Oxidation of water

Figure 2Liquid fuels are a medium of choice to convert into and store the energy from intermittent energy sources such as sunlight and wind. They present multiple advantages including high energy density and ease of storage over other options. Additionally, liquid fuels benefit from the existing distribution infrastructure, which would ease the utilization of renewable sources to power the transportation sector. The most relevant liquid fuel options in this context are hydrogen, light hydrocarbons, and alcohols, all of which can be synthesized electrochemically and combusted in a carbon-free or carbon-neutral scheme. Hydrogen can be produced by water splitting, where water molecules get oxidized and reduced into oxygen and hydrogen respectively using an external source of electrons. Subsequently, energy from hydrogen can be extracted by combustion either in a fuel cell or an internal combustion engine, resulting in the emission of water. Light hydrocarbons and alcohols can be synthesized by reducing CO2 electrochemically.Figure 1 By using high-concentration CO2 emissions from existing fossil-fueled power plants and chemical facilities and CO2 eventually extracted from the atmosphere, carbon fuels may be used in a carbon-neutral or even carbon-negative cycle, as depicted in Figure 1.

Currently, both water oxidation and the electro-reduction of CO2 suffer from considerable inefficiencies even in the presence of state-of-the-art catalysts. Their improvement requires the development of novel classes of catalysts with enhanced activity and selectivity. This research effort focuses on developing design principles for robust, purely inorganic catalysts with features mimicking natural enzymes. The emphasis is put on the fundamental understanding of the effects of the morphological tailoring at the atomic scale of the catalyst active sites on the surface chemistry and physics involved in the above reactions. The chemical structure and morphology of the active sites are engineered at the atomic level, based on results from Density Functional Theory (DFT) models on reactive surfaces and experimental investigation of well-defined, atomically resolved catalyst surfaces.

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