Sustainable Ruthenium- and Rhodium-Catalyzed C−H Activations with Photochemistry and Electrochemistry

by Agnese Zangarelli
Doctoral thesis
Date of Examination:2024-02-29
Date of issue:2024-03-18
Advisor:Prof. Dr. Lutz Ackermann
Referee:Prof. Dr. Lutz Ackermann
Referee:Prof. Dr. Konrad Koszinowski
Referee:Prof. Dr. Franc Meyer
Referee:Prof. Dr. Dr. Lutz Tietze
Referee:Dr. Holm Frauendorf
Referee:Dr. Daniel Janßen-Müller
Persistent Address: http://dx.doi.org/10.53846/goediss-10400

 

 

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Abstract

English

Cross-coupling chemistry stands out as a fundamental tool in synthetic organic chemistry for forging C‒C and C‒Het bonds. However, the necessity for substrate prefunctionalization imposes significant sustainability challenges on these transformations. In contrast, advancements in transition metal-catalyzed direct functionalization of ubiquitous C‒H bonds present a more sustainable avenue for constructing complex molecular structures. Despite the pivotal contributions of C–H activation, also driven by key principles like atom- and step-economy, this approach has inherent limitations. To overcome these, innovative mechanistic pathways integrating renewable energy sources in electrocatalysis and photocatalysis are pursued to address issues related to hazardous chemical oxidants and harsh reaction conditions. Additionally, with the aim of synthetic utility and applicability in drug discovery and medicinal chemistry, late-stage C–H functionalization can be implemented with the promise for simplifying reaction pathways and diversifying product outputs. These themes constitute the central investigative focus of this thesis.
Keywords: Catalysis; C–H Activation; C–H Functionalization; Sustainability; Photochemistry; Electrochemistry; Late-Stage Functionalization
 
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