| Titre : |
Iron, manganese and rhenium-catalyzed (de)-hydrogenation and hydroelementation reations |
| Type de document : |
texte imprimé |
| Auteurs : |
Yun Wei, Auteur ; Christophe Darcel, Directeur de thèse ; Sortais, Jean-Baptiste, Directeur de thèse |
| Langues : |
Anglais (eng) |
| Tags : |
CATALYSE FER RHÉNIUM MANGANÈSE |
| Résumé : |
"This research work is aimed at developing advanced eco-friendly methodologies in the area of iron, manganese and rhenium-catalyzed (de)hydrogenation and hydroelementation reactions. Initially, we reported the first examples of highly selective catalytic direct C-H borylation of styrene derivatives and terminal alkynes with pinacolborane using Fe(PMe3)4 and Fe(OTf)2/DABCO as catalyst systems, respectively. Afterwards, N-heterocyclic carbene (NHC) based iron complexes Fe(CO)4(IMes) and [CpFe(CO)2(IMes)][I] were efficiently employed in the catalytic reductive amination reactions with hydrosilanes to access a large variety of cyclic amines (pyrrolidines, piperidines and azepanes). Interestingly, with the commercially available Mn2(CO)10 or Re2(CO)10 as catalyst and Et3SiH as an inexpensive hydrosilane source, carboxylic esters, acids and amides can be chemospecifically reduced to the corresponding acetals, alcohols and amines. Besides hydrosilylation, we also explored the application of a series of well-defined manganese pre-catalysts featuring readily available bidendate pyridinyl-phosphine and 2-picolylamine ligands in hydrogenation reactions of aldehydes, ketones and aldimines. In line with our interest in developing group 7 metals based catalysts, we have also demonstrated that a series of amino-bisphosphino ligands coordinated rhenium catalysts can efficiently promote the hydrogenation of carbonyl derivatives, the mono N-methylation of anilines with methanol and the dehydrogenative synthesis of substituted quinolines. Lastly we also developed the Mn-catalysed ligand- and additive-free aerobic oxidation of amines to prepare aldimines, N-heteroaromatics and benzoimidazole derivatives."
|
| Document : |
Thèse de Doctorat |
| Etablissement_delivrance : |
Université de Rennes 1 |
| Date_soutenance : |
10/09/2019 |
| Ecole_doctorale : |
École doctorale Matière, Molécules Matériaux et Géosciences (Le Mans) Accéder à IdRef, la base des identifiants et des référentiels utilisés pour l’en |
| Domaine : |
Chimie moléculaire et macromoléculaire |
| En ligne : |
https://www.theses.fr/2019REN1S105 |
Iron, manganese and rhenium-catalyzed (de)-hydrogenation and hydroelementation reations [texte imprimé] / Yun Wei, Auteur ; Christophe Darcel, Directeur de thèse ; Sortais, Jean-Baptiste, Directeur de thèse . - [s.d.]. Langues : Anglais ( eng)
| Tags : |
CATALYSE FER RHÉNIUM MANGANÈSE |
| Résumé : |
"This research work is aimed at developing advanced eco-friendly methodologies in the area of iron, manganese and rhenium-catalyzed (de)hydrogenation and hydroelementation reactions. Initially, we reported the first examples of highly selective catalytic direct C-H borylation of styrene derivatives and terminal alkynes with pinacolborane using Fe(PMe3)4 and Fe(OTf)2/DABCO as catalyst systems, respectively. Afterwards, N-heterocyclic carbene (NHC) based iron complexes Fe(CO)4(IMes) and [CpFe(CO)2(IMes)][I] were efficiently employed in the catalytic reductive amination reactions with hydrosilanes to access a large variety of cyclic amines (pyrrolidines, piperidines and azepanes). Interestingly, with the commercially available Mn2(CO)10 or Re2(CO)10 as catalyst and Et3SiH as an inexpensive hydrosilane source, carboxylic esters, acids and amides can be chemospecifically reduced to the corresponding acetals, alcohols and amines. Besides hydrosilylation, we also explored the application of a series of well-defined manganese pre-catalysts featuring readily available bidendate pyridinyl-phosphine and 2-picolylamine ligands in hydrogenation reactions of aldehydes, ketones and aldimines. In line with our interest in developing group 7 metals based catalysts, we have also demonstrated that a series of amino-bisphosphino ligands coordinated rhenium catalysts can efficiently promote the hydrogenation of carbonyl derivatives, the mono N-methylation of anilines with methanol and the dehydrogenative synthesis of substituted quinolines. Lastly we also developed the Mn-catalysed ligand- and additive-free aerobic oxidation of amines to prepare aldimines, N-heteroaromatics and benzoimidazole derivatives."
|
| Document : |
Thèse de Doctorat |
| Etablissement_delivrance : |
Université de Rennes 1 |
| Date_soutenance : |
10/09/2019 |
| Ecole_doctorale : |
École doctorale Matière, Molécules Matériaux et Géosciences (Le Mans) Accéder à IdRef, la base des identifiants et des référentiels utilisés pour l’en |
| Domaine : |
Chimie moléculaire et macromoléculaire |
| En ligne : |
https://www.theses.fr/2019REN1S105 |
|  |
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