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This study discusses a class of ceria-based high-entropy oxides designed to optimize charge carrier dynamics, surface reactivity, and CO2 activation efficiency. Due to the advantages of high configurational entropy and multi-element synergy, these materials achieved improved photocatalytic performance, surpassing conventional ceria-based systems. Structural and spectroscopic analyses reveal that Pr3+\/Pr4+ redox pairs and abundant oxygen vacancies create an electronically disordered yet thermodynamically stable environment, which enhances charge separation and suppresses electron-hole recombination. Photocatalytic experiments demonstrated that Ce0.2Zr0.2La0.2Pr0.2Sm0.2O2\u2212\u03b4 (CZLPS) achieves the highest CO2 conversion rate, reaching a conversion of 20.3% under visible light irradiation, significantly surpassing pure ceria (1.4%), with a calculated space-time yield (STY) of 10.15 molCOkg\u20131h\u20131 under the same conditions. First-principles density functional theory (DFT) simulations were employed to investigate the CO2 reduction mechanism on CZLPS catalysts. The study elucidates the Gibbs free energy changes (\u0394G) for each step of the reaction pathways leading to CO and HCOOH formation, highlighting the Zr site of CZLPS as the most active for the CO2RR, which is responsible for the outstanding catalytic activity.<\/jats:p>","DOI":"10.1021\/prechem.5c00456","type":"journal-article","created":{"date-parts":[[2026,4,14]],"date-time":"2026-04-14T04:20:22Z","timestamp":1776140422000},"page":"1414-1432","source":"Crossref","is-referenced-by-count":3,"title":["Defect Chemistry\nin Rare-Earth High-Entropy Oxides\nfor Solar-Driven CO2 Conversion"],"prefix":"10.1021","volume":"4","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3722-7420","authenticated-orcid":true,"given":"Dalibor","family":"Tatar","sequence":"first","affiliation":[{"name":"Josip Juraj Strossmayer University of Osijek , , Cara Hadrijana 8\/A , ,","place":["Osijek, Croatia, 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