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Identifying Structure–Selectivity Correlations in the Electrochemical Reduction of CO 2 : A Comparison of Well‐Ordered Atomically Clean and Chemically Etched Copper Single‐Crystal Surfaces
Author(s) -
Scholten Fabian,
Nguyen KhanhLy C.,
Bruce Jared P.,
Heyde Markus,
Roldan Cuenya Beatriz
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202103102
Subject(s) - selectivity , copper , electrochemistry , yield (engineering) , single crystal , etching (microfabrication) , catalysis , electrode , materials science , crystal (programming language) , chemical engineering , chemistry , analytical chemistry (journal) , inorganic chemistry , crystallography , nanotechnology , metallurgy , organic chemistry , layer (electronics) , engineering , computer science , programming language
The identification of the active sites for the electrochemical reduction of CO 2 (CO 2 RR) 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 CO 2 RR 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 CO 2 RR.