Abstract
Oxygen vacancy control has been one of the most efficient methods to tune the physicochemical properties of conventional oxide materials. A new conceptual multi-principal oxide (MPO) is still lacking a control approach to introduce oxygen vacancies for tuning its inherent properties. Taking multi-principal rare earth-transition metal (CeGdLa-Zr/Hf) oxides as model systems, here we report temperature induced oxygen vacancy generation (OVG) phenomenon in MPOs. It is found that the OVG is strongly dependent on the composition of the MPOs showing different degrees of oxygen loss in (CeGdLaZr)Ox and (CeGdLaHf)Ox under identical high temperature annealing conditions. The results revealed that (CeGdLaZr)Ox remained stable single phase with a marginal decrease in the band gap of about 0.08 eV, whereas (CeGdLaHf)Ox contained two phases with similar crystal structure but different oxygen vacancy concentrations causing semiconductor-to-metal like transition. Due to the intrinsic high entropy, the metallic atoms sublattice in (CeGdLaHf)Ox remains rather stable, regardless of the interstitial oxygen atoms ranging from almost fully occupied (61.84 at%) to almost fully empty (8.73 at%) state in the respective crystal phases. Such highly tunable oxygen vacancies in (CeGdLa-Zr/Hf) oxides show a possible path for band gap engineering in MPOs for the development of efficient photocatalysts.
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