Publication date: 27th March 2025
Several rare-earth-based nanocrystalline high-entropy oxides (HEOs) with fluorite type of structure and average crystallite sizes between 6 and 8 nm were prepared and their photocatalytic behaviour towards photocatalytic CO2 reduction and photoelectrochemical water splitting for hydrogen generation was examined [1], [2]. The cationic site in the fluorite lattice consists of five equimolar elements selected from the group of rare-earth elements including La, Ce, Pr, Eu, and Gd and second-row transition metals, Y and Zr. Studied HEOs exhibit bandgaps in the range from 1.91 eV to 3.0 eV and appropriate valence and conduction bands for water splitting. They reveal high photocatalytic activity that is mostly attributed to the accessibility of more photocatalytic active sites. The materials successfully produce hydrogen by photocatalytic water splitting, suggesting the potential of HEOs as new photocatalysts. The photocatalytic performances of all studied HEOs outperform the single fluorite oxides or equivalent mixed oxides. The Ce0.2Zr0.2La0.2Pr0.2Y0.2O2 (CZLPY) engender hydrogen in 9.2 µmolmg–1 per hour that is much higher content than for pristine CeO2 material which amounts to 0.8 µmolmg–1 per hour. Systematic tests showed the effect of a high–entropy system compared to mid–entropy oxides. XPS, in–situ DRIFTS as well as DFT calculation elucidate the synergistic impact of Ce, Zr, La, Nd, and Sm, resulting in an optimal Ce3+/Ce4+ ratio. The observed formate–routed mechanism and a surface with high affinity to CO2 reduction offer insights into the photocatalytic enhancement.
This work has been supported by the Croatia-Israeli bilateral project entitled: High-Entropy Oxides Photoabsorbers for Efficient and Stable Photoelectrochemical Hydrogen Generation.
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