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2D materials for electrocatalysis and hydrogen generation as clean energy source
Sanna, Michela ; Kim, Daewoo (oponent) ; Urso, Mario (oponent) ; Pumera, Martin (vedoucí práce)
The electrochemical production of hydrogen from water is gaining more attention as a clean and renewable energy source in response to the alarming environmental issues caused by the exploitation of fossil fuels during the last centuries. However, the process can be considered an environmentally friendly alternative only if it is fuelled using renewable sources of energy, like solar energy, the largest carbon-free resource available on our planet. Solar energy can be converted to electricity via solar panels and electrical energy be used for water splitting via electrocatalysts, such as platinum. Alternatively, the water splitting to hydrogen can be carried out directly via solar light energy. However, the yields of direct photochemical water splitting are low. The combination of both approaches, also called photoelectrochemical water splitting, combines the best of both worlds – electrocatalytic water splitting with the aid of photons. For these reason, the study of novel materials based on earth-abundant elements that can be applied as photoelectrocatalysts for hydrogen generation is fundamental to guiding society toward more sustainable energy production. This thesis explores the potential of the emerging two-dimensional (2D) materials and related layered compounds, alongside investigations into the utility of 3D printing for fabricating functional electrodes in the field of photoelectrochemistry. The study of several transition metal selenophosphites confirmed their potential as photoelectrocatalysts for hydrogen generation, in particular under the influence of visible light. MAX phases were modified through exposure to fluorine gas and the properties of the obtained fluorinated MAX were investigated, starting from their morphology to their potential as photoelectrocatalysts for the hydrogen evolution reaction. The fluorinated phases showed better performances compared to the untreated MAX phases. The improved catalytic activity was attributed to photoactive oxyfluorides that formed as a consequence of the fluorination process. The photoactivity of the MAX phases was further investigated both by theoretical and experimental approaches, to understand the origin of the photocatalytic behaviour. The results showed that the presence of oxide impurities on the phases plays a crucial role in the photoelectrochemical production of hydrogen. The role of the oxides in the photocatalytic activity of these compounds inspired the fabrication and investigation of 3D printed electrodes and their modification with atomic layer deposited oxides, like TiO2, SiO2, and Al2O3. Also in this case, the presence of a thin layer of oxide on the surface of the electrode contributed to significantly better performances under the influence of visible light. The obtained results demonstrated the importance of the fundamental study of novel 2D materials for application in the photoelectrochemical production of hydrogen and open new insights into the fabrication of innovative 3D printed conductive devices that can be modified with functional materials for energy conversion.
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