Bipotentiostatic tandem electrocatalysis of the CO2 reduction reaction yielding C2+ fuels

Electrochemical CO2 conversion to fuel molecules is an attractive strategy towards atmospheric carbon attenuation. In the fuel conversion catalysis of carbon dioxide, surface adsorbed CO was often identified as a key intermediate, and the inherently low concentration of which has recently been highl...

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Bibliographic Details
Published in:Green chemistry : an international journal and green chemistry resource : GC 2023-07, Vol.25 (13), p.5290-5295
Main Authors: Kim, Joo Yeon, Kim, Yeonsu, Ryu, C Hyun, Ahn, Hyun S
Format: Article
Language:English
Subjects:
Atmospheric attenuation
Carbon dioxide
Catalysis
Chemical reactions
Chemical reduction
Conversion
Coupling
Coupling (molecular)
Electrochemistry
Electrodes
Fuels
Green chemistry
Mass transport
Propanol
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Summary:Electrochemical CO2 conversion to fuel molecules is an attractive strategy towards atmospheric carbon attenuation. In the fuel conversion catalysis of carbon dioxide, surface adsorbed CO was often identified as a key intermediate, and the inherently low concentration of which has recently been highlighted as an important factor in the low yields of C2+ fuels. Here a bipotentiostatic tandem catalysis system was designed such that the loads for electrosynthesis of CO from CO2 and the subsequent C–C coupling reaction were split to two separate working electrodes with independent potential programming. Coulometric tracking of the reaction indicated efficient turnover of the electrosynthetic CO to fuel molecules at the second working electrode, achieving a high C2+ yield of 67.3% and a 6.5% faradaic efficiency towards 1-propanol. Importantly, the unique capability of the tandem catalysis system allowed control of the CO flux to the second working electrode, which enabled the direct quantification of the C–C coupling turnover frequency on a surface copper atom (0.43 ± 0.06 s−1), when the reaction current was electrode-kinetics controlled with sufficient CO mass transport. Furthermore, the bipotentiostatic reaction platform developed here exhibits modular tunability, such that the expansion of the platform to other sequential electrocatalyses is imaginable.
ISSN:1463-9262
1463-9270
DOI:10.1039/d3gc00974b