Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 35, Pages 19169-19175Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103102
Keywords
carbon dioxide; copper; electrochemistry; electro-reduction; single crystals
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Funding
- European Research Council under grant ERC-OPERANDOCAT [ERC-725915]
- deutsche Forschungsgemeinschaft (DFG) [SFB1316, EXC 2008-390540038]
- Projekt DEAL
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The identification of active sites for the electrochemical reduction of CO2 to specific products is challenging due to insufficient data on clean electrode surfaces. Research using ultrahigh vacuum methods and surface science techniques showed that minor changes in the preparation of copper single crystals greatly impact their CO2RR selectivity, with structural and morphological effects playing a key role in determining catalytic selectivity.
The identification of the active sites for the electrochemical reduction of CO2 (CO2RR) to specific chemical products is elusive, owing in part to insufficient data gathered on clean and atomically well-ordered electrode surfaces. Here, ultrahigh vacuum based preparation methods and surface science characterization techniques are used 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 predicted to yield hydrocarbons; however, these were found experimentally to favor the production of H-2. Only when roughness and defects are introduced, for example by electrochemical etching or a plasma treatment, are significant amounts of hydrocarbons generated. These results show that structural and morphological effects are the key factors determining the catalytic selectivity of CO2RR.
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