the motif RuSi3H comprising heptacoordinated moieties with three N-heterocycle-silane ligands and a hydride. As explored in chapter 2, two degenerate systems are encountered for RuSi3H; with the hydride located equidistant from the three silicon atoms or with the hydride closer to two silicon atoms than the third. Protonation of RuSi3H led to RuSi3H2+ bearing hydride, silyl and ??-(H??Si) ligands. In chapter 3, the wide range in oxidation potentials of the RuSi3H complexes is correlated to the electronic properties of the ligands. Chemical and electrochemical oxidation of a RuSi3H species gave rise to RuSi3H2+ and possible routes accounting for the transformation are examined. The focus shifts in chapter 4 to the activation of Ge - H bonds. Complexes of the type Ru(diphosphine)2(GeH3)(H) were accessed by the photochemical reaction of GeH4 with Ru(diphosphine)2H2. Study of germane systems continued with the reaction of Ph2GeH2 and the polyhydride complex Ru(H)2(?2-H2)2(PCy3)2 giving rise to a unique dihydrogen-germylene-ruthenium complex, Ru(H)2(=GePh2)(?2-H2)(PCy3)2. It was also possible to prepare (Ph2HGe)2O from the coupling of Ph2GeH2 and water in the presence of a catalytic amount of ruthenium. The complex Ru(H)4{(Ph2Ge)2O}(PCy3)2 was also isolated and identified as a key intermediate in the generation of (Ph2HGe)2O. The final chapter describes the selective catalytic deuteration of hydridosilanes with deuterium gas. It was possible to achieve the successful deuteration of a range of silanes with very low catalyst loading." Document : Thèse de Doctorat Etablissement_delivrance : Université de Toulouse 3 Date_soutenance : 11/10/2013 Ecole_doctorale : Sciences de la matière (SdM) Domaine : Chimie Organométallique et de Coordination En ligne : http://thesesups.ups-tlse.fr/2186/

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