Bioinspired metal-based oxidants: selectivity in catalytic hydroxylation of aliphatic C-H bonds and insight into the reactivity of oxoiron species

Selective oxidation of C-H bonds is an important reaction, as it can disclose novel synthetic strategies to get functionalized products through efficient paths. Nonetheless, due to the inert character of C-H bonds, the use of powerful oxidants is needed. In addition, achieving selectivity in such re...

ver descrição completa

Detalhes bibliográficos
Autor: Dantignana, Valeria
Tipo de documento: tese
Estado:Versão publicada
Data de publicação:2020
País:España
Recursos:CBUC, CESCA
Repositório:TDR. Tesis Doctorales en Red
OAI Identifier:oai:www.tdx.cat:10803/671447
Acesso em linha:http://hdl.handle.net/10803/671447
Access Level:Acceso aberto
Palavra-chave:Enllaç C-H
Enlace C-H
C-H bond
Oxidació selectiva
Oxidación selectiva
Selective oxidation
Complexos bioinspirats
Complejos bioinspirados
Bioinspired complexes
Oxoiron species
Hidroxilació
Hidroxilación
Hydroxylation
Catalitzadors
Catalizadores
Catalysts
546
Descrição
Resumo:Selective oxidation of C-H bonds is an important reaction, as it can disclose novel synthetic strategies to get functionalized products through efficient paths. Nonetheless, due to the inert character of C-H bonds, the use of powerful oxidants is needed. In addition, achieving selectivity in such reactions is difficult. In that regard, nature can be taken as inspiration, since oxidation reactions are efficiently and selectively performed by iron-dependent oxygenases. Thus, in order to develop novel methodologies, bioinspired complexes have been explored as oxidation catalysts. In this line, in this thesis hydroxylation of C-H bonds catalyzed by bioinspired iron and manganese complexes has been first investigated. Subsequently, being mechanistic understanding important for the design of efficient catalysts, high-valent oxoiron compounds have been investigated to deeper comprehend how to modulate their oxidative ability