TY - JOUR
T1 - Hydroxide Is Not a Promoter of C2+ Product Formation in the Electrochemical Reduction of CO on Copper
AU - Li, Jing
AU - Wu, Donghuan
AU - Malkani, Arnav S.
AU - Chang, Xiaoxia
AU - Cheng, Mu Jeng
AU - Xu, Bingjun
AU - Lu, Qi
N1 - Funding Information:
This work is supported by the National Key Research and Development Program of China (grant number 2017YFA0208200) and the National Natural Science Foundation of China (grant number 21872079, 21606142).
Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2020/3/9
Y1 - 2020/3/9
N2 - Highly alkaline electrolytes have been shown to improve the formation rate of C2+ products in the electrochemical reduction of carbon dioxide (CO2) and carbon monoxide (CO) on copper surfaces, with the assumption that higher OH− concentrations promote the C−C coupling chemistry. Herein, by systematically varying the concentration of Na+ and OH− at the same absolute electrode potential, we demonstrate that higher concentrations of cations (Na+), rather than OH−, exert the main promotional effect on the production of C2+ products. The impact of the nature and the concentration of cations on the electrochemical reduction of CO is supported by experiments in which a fraction or all of Na+ is chelated by a crown ether. Chelation of Na+ leads to drastic decrease in the formation rate of C2+ products. The promotional effect of OH− determined at the same potential on the reversible hydrogen electrode scale is likely caused by larger overpotentials at higher electrolyte pH.
AB - Highly alkaline electrolytes have been shown to improve the formation rate of C2+ products in the electrochemical reduction of carbon dioxide (CO2) and carbon monoxide (CO) on copper surfaces, with the assumption that higher OH− concentrations promote the C−C coupling chemistry. Herein, by systematically varying the concentration of Na+ and OH− at the same absolute electrode potential, we demonstrate that higher concentrations of cations (Na+), rather than OH−, exert the main promotional effect on the production of C2+ products. The impact of the nature and the concentration of cations on the electrochemical reduction of CO is supported by experiments in which a fraction or all of Na+ is chelated by a crown ether. Chelation of Na+ leads to drastic decrease in the formation rate of C2+ products. The promotional effect of OH− determined at the same potential on the reversible hydrogen electrode scale is likely caused by larger overpotentials at higher electrolyte pH.
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U2 - 10.1002/anie.201912412
DO - 10.1002/anie.201912412
M3 - Article
C2 - 31814246
AN - SCOPUS:85077899127
VL - 59
SP - 4464
EP - 4469
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 11
ER -