Abstract
This thesis explores the reactivity of cationic gold(I) centres towards a series of small molecules, with particular focus on C2H4, N2O, and H2 coordination. In addition, this thesis presents the preparation of porous metal oxides and their potential as N2O abatement catalysts.Firstly, Chapter 1 gives an introduction to gold chemistry, with particular focus on gold(I)–alkene coordination complexes. Secondly, a brief overview of N2O abatement strategies is provided.
Chapters 2 and 3 describe investigations into complexes supported by an NHC ligand with vari-dentate N-donor side arm previously developed in the Russell group. Chapter 2 presents the synthesis of a gold(I)–ethylene complex supported by this ligand, as well as a copper(I) analogue and NHC supported gold(I) complexes with substituted alkenes. Chapter 3 expands this work by altering the substituents on the NHC N-donor side arm and presenting the synthesis of the corresponding NHC–gold(I)–ethylene complexes. Further work found that the use of alternative substituents on the N-donor side arm enabled oxidative addition of MeI to [NHC–gold(I)]+ fragments.
Chapter 4 explores the reactivity of cationic gold(I) centres towards N2O, H2, and CO2. Based on previous work by Dias et al. which isolated [Au(C2H4)][SbF6], initial attempts focussed on preparing [Au(L)n][X] type complexes, which produced inconclusive results. Use of bipyridyl type ligands and bulky phosphine ligands to stabilise possible coordination complexes did not result in isolable complexes, but spectroscopic data hinted that phosphine supported gold(I) complexes reacted with H2.
Chapter 5 presents the preparation of metal oxides using melamine formaldehyde foam templates via a method developed in the Hall group. The oxides were shown to have porous microstructures, which, in the case of CuO, were dependent on the calcination temperature. The metal oxides were found to show varying activity towards N2O at elevated temperatures, showing potential as N2O abatement catalysts.
| Date of Award | 1 Oct 2024 |
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| Original language | English |
| Awarding Institution |
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| Supervisor | Chris A Russell (Supervisor) & Natalie Fey (Supervisor) |