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https://hdl.handle.net/2440/137702
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Type: | Journal article |
Title: | Stabilizing Oxidation State of SnO₂ for Highly Selective CO₂ Electroreduction to Formate at Large Current Densities |
Other Titles: | Stabilizing Oxidation State of SnO2 for Highly Selective CO2 Electroreduction to Formate at Large Current Densities |
Author: | Jiang, Y. Shan, J. Wang, P. Huang, L. Zheng, Y. Qiao, S.-Z. |
Citation: | ACS Catalysis, 2023; 13(5):3101-3108 |
Publisher: | American Chemical Society |
Issue Date: | 2023 |
ISSN: | 2155-5435 2155-5435 |
Statement of Responsibility: | Yunling Jiang, Jieqiong Shan, Pengtang Wang, Linsen Huang, Yao Zheng, and Shi-Zhang Qiao |
Abstract: | Even though electrocatalytic CO2 reduction reaction (CO2RR) to formate has made significant advances, achieving a high cell energy efficiency at industrial-level current densities is still a bottleneck for the large-scale application of this technology. SnO2 is a promising electrocatalyst for formate production but is restricted by the unstable oxidation state under high reduction potentials, causing catalyst reconstruction and inactivation. Herein, we present an atomic doping strategy (by Cu, Bi, or Pt) to trigger the emergence of oxygen vacancy in the SnO2 lattice and stabilize the oxidation state of SnO2 during CO2RR. As a result, the optimal Cu-incorporated SnO2 can keep a high formate Faradic efficiency of >80% and a cell energy efficiency of about 50−60% at a wide range of current densities up to 500 mA cm−2 in a commercial flow cell, surpassing most reported works. A set of in situ spectroscopy measurements and controlled electrochemical tests suggest that the oxygen vacancy, induced by the participation of Cu/Bi/Pt single atoms, holds the key to stabilizing SnO2 as well as promoting the adsorption of formate-related *OCHO reaction intermediate. A qualitative relationship between the oxygen vacancy concentration and CO2-to-formate conversion is constructed on a series of doped SnO2 catalysts. |
Keywords: | oxidation state of SnO2; atom doping; oxygen vacancy; electrocatalytic CO2 reduction; large current density; formate |
Rights: | © 2023 American Chemical Society |
DOI: | 10.1021/acscatal.3c00123 |
Grant ID: | http://purl.org/au-research/grants/arc/FL170100154 http://purl.org/au-research/grants/arc/FT200100062 http://purl.org/au-research/grants/arc/DP220102596 http://purl.org/au-research/grants/arc/LP210301397 http://purl.org/au-research/grants/arc/DP190103472 |
Published version: | http://dx.doi.org/10.1021/acscatal.3c00123 |
Appears in Collections: | Chemical Engineering publications |
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