In the quest for developing a sustainable energy economy, the electrochemical reduction of carbon dioxide (CO2RR) into value-added chemicals and fuels offers the potential to close the anthropogenic carbon cycle and store renewable energy into chemical bonds. It is therefore of particular interest to develop efficient and selective electrocatalysts, which reduce the reaction overpotential and steer the reaction toward hydrocarbons and multicarbon oxygenates (C2+ products). Nonetheless, in order to tailor the chemical reactivity of CO2RR nanocatalysts at the atomic level, fundamental understanding of their physical and chemical properties under reaction conditions must be obtained. To fulfill this challenging goal, a synergistic experimental approach taking advantage of a variety of cutting-edge methods (EC-AFM, EC-TEM, TPD, XPS, XAS, Raman Spectr., DEMS, GC) has been undertaken.
This talk will provide insight into the electrocatalytic reduction of CO2. Important aspects that will be discussed are: (i) the design of size- and shape-controlled catalytically active nanoparticles (Cu, Zn, Cu-Zn, Cu-Ag) (ii) the role of the NP size and shape on the catalytic activity and selectivity, (iii) the importance of defects to activate well-oriented and atomically-ordered Cu single crystal surfaces, (iv) the evolution of the structure and composition of the electrocatalysts under operando reaction conditions and their influence on the catalytic performance, (v) the possibility of using pulsed-electrolysis to tune the reaction selectivity, including a comparison of model (Cu(100)) and real (Cu nanocubes) electrocatalysts at industrially relevant current densities in a gas-fed flow cell. These findings are expected to open up new routes for the reutilization of CO2 through its direct conversion into valuable chemicals and fuels such as ethylene and ethanol.
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