High-entropy oxides (HEOs) have recently emerged as a novel class of catalyst supports with highly tunable composition–function relationships, showing significant potential across various chemical reactions. Herein, we developed highly dispersed iron oxide nanoparticles supported on HEOs through a one-step precipitation method, utilizing a spinel FeAl2O4 framework doped with multiple elements. The resulting HEOs demonstrated markedly stronger metal-support interactions (SMSI) compared to pure FeAl2O4. Structural analysis via XRD, HTEM, and EDS confirmed the formation of a single-phase HEO matrix with smaller Fe2O3 nanoparticles on the surface relative to FeAl2O4. H2-TPR analysis revealed a lower reduction temperature for HEOs than FeAl2O4, indicating enhanced reducibility. With catalytic CO2 hydrogenation as a model, the FeNa/HEO catalyst outperformed FeNa/FeAl2O4, achieving a CO2 conversion rate of 40.03% and a C2-C4 olefin (C2=-C4=) selectivity of 39.28%. Furthermore, H2-TPD analysis showed that FeNa/HEO exhibited improved H2 adsorption capability and resistance to secondary hydrogenation, thereby increasing the olefin/paraffin (O/P) ratio and enhancing C2=-C4=selectivity. This study presents a promising approach for designing high-entropy-supported catalysts and offers valuable insights for developing metal oxide-supported catalysts with tailored SMSI effects.

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