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Selectivity Map for the Late Stages of CO and CO 2 Reduction to C 2 Species on Copper Electrodes
Author(s) -
Piqué Oriol,
Low Qi Hang,
Handoko Albertus D.,
Yeo Boon Siang,
CalleVallejo Federico
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202014060
Subject(s) - ethylene , selectivity , copper , acetaldehyde , chemistry , electrochemistry , ethanol , catalysis , ethylene oxide , inorganic chemistry , electrode , organic chemistry , polymer , copolymer
The electrochemical CO and CO 2 reduction reactions (CORR and CO 2 RR) using copper catalysts and renewable electricity hold promise as a carbon‐neutral route to produce commodity chemicals and fuels. However, the exact mechanisms and structure sensitivity of Cu electrodes toward C 2 products are still under debate. Herein, we investigate ethylene oxide reduction (EOR) as a proxy to the late stages of CORR to ethylene, and the results are compared to those of acetaldehyde reduction to ethanol. Density functional theory (DFT) calculations show that ethylene oxide undergoes ring opening before exclusively reducing to ethylene via *OH formation. Based on generalized coordination numbers ( CN ), a selectivity map for the late stages of CORR and CO 2 RR shows that sites with moderate coordination (5.9 < CN < 7.5) are efficient for ethylene production, with pristine Cu(100) being more active than defective surfaces such as Cu(311). In contrast, kinks and edges are more active for ethanol production, while (111) terraces are relatively inert.