期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 20, 页码 22760-22770出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c00412
关键词
CO2 electrochemical reduction; formate production; electronegativity; tin electrocatalyst; catalyst substrate
资金
- HBIS Group
- Australian Research Council (ARC) [LP160101729]
- University of Queensland (UQ)
- Australian Research Council's Centre for LNG Futures [IC150100019]
- UQ Research Training Program (RTP) scholarship
- Australian Research Council [LP160101729] Funding Source: Australian Research Council
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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