4.7 Article

A partially Fe-substituted perovskite electrode for enhancing Zn-CO2 batteries

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CHEMICAL ENGINEERING JOURNAL
卷 474, 期 -, 页码 -

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ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2023.145594

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Perovskite catalyst; Faraday efficiency; In-situ Raman; Fe substitution; Zn-CO2 battery

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Efficient and cost-effective CO2RR perovskite catalyst was developed by partially substituting Fe to the B site of precious metal-free La0.5Sr0.5MnO3 (LSM) perovskite. The Fe-doped catalyst showed improved electrochemical performance, Faraday efficiency, battery durability, and battery power density, making it a promising CO2RR electrocatalyst for Zn-CO2 batteries.
Aqueous Zn-CO2 batteries are a new technology for reducing carbon dioxide emissions and converting CO2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO2 reduction reaction(CO2RR) in these batteries. The technical challenges of CO2RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO2RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La0.5Sr0.5MnO3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La0.5Sr0.5MnO3 (LSM) and substituted La0.5Sr0.5Fe0.6MnO3 (LSF0.6M) catalysts were conducted, LSF0.6M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO2 reduction reaction (CO2RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO2RR within the battery system. These results highlight LSF0.6M perovskite as a very promising CO2RR electrocatalyst for Zn-CO2 battery.

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