La(FeCuMnMgTi)O3 High-Entropy Oxide Nanoparticles as Highly Efficient Catalysts for Solvent-Free Aerobic Oxidation of Benzyl Alcohol

The Journal of Physical Chemistry Letters. 2024. Vol. 15. No. 30. P. 7577–7583.

Ahmad Ostovari Moghaddam, Mehrabi-Kalajahi S., Qi X., Salari R., Fereidonnejad R., Abdollahzadeh A., Uchaev D., Kazakova E., Varfolomeev M., Cabot A., Васенко А. С., Trofimov E.

In this work, a solid-state method for the synthesis of perovskite La-(FeCuMnMgTi)O3 high-entropy oxide (HEO) nanoparticles is detailed. Additionally, the high performance of these nanoparticles as catalysts in the aerobic and solvent-free oxidation of benzyl alcohol is demonstrated. The structural features of HEO nanoparticles are studied by Xray diffraction and high-resolution transmission electron microscopy. The La(FeCuMnMgTi)-O3 nanoparticles demonstrate excellent benzyl alcohol conversion rates and selectivity for benzaldehyde, reaching 10.6% conversion and 52.8% selectivity after reaction for only 4 h and ≤75.6% conversion after 24 h. In addition, the as-prepared HEO catalyst displays robust stability in benzyl alcohol oxidation. Density functional theory calculations demonstrate that the adsorption energy of benzaldehyde on the HEO surface is lower than that of the benzoic acid. This, in turn, hinders the gradual conversion of benzaldehyde to benzoic acid on the surface of HEO and retains benzaldehyde as the main product.

Ключевые слова: nanoparticles, Density functional theory (DFT), High-entropy oxides, benzyl alcohol