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Nature achieves the selective transformation of simple and inert chemical building blocks into highly functionalised molecules. The amino acid family is one representative example which features a multicarbon backbone and different functional groups. Although the activation of small molecules such as carbon monoxide (CO) and carbon dioxide (CO2) has attracted a lot of recent attention, systems allowing the transformation of these C1 building blocks into multicarbon (C2+) products are scarce, with very little precedence for their functionalisation into value-added C2+ molecules of high general interest. In this JCJC project, I describe an innovative strategy using divalent lanthanide complexes for the activation and reductive coupling of CO into reactive oxocarbon products. Upon treatment with CO2, very reactive intermediates are formed that allow C–H activation on typically inert hydrocarbon substrates, as well as other functionalisation patterns through the formation of new C–C or C–N bonds. Supported by preliminary results, the goal of this project is to create functionalised molecules of high structural complexity through a unique activation and functionalisation procedure of CO and CO2. Following the functionalisation reactions, I will develop strategies for the recycling of the active divalent lanthanide complexes under mild conditions. For this purpose, electrochemical procedures will be of high interest as they constitute resource-economical alternatives to the use of external reducing agents. The ultimate goal is to achieve electrocatalytic procedures for these transformations. Successful results will open new avenues in the field of small molecule activation, as value-added functionalised C2+ products will be directly formed from simple abundant and polluting gaseous molecules, therefore minimising our dependency on pre-functionalised petroleum-derived reagents.
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