Innovative aerosol-based synthesis of nanostructured catalysts for the direct upgrading of glycerol
(2023)
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- Abstract
- Fossil fuels' scarcity, expense, and environmental hazards necessitate sustainable alternatives. Biofuels, like biodiesel, derived from organic materials, offer promising renewable energy options with low environmental impact. Biodiesel production has significantly grown and is projected to reach 46 billion liters by 2030. The main by-product, crude glycerol, poses a waste issue, but its valorization into high-value chemicals can enhance biodiesel production's value chain. Alkyl lactates offer versatile applications, especially for synthesizing biopolymers such as polylactic acid from bio-based sources like sugars and glycerol. The catalytic transformation of glycerol to alkyl lactates relies on a multistep process involving noble metal nanoparticles and Lewis acid sites. Green chemistry principles emphasize developing heterogeneous catalysts, combining different catalysts in one reactor, or creating multifunctional catalysts to efficiently run the reactions. However, combining different catalytic sites on one unique material can be challenging as multi-steps synthesis can damage the pre-existing active sites, be timeconsuming and produce many wastes. This thesis addresses the existing challenges in the current research on synthesizing bifunctional catalysts. On the one hand, new types of supported gold nanoparticles are prepared in one-pot with their support by the aerosol-assisted sol-gel technique, and investigated with a particular focus on the control of the nanoparticles formation and avoiding their sintering. Upon optimization of the synthesis parameters, small gold nanoparticles embedded on a silica support is successfully prepared and this novel synthesis protocol was successfully extended to other metals. These materials are exploited for the selective oxidation of glycerol to dihydroxyacetone. On the other hand, the synthesis of bifunctional catalysts, and more precisely combining supported metal nanoparticles and Lewis acid sites is investigated. These catalysts promote the direct conversion of glycerol to lactates, converting rapidly the intermediate (dihydroxyacetone) and minimizing the formation of side-products. The benefit to run the cascade reaction with a bifunctional material as compared to mechanical mixtures is demonstrated.
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Citations
Van der Verren, M. (2023). Innovative aerosol-based synthesis of nanostructured catalysts for the direct upgrading of glycerol. https://hdl.handle.net/2078.5/233939