Li, Mengran and Tian, Xiaohe and Garg, Sahil and Rufford, Thomas E. and Zhao, Peiyao and Wu, Yuming and Yago, Anya Josefa and Ge, Lei 
ORCID: https://orcid.org/0000-0003-2989-0329 and Rudolph, Victor and Wang, Geoff (Guoxiong)
(2020)
Modulated Sn Oxidation States over a Cu2O-Derived Substrate for Selective Electrochemical CO2 Reduction.
ACS Applied Materials & Interfaces, 12 (20).
pp. 22760-22770.
ISSN 1944-8244
Abstract
Pursuing high catalytic selectivity is challenging but paramount for an efficient and low-cost CO2 electrochemical reduction (CO2R). In this work, we demonstrate a significant correlation between the selectivity of CO2R to formate and the duration of tin (Sn) electrodeposition over a cuprous oxide (Cu2O)-derived substrate. A Sn electrodeposition time of 120 s led to a cathode with a formate Faradaic efficiency of around 81% at −1.1 V vs reversible hydrogen electrode (RHE), which was more than 37% higher than those of the Sn foil and the sample treated for 684 s. This result highlights the significant role of the interface between deposited Sn and the cuprous-derived substrate in determining the selectivity of CO2R. High-resolution X-ray photoelectron spectra revealed that the residual cuprous species at the Cu/Sn interfaces could stabilize Sn species in oxidation states of 2+ and 4+, a mixture of which is essential for a selective formate conversion. Such modulation effects likely arise from the moderate electronegativity of the cuprous species that is lower than that of Sn2+ but higher than that of Sn4+. Our work highlights the significant role of the substrate in the selectivity of the deposited catalyst and provides a new avenue to advance selective electrodes for CO2 electrochemical reduction.
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| Item Type: | Article (Commonwealth Reporting Category C) |
|---|---|
| Refereed: | Yes |
| Item Status: | Live Archive |
| Faculty/School / Institute/Centre: | Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -) |
| Faculty/School / Institute/Centre: | Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -) |
| Date Deposited: | 05 Jan 2021 02:53 |
| Last Modified: | 19 Jan 2021 04:01 |
| Uncontrolled Keywords: | CO2 electrochemical reduction; formate production; electronegativity; tin electrocatalyst catalyst; substrate |
| Fields of Research (2008): | 03 Chemical Sciences > 0306 Physical Chemistry (incl. Structural) > 030604 Electrochemistry 09 Engineering > 0904 Chemical Engineering > 090402 Catalytic Process Engineering |
| Fields of Research (2020): | 34 CHEMICAL SCIENCES > 3406 Physical chemistry > 340604 Electrochemistry 40 ENGINEERING > 4004 Chemical engineering > 400404 Electrochemical energy storage and conversion |
| Socio-Economic Objectives (2008): | D Environment > 96 Environment > 9603 Climate and Climate Change > 960302 Climate Change Mitigation Strategies |
| Socio-Economic Objectives (2020): | 19 ENVIRONMENTAL POLICY, CLIMATE CHANGE AND NATURAL HAZARDS > 1903 Mitigation of climate change > 190301 Climate change mitigation strategies |
| Identification Number or DOI: | https://doi.org/10.1021/acsami.0c00412 |
| URI: | http://eprints.usq.edu.au/id/eprint/38709 |
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