Modelling mechanisms of organometallic reactions from surface deposition to heterogeneous catalysis
| dc.contributor.author | Donnecke, Sofia | |
| dc.contributor.supervisor | Paci, Irina | |
| dc.contributor.supervisor | McIndoe, J. Scott | |
| dc.date.accessioned | 2023-08-25T20:49:53Z | |
| dc.date.copyright | 2023 | en_US |
| dc.date.issued | 2023-08-25 | |
| dc.degree.department | Department of Chemistry | |
| dc.degree.level | Doctor of Philosophy Ph.D. | en_US |
| dc.description.abstract | Theoretical and experimental methods are applied to study the elementary steps taking place in the gas phase and on the surface to help guide the rational design of new precursors and catalysts. The body of this work sets out to improve our fundamental understanding of the reactions taking place on various surfaces. A number of reaction pathways are modelled on the surface ranging from benchmarking the energetics of known reactions to modelling new systems and unexplored reaction pathways. Atomic layer deposition (ALD) of cobalt thin films is desirable in the fabrication of complex nanodevices and development of effective precursors requires a mechanistic understanding of the deposition pathways. The first two projects set out to understand the reactivity and deposition pathways of a number of existing and new Co precursors for ALD, and identify promising precursors to improve deposition. In a third project, the catalyzed oxygen reduction reaction (ORR) is studied to both benchmark computational methods and identify electronic trends across different metals and systems. DFT is shown to perform relatively well compared to CCSD(T) on difficult, high spin systems and modest model reduction in molecular catalysts is found to improve cost and convergence, while retaining the calculated chemical trends. A large number of reaction pathways are computed for known and new transition metal systems and the results are reported herein. | en_US |
| dc.description.scholarlevel | Graduate | en_US |
| dc.identifier.uri | http://hdl.handle.net/1828/15287 | |
| dc.language | English | eng |
| dc.language.iso | en | en_US |
| dc.rights | Available to the World Wide Web | en_US |
| dc.subject | chemistry | en_US |
| dc.subject | organometallics | en_US |
| dc.subject | surface | en_US |
| dc.subject | computational | en_US |
| dc.subject | ALD | en_US |
| dc.subject | ESI-MS | en_US |
| dc.subject | deposition | en_US |
| dc.subject | catalysis | en_US |
| dc.title | Modelling mechanisms of organometallic reactions from surface deposition to heterogeneous catalysis | en_US |
| dc.type | Thesis | en_US |