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Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
Author(s) -
Ting Louisa Rui Lin,
GarcíaMuelas Rodrigo,
Martín Antonio J.,
Veenstra Florentine L. P.,
Chen Stuart TzeJin,
Peng Yujie,
Per Edwin Yu Xuan,
PabloGarcía Sergio,
López Núria,
PérezRamírez Javier,
Yeo Boon Siang
Publication year - 2020
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.202008289
Subject(s) - chemistry , electrochemistry , crotonaldehyde , butanol , electrolysis , acetaldehyde , electrochemical reduction of carbon dioxide , inorganic chemistry , catalysis , aldol condensation , context (archaeology) , faraday efficiency , electrolyte , organic chemistry , carbon monoxide , ethanol , electrode , paleontology , biology
The electroreduction of carbon dioxide using renewable electricity is an appealing strategy for the sustainable synthesis of chemicals and fuels. Extensive research has focused on the production of ethylene, ethanol and n ‐propanol, but more complex C 4 molecules have been scarcely reported. Herein, we report the first direct electroreduction of CO 2 to 1‐butanol in alkaline electrolyte on Cu gas diffusion electrodes (Faradaic efficiency=0.056 %, j 1‐Butanol =−0.080 mA cm −2 at −0.48 V vs. RHE) and elucidate its formation mechanism. Electrolysis of possible molecular intermediates, coupled with density functional theory, led us to propose that CO 2 first electroreduces to acetaldehyde‐a key C 2 intermediate to 1‐butanol. Acetaldehyde then undergoes a base‐catalyzed aldol condensation to give crotonaldehyde via electrochemical promotion by the catalyst surface. Crotonaldehyde is subsequently electroreduced to butanal, and then to 1‐butanol. In a broad context, our results point to the relevance of coupling chemical and electrochemical processes for the synthesis of higher molecular weight products from CO 2 .