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Abstract:
Despite significant theoretical efforts, the identification of the active sites for the electrochemical reduction of CO2(CO2RR) to specific chemical products has remained elusive. This is partially due to insufficient experimental data gathered on clean and atomically well-ordered electrode surfaces. Here, ultrahigh vacuum based preparation methods and surface science characterization techniques are used together with gas chromatography to demonstrate that subtle changes in the preparation of well-oriented Cu(100) and Cu(111) single crystal surfaces drastically affect their CO2RR selectivity. Copper single crystals with clean, flat, and atomically ordered surfaces are theoretically predicted to yield hydrocarbons. However, these were found experimentally to favour the production of H2. Only when roughness and defects are introduced, for example through an electrochemical etching or a plasma treatment, significant amounts of hydrocarbons are generated. These results clearly indicate that structural and morphological effects are the key factors determining the catalytic selectivity of CO2RR.
