Issue 10, 2011

A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes

Abstract

We have investigated the reaction mechanism of the electrochemical reduction of carbon dioxide to hydrocarbons on copper electrodes. This reaction occurs via two pathways: a C1 pathway leading to methane, and a C2 pathway leading to ethylene. To identify possible intermediates in the reduction of carbon dioxide we have studied the reduction of small C1 and C2 organic molecules containing oxygen. We followed the formation and consumption of intermediates during the reaction as a function of potential, using online mass spectrometry. For the C1 pathway we show that it is very likely that CHOads is the key intermediate towards the breaking of the C–O bond and, therefore, the formation of methane. For the C2 pathway we suggest that the first step is the formation of a CO dimer, followed by the formation of a surface-bonded enediol or enediolate, or the formation of an oxametallacycle. Both the enediol(ate) and the oxametallacycle would explain the selectivity of the C2 pathway towards ethylene. This new mechanism is significantly different from existing mechanisms but it is the most consistent with the available experimental data.

Graphical abstract: A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes

Article information

Article type
Edge Article
Submitted
08 May 2011
Accepted
17 Jun 2011
First published
21 Jul 2011

Chem. Sci., 2011,2, 1902-1909

A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes

K. J. P. Schouten, Y. Kwon, C. J. M. van der Ham, Z. Qin and M. T. M. Koper, Chem. Sci., 2011, 2, 1902 DOI: 10.1039/C1SC00277E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements