Issue 23, 2021

Spatial-confinement induced electroreduction of CO and CO2 to diols on densely-arrayed Cu nanopyramids

Abstract

The electroreduction of carbon dioxide (CO2) and carbon monoxide (CO) to liquid alcohol is of significant research interest. This is because of a high mass-energy density, readiness for transportation and established utilization infrastructure. Current success is mainly around monohydric alcohols, such as methanol and ethanol. There exist few reports on converting CO2 or CO to higher-valued diols such as ethylene glycol (EG; (CH2OH)2). The challenge to producing diols lies in the requirement to retain two oxygen atoms in the compound. Here for the first time, we demonstrate that densely-arrayed Cu nanopyramids (Cu-DAN) are able to retain two oxygen atoms for hydroxyl formation. This results in selective electroreduction of CO2 or CO to diols. Density Functional Theory (DFT) computations highlight that the unique spatial-confinement induced by Cu-DAN is crucial to selectively generating EG through a new reaction pathway. This structure promotes C–C coupling with a decreased reaction barrier. Following C–C coupling the structure facilitates EG production by (1) retaining oxygen and promoting the *COH–CHO pathway, which is a newly identified pathway toward ethylene glycol production; and, (2) suppressing the carbon–oxygen bond breaking in intermediate *CH2OH–CH2O and boosting hydrogenation to EG. Our findings will be of immediate interest to researchers in the design of highly active and selective CO2 and CO electroreduction to diols.

Graphical abstract: Spatial-confinement induced electroreduction of CO and CO2 to diols on densely-arrayed Cu nanopyramids

Supplementary files

Article information

Article type
Edge Article
Submitted
24 mars 2021
Accepted
04 mai 2021
First published
07 mai 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2021,12, 8079-8087

Spatial-confinement induced electroreduction of CO and CO2 to diols on densely-arrayed Cu nanopyramids

L. Chen, C. Tang, K. Davey, Y. Zheng, Y. Jiao and S. Qiao, Chem. Sci., 2021, 12, 8079 DOI: 10.1039/D1SC01694F

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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