A High‐Entropy Layered Perovskite Coated with In‐situ Exsolved Core‐shell CuFe@FeOx Nanoparticles for Efficient CO2 ElectrolysisZiming Wang, Ting Tan, Ke Du, Qimeng Zhang, Meilin Liu, Chenghao Yang
- Mechanical Engineering
- Mechanics of Materials
- General Materials Science
Solid oxide electrolysis cells (SOECs) are promising energy conversion devices capable of efficiently transforming CO2 into CO, reducing CO2 emissions, and alleviating the greenhouse effect. However, the development of a suitable cathode material remains a critical challenge. Here we report a new SOEC cathode for CO2 electrolysis consisting of high‐entropy Pr0.8Sr1.2(CuFe)0.4Mo0.2Mn0.2Nb0.2O4‐δ (HE‐PSCFMMN) layered perovskite uniformly coated with in‐situ exsolved core‐shell structured CuFe alloy@FeOx (CFA@FeO) nanoparticles. Single cells with the HE‐PSCFMMN‐CFA@FeO cathode exhibits a consistently high current density of 1.95 A cm−2 for CO2 reduction at 1.5 V while maintaining excellent stability for up to 200 h under 0.75 A cm−2 at 800 °C in pure CO2. In‐situ XPS and density functional theory (DFT) calculations confirm that the exsolution of CFA@FeO nanoparticles introduces additional oxygen vacancies within HE‐PSCFMMN substrate, acting as active reaction sites. More importantly, the abundant oxygen vacancies in FeOx shell, in contrast to conventional in‐situ exsolved nanoparticles, enable the extension of the triple‐phase boundary (TPB) from the CFA@FeO/HE‐PSCFMMN interface to the entire FeOx shell, thereby enhancing the kinetics of CO2 adsorption, dissociation, and reduction.
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