Pd and co-based (nano)catalysts for c-c coupling and artificial photosynthesis
- Autores: Jonathan De Tovar Villanueva
- Directores de la Tesis: Xavier Sala Román (dir. tes.), Jordi García-Antón Aviñó (codir. tes.)
- Lectura: En la Universitat Autònoma de Barcelona ( España ) en 2018
- Idioma: español
- Tribunal Calificador de la Tesis: Ramón Yáñez López (presid.), Laia Francàs Forcada (secret.), María Isabel Romero García (voc.)
- Programa de doctorado: Programa de Doctorado en Química por la Universidad Autónoma de Barcelona
- Materias:
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- Resumen
Given the expected increase of global energy consumption and the drawbacks of using fossil fuels (ill-distributed, non-renewable and highly CO2 polluting), it is mandatory to find a new carbon-neutral renewable source of energy for the sustainable development of our society. Hence, a different strategy should be considered to overcome these difficulties. For this purpose and as in many other cases, researchers have obtained inspiration from Nature, particularly from the photosynthetic processes where sunlight energy is stored in the chemical bonds of sugars and starches. Researchers try to mimic Nature storing sunlight energy in the chemical bonds of a fuel such as dihydrogen. From here, the Water Splitting reaction supposes a good candidate since the absorption of four photons provokes the formation of both dioxygen and dihydrogen. Within this context, the use of catalysts usually based in transition metals is necessary to make these two processes viable. In Chapter I, a general introduction about catalysis, nanoparticles, nanocatalysis, C-C coupling and the challenge of artificial photosynthesis is presented as a motivation for the present work. An overview of water oxidation catalysts based on metal nanoparticles is also discussed exposing the most relevant catalysts reported to date.
Chapter II is focused in the objectives of the present work. The main goal of this PhD thesis is the synthesis and the structural characterization of PS-Co3O4-based nanocatalysts for the ulterior study of their reactivity towards electro- and photocatalytic water oxidation. The final objective is to understand the factors that affect their catalytic performance for helping in the future rational design of more efficient and robust catalysts. Additionally, the second goal of this thesis is the testing of molecular and colloidal catalytic systems towards the Suzuki-Miyaura reaction in order to study their dissimilar catalytic behavior.
In Chapter III, a novel method for the preparation of a Co3O4 nanocatalyst functionalized by light-harvesting photosensitizers is presented. All NPs have been thoroughly characterized by ICP, HREM, XPS, IR and Wide Angle X-ray Scattering, while electrochemical and photophysical studies have been undergone with the bare NPs and the hybrid PS-NP systems, respectively, to extract conclusions with regards to their respective ability to electro- and photo-oxidize water.
In Chapter IV, both molecular and colloidal Pd systems based both on an ionic liquid or its N-heterocyclic carbene (NHC) are tested in C-C coupling processes. The conversion, yield and the different reactivity are discussed for the set of four systems.
In Chapter V, the most relevant conclusions of the present research work are discussed.
Finally, Chapter VI includes an annex containing other works that have been carried out and published during this PhD thesis and that are closely related with the present work.
