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. Nonetheless, in order to tailor the chemical reactivity of CO2RR nanocatalysts at the atomic level, fundamental understanding of their structure and surface composition under reaction conditions must be obtained. To fulfill this challenging aim, a synergistic experimental approach taking advantage of a variety of cutting-edge microscopy (EC-AFM, EC-TEM) and spectroscopy (XPS, XAS, MS/GC) methods has been undertaken. This talk will provide new insights into the CO2RR, with special focus on: (i) the evolution of the surface structure of well-oriented single crystal Cu catalysts [Cu(100), Cu(111), Cu(310)]; (ii) the design of size- and shape-controlled catalytically active nanoparticle pre-catalysts (Cu, Cu2O spheres, cubes, octahedra, Ag-Cu2O cubes, ZnO/Cu2O cubes), and (iii) the correlation between the dynamically evolving structure and composition of the electrocatalysts under operando reaction conditions, including pulse electrolysis treatments, and their activity and selectivity. The results 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.

Unveiling the dynamic behavior of CO2 electroreduction catalysts through in situ microscopy and Operando spectroscopy

ACS Spring 2022

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