High-Entropy La(FeCuMnMgTi)O3 Nanoparticles as Heterogeneous Catalyst for CO2 Electroreduction Reaction

Abstract

In this work, La(FeCuMnMgTi)O₃ HEO nanoparticles with a perovskite-type structure are synthesized and used in the electrocatalytic CO₂ reduction reaction (CO₂RR). The catalyst demonstrates high performance as an electrocatalyst for the CO₂RR, with a Faradaic efficiency (FE) of 92.5% at a current density of 21.9 mA cm^-2 under -0.75 V vs a saturated calomel electrode (SCE). Particularly, an FE above 54% is obtained for methyl isopropyl ketone (C₅H₁₀O, MIPK) at a partial current density of 16 mA cm^-2, overcoming all previous works. Besides, the as-prepared HEO catalyst displays robust stability in the CO₂RR. The excellent catalytic performance of La(FeCuMnMgTi)O₃ is ascribed to the synergistic effect between the electronic effects associated with five cations occupying the high-entropy sublattice sites and the oxygen vacancies within the perovskite structure of the HEO. Finally, DFT calculations indicate that Cu plays a vital role in the catalytic activity of the La(FeCuMnMgTi)O₃ HEO nanoparticles toward C2+ products.