Transition Metal-Free Catalytic Systems for the Utilization of CO2 to Achieve Valuable Chemicals

by Daniel Riemer
Doctoral thesis
Date of Examination:2020-09-28
Date of issue:2020-11-03
Advisor:Prof. Dr. Shoubhik Das
Referee:Prof. Dr. Shoubhik Das
Referee:Prof. Dr. Manuel Alcarazo
Referee:Prof. Dr. Lutz Ackermann
Referee:Prof. Dr. Konrad Koszinowski
Referee:Dr. Michael John
Referee:Dr. Holm Frauendorf
Persistent Address: http://dx.doi.org/10.53846/goediss-8244

 

 

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Abstract

English

The utilization of one of the most threatening greenhouse gases regarding the climate change could help changing its reputation from a harmful waste toward a green alternative feedstock. For the afore-mentioned reason, it would be thus highly interesting to generate valuable fine chemicals and pharmaceutically active drug molecules or their respective intermediates via mild reaction pathways regarding energy consumption and safe reaction procedures and through replacing toxic and harmful reactants by CO2. Thus, four main reactions were envisioned for this thesis with the aim laid on mild reaction conditions. Hence, atmospheric CO2 pressure is one of the key elements for the use of simpler reaction setups and lower operational complexity. A first step towards the fixation of CO2 was the reaction of amines with CO2 toward carbamates, which took place with the aid of a simple base. Moreover, the utilization of CO2 as a soft oxidation promoter was envisioned for the oxidation of primary or secondary alcohol substrates to their respective carbonyl compounds. This reactivity was further extended towards the benzoin condensation of aldehydes with in situ oxidation to their corresponding diketo compounds. Furthermore, the scope of substrates of this oxidation was broadened toward the oxidation of amines to imines.
Keywords: Green Chemistry; CO2 chemistry; metal-free catalysis; organic syntheses
 
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