The development of efficient synthetic methodologies for the construction of complex molecules has been a prominent area of research in recent decades. Ligand-directed transition metal-catalyzed C–H functionalization reactions have made significant strides in this regard, initially relying on noble transition metals. However, the emergence of more cost-effective first-row metals, such as cobalt, has provided an attractive, more sustainable alternative. Notably, Cp*Co(III) complexes have demonstrated their remarkable potential especially involving electrophiles as coupling partners, while methodologies involving nucleophiles remain scarce.
This thesis advances the understanding of the participation of Cp*Co-based complexes in relevant nucleophilic couplings to form C–C and C–X bond-forming reactions. Specifically, we have explored: i) the mechanistic intricacies underlying C–SCF3 bond formation; ii) the mechanism of action of F+ oxidants leading to C–I bond formation; iii) nucleophilic coupling with a diverse family of well-established and isolable Cp*Co(III) complexes. By employing a combination of experimental and computational approaches, this thesis provides fundamental insights into the behavior of these complexes, including the unprecedented involvement of high-valent cobalt species in the targeted C–X reductive elimination events. The acquired knowledge not only enhances our understanding of the studied processes but also contributes to the broader field of knowledge-driven research in Chemistry.
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