Functionalisations at activated and non-activated C-H bonds

Site-selective, late-stage functionalisation of non-activated C-H bonds represents a challenge for organic chemists because these bonds are among the strongest in nature. Particularly, with regards to chlorination of non-activated C-H bonds, a method that allows for their benign, facile ad site-sele...

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Main Author: Ambrosio, Teresina
Format: Thesis (University of Nottingham only)
Language:English
Published: 2021
Subjects:
Online Access:https://eprints.nottingham.ac.uk/64278/
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author Ambrosio, Teresina
author_facet Ambrosio, Teresina
author_sort Ambrosio, Teresina
building Nottingham Research Data Repository
collection Online Access
description Site-selective, late-stage functionalisation of non-activated C-H bonds represents a challenge for organic chemists because these bonds are among the strongest in nature. Particularly, with regards to chlorination of non-activated C-H bonds, a method that allows for their benign, facile ad site-selective chlorination has yet to be developed. With this doctoral thesis, we aimed at developing a novel and more sustainable procedure to perform halogenation of non-activated C-H bonds as well as giving our contribution to expanding the knowledge and understanding of the mechanism and catalytic cycle of the reaction. We also explored the use of palladium catalysts for the alpha-arylation of ortho-chloro toluenes with diketones. Despite diketones carry activated C-H bonds, a facile and sustainable functionalization of those bonds hasn't been found yet and existing protocols rely on the use of stoichiometric amounts of lead complexes. The aim of this project was to substitute the toxic metal lead with palladium used in catalytic amounts. We also gave our contribution to gaining evidence and exploring the mechanism and catalytic cycle of the cross-coupling reaction.
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spelling nottingham-642782025-02-28T15:09:42Z https://eprints.nottingham.ac.uk/64278/ Functionalisations at activated and non-activated C-H bonds Ambrosio, Teresina Site-selective, late-stage functionalisation of non-activated C-H bonds represents a challenge for organic chemists because these bonds are among the strongest in nature. Particularly, with regards to chlorination of non-activated C-H bonds, a method that allows for their benign, facile ad site-selective chlorination has yet to be developed. With this doctoral thesis, we aimed at developing a novel and more sustainable procedure to perform halogenation of non-activated C-H bonds as well as giving our contribution to expanding the knowledge and understanding of the mechanism and catalytic cycle of the reaction. We also explored the use of palladium catalysts for the alpha-arylation of ortho-chloro toluenes with diketones. Despite diketones carry activated C-H bonds, a facile and sustainable functionalization of those bonds hasn't been found yet and existing protocols rely on the use of stoichiometric amounts of lead complexes. The aim of this project was to substitute the toxic metal lead with palladium used in catalytic amounts. We also gave our contribution to gaining evidence and exploring the mechanism and catalytic cycle of the cross-coupling reaction. 2021-03-15 Thesis (University of Nottingham only) NonPeerReviewed application/pdf en arr https://eprints.nottingham.ac.uk/64278/1/Doctoral%20Thesis%20Teresa%20Ambrosio%20Revisions.pdf Ambrosio, Teresina (2021) Functionalisations at activated and non-activated C-H bonds. PhD thesis, University of Nottingham. Catalysis Iron-catalysis Palladium Cross-coupling C-H activation Late-stage functionalisation
spellingShingle Catalysis
Iron-catalysis
Palladium
Cross-coupling
C-H activation
Late-stage functionalisation
Ambrosio, Teresina
Functionalisations at activated and non-activated C-H bonds
title Functionalisations at activated and non-activated C-H bonds
title_full Functionalisations at activated and non-activated C-H bonds
title_fullStr Functionalisations at activated and non-activated C-H bonds
title_full_unstemmed Functionalisations at activated and non-activated C-H bonds
title_short Functionalisations at activated and non-activated C-H bonds
title_sort functionalisations at activated and non-activated c-h bonds
topic Catalysis
Iron-catalysis
Palladium
Cross-coupling
C-H activation
Late-stage functionalisation
url https://eprints.nottingham.ac.uk/64278/