Modulated Sn Oxidation States over a Cu2O-Derived Substrate for Selective Electrochemical CO2 Reduction

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.


Statistics for USQ ePrint 38709
Statistics for this ePrint Item
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

Actions (login required)

View Item Archive Repository Staff Only