Please use this identifier to cite or link to this item:
https://hdl.handle.net/2440/131382
Citations | ||
Scopus | Web of Science® | Altmetric |
---|---|---|
?
|
?
|
Type: | Journal article |
Title: | Role of oxygen-bound reaction intermediates in selective electrochemical CO₂ reduction |
Other Titles: | Role of oxygen-bound reaction intermediates in selective electrochemical CO(2) reduction |
Author: | Zhi, X. Vasileff, A. Zheng, Y. Jiao, Y. Qiao, S. |
Citation: | Energy and Environmental Science, 2021; 14(7):3912-3930 |
Publisher: | Royal Society of Chemistry |
Issue Date: | 2021 |
ISSN: | 1754-5692 1754-5706 |
Statement of Responsibility: | Xing Zhi, Anthony Vasileff, Yao Zheng, Yan Jiao and Shi-Zhang Qiao |
Abstract: | The electrochemical CO₂ reduction reaction (CRR) is intrinsically complex given the multiple possible reaction pathways and end products. Consequently, selectivity is a persistent challenge for the design and operation of CRR electrocatalysts. A detailed understanding of key elementary steps and surface-bound species involved in the C₁–C₃ pathways is important for directing the reaction to a target product. However, there has been limited success in fully explaining the selectivity of CO₂ reduction, such as the competing production of oxygen-free hydrocarbons and oxygen-containing alcohols. Recently, oxygen-bound intermediates have been identified as essential species to help explain the full reaction roadmap for CO₂ reduction. This Review explores the important role of oxygen-bound intermediates in affecting CRR selectivity to the many reduction products, ranging from two electron products to higher reduced products. These oxygen-bound intermediates have a big influence on addressing mechanistic aspects of competing reaction pathways, based on extensive analysis of adsorption behaviour, reaction thermodynamics and reaction kinetics. Considering available theoretical calculations, electrochemical measurements and operando spectroscopy observations, we highlight the preferred reaction pathways to certain products when regulated by oxygen-bound species. The geometries of these oxygen-bound intermediates and their binding on a catalyst surface dictate the breakage or preservation of C–O bonds, which has a significant effect on directing selectivity toward a final product. Based on this mechanistic evaluation, we summarize practical techniques for probing the evolution of intermediates and propose possible strategies for promoting the selectivity of electrocatalysts. |
Rights: | This journal is © The Royal Society of Chemistry 2021 |
DOI: | 10.1039/d1ee00740h |
Grant ID: | http://purl.org/au-research/grants/arc/DP190103472, http://purl.org/au-research/grants/arc/FT190100636 http://purl.org/au-research/grants/arc/FL170100154 |
Published version: | http://dx.doi.org/10.1039/d1ee00740h |
Appears in Collections: | Aurora harvest 4 Chemical Engineering publications |
Files in This Item:
There are no files associated with this item.
Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.