Merging Electrosynthesis with 3d Transition Metal-Catalyzed C–H Transformations

by Tjark Hannes Meyer
Doctoral thesis
Date of Examination:2021-06-28
Date of issue:2021-07-12
Advisor:Prof. Dr. Lutz Ackermann
Referee:Prof. Dr. Lutz Ackermann
Referee:Prof. Dr. Shoubhik Das
Referee:Prof. Dr. Konrad Koszinowski
Referee:Prof. Dr. Johannes C. L. Walker
Referee:Dr. Holm Frauendorf
Referee:Dr. Daniel Janßen-Müller
Persistent Address: http://dx.doi.org/10.53846/goediss-8723

 

 

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Abstract

English

In recent years, oxidative C–H transformations have emerged as increasingly powerful tools in molecular syntheses. However, despite great progress towards more atom and step economic synthetic methods, oxidative couplings largely rely on precious metal catalysts and stoichiometric amounts of toxic metal oxidants, which compromises the overall sustainability of the C–H activation strategy. Within this thesis, this contradiction was resolved by the direct merger of electrochemistry with 3d metal-catalyzed C–H activation, thus setting the stage for organic syntheses at a unique level of resource economy. The novel metallaelectrocatalysis was employed for the traceless formation of various C–C or C–Het bonds. In addition, the mechanisms of these reactions were investigated by detailed mechanistic studies, uncovering, among others, novel mechanistic scenarios to be effective within cobaltaelectrocatalysis.
Keywords: Electrochemistry; Electrocatalysis; Transition Metal Catalysis; C-H Activation; Renewable Energy; Cobalt; Manganese; Reaction mechanism
 
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