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Anthropogenic carbon dioxide emissions leading to climate change require to use of renewable carbon sources such as CO2 and biomass which differ from fossil resources by having a higher number of oxygen atoms. Therefore, catalytic C-O bond cleavage will play a pivotal role in their conversion into carbon neutral fuels, materials and chemicals. This thesis will focus on the most challenging substrate for selective C-O bond hydrogenolysis, diaryl ether present in lignin (i.e. one of the components of biomass), summarise the state of research and improve the comprehension in the characteristics a catalyst requires to selectively cleave these bonds without altering other functionalities. We showed that the modification in the electronic state and the resulting polarity between two different metals present in a bimetallic nanoparticle favour the selectivity towards hydrogenolysis of a polar C-O bonds over aromatic ring hydrogenation. In addition, we demon-strate that single metal sites cannot hydrogenate an aromatic ring and hence are selective. Final-ly, we applied our knowledge in C-O bond cleavage in CO2 conversion using propylene carbonate as a relay molecule to produce propylene glycol and methane.
François Maréchal, Daniel Alexander Florez Orrego, Meire Ellen Gorete Ribeiro Domingos, Réginald Germanier
Jan Van Herle, Jürg Alexander Schiffmann, Victoria Xu Hong He, Michele Gaffuri
François Maréchal, Daniel Alexander Florez Orrego, Meire Ellen Gorete Ribeiro Domingos, Réginald Germanier