Towards a more sustainable future : development and application of heterogeneous CeO2-based catalysts

At present, the majority of all intricate global challenges are related to sustainability. Therefore, the urge for sustainable development is bigger than ever. To date, the chemical sector is already a major driving force for innovation and essential for sustainable growth across all sectors. However, much more scientific contributions will be needed to tackle the difficult task ahead, which is to create a sustainable world whereby the needs of the present are met without compromising the ability of future generations to meet their own needs. Hence, the aim of this thesis is to make a positive contribution to sustainability by applying heterogeneous catalysis in various green chemistry related applications. The research in this PhD thesis is mainly focussed on the development of innovative CeO2-based catalysts and can be divided into four different topics: catalytic combustion of VOCs, plasma-catalytic conversion of CO2, photo-induced reduction of nitrobenzene to aniline, and the selective hydrodeoxygenation of aromatic carbonates. In more detail, chapters 2, 3 and 4 focus on catalyst optimisation to improve the catalytic combustion of toluene, which is a model compound for aromatic VOCs. Based on the obtained results it can be stated that combining noble and transition metals offers a unique approach to limit the costs and consumption of noble metals for industrial large-scale combustion of VOCs. Unfortunately, while intriguing results are obtained regarding the catalytic combustion of VOCs, it cannot be ignored that combustion of carbonaceous compounds results in the production of CO2. Therefore, the fifth chapter tackles the plasma-catalytic conversion of CO2 using CeO2. More specifically, it is investigated if increasing the amount of oxygen vacancies at the surface of CeO2 enhances the dissociation of the stable CO2 molecule, which facilitates the conversion of CO2 into value-added products. Next, in chapter 6 the development of a more sustainable photochemical process to convert nitroarenes into anilines at room temperature and in open atmosphere without the addition of hydrogen is discussed. Additionally, it is examined if the presence of a heterogeneous catalyst can further improve the obtained results. Finally, in chapter 7 a thorough characterisation is provided to gain a better understanding on the selective hydrodeoxygenation of aromatic carbonates when commercially available heterogeneous Ni-SiO2 catalysts are applied. Unravelling the reason behind the remarkable activity is trivial as the successful hydrodeoxygenation provides a next step in the development of important bio-based compounds from wood.