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Date of PhD defence: October 25th, 2024.
Main research findings
Transition metal (TM) catalysts are indispensable in industrial operations and organic synthesis due to their unique properties, such as variable oxidation states, rich coordination chemistry, and ability to enable electron transfer processes. These properties allow them to activate a diverse range of substrates by lowering activation energies, and the catalysts can be fine-tuned to enhance chemo-, regio-, and stereoselectivities for desired products. One of the prominent and requisite uses of TM catalysts is in the conversion of CO2 to higher-value products.
With the advent of climate change, scientists are looking for renewable carbon sources to replace fossil fuels. One promising option is CO2, a non-toxic and highly abundant greenhouse gas. However, the use of CO2 in chemical synthesis is limited due to its kinetic and thermodynamic stability. TM catalysts have the potential to address these challenges, making the study of these catalysts vital for developing effective CO2 activation processes. Nonetheless, their complex electronic structures, ligand coordination dynamics, assorted reaction pathways, broad spectroscopic signals, and environmental sensitivity make it difficult to study them experimentally. Computational chemistry, with its explanatory and predictive power, can help elucidate their intricate behaviors and interactions.
In this thesis, I examined TM-mediated processes using computational chemistry techniques, particularly density functional theory (DFT), to identify transient species like intermediates and transition states, and to understand their nuclear and electronic structures. My research included an analysis of the factors leading to enantioenriched carbamate formation from CO2, catalyzed by an Ir-based complex (Paper I). Another study investigated the CO2-insertion mechanism into diverse Pd-alkyl complexes and its relationship with the experimentally observed reaction kinetics, in close collaboration with an experimental group from Yale University (Paper II).
I also collaborated with Aarhus University to examine diverse mechanistic pathways for a Nicatalyzed aryl-alkyl cross-coupling reaction with CO (originating from CO2) insertion (Paper III). Additionally, I employed state-of-the-art computational techniques, involving ab initio molecular dynamics simulations (AIMD), to precisely predict 19F nuclear magnetic resonance (NMR) chemical shifts in a Ni-fluoride complex (Paper IV).
PhD thesis: https://munin.uit.no/handle/10037/35298
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Supervisors, evaluation committee and leader of defence
Principal supervisor
Professor Kathrin H. Hopmann. Department of Chemistry, UiT The Arctic University of Norway.
Co-supervisors
Research Abril Castro Aguilera. Department of Chemistry, University of Oslo.
Principal Scientist Per-Ola Norrby. AstraZeneca.
Evaluation committee
Professor Vidar Remi Jensen. Department of Chemistry, University of Bergen (1. opponent).
Researcher Dr. Cristina Trujillo. Computational Organic Chemistry Group, University of Manchester, UK (2. opponent).
Researcher Dr. Bin Gao, Department. of Chemistry, UiT The Arctic University of Norway (internal member and leader of the committee).
Leader of defence
Pro-Dean, Professor Cordian Riener. Department of Mathematics and Statistics, UiT The Arctic University of Norway.
Funding
The reported research was performed with funding from the Research Council of Norway (grants no. 300769 and 325231, and Centre of Excellence grant no. 262695), Sigma2 (nn9330k and nn14654k), NordForsk (grant no. 85378), and the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no. 859910.