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New insight into the visible-light-driven photoinduced electron transfer mechanism for ozone activation over defective sites of ceria for organic compounds destruction

초록/요약

Herein, we prepared CeO2 with varying concentrations of oxygen vacancies (Ov) and investigated the effects of the Ov concentration and photoinduced electron transfer (PET) on O3 activation under visible-light-driven (VLD) photocatalytic-ozonation (PO) for removal of oxalic acid (OA). Density functional theory calculations showed the formation of Ov reduced the bandgap of CeO2, leading to region around the Ce atom with a low adsorption energy barrier toward O3. Notably, no distinct linear correlation was found between the Ov concentration and VLD-PO activity. This implies that CeO2 with a lower amount of Ov (14.64%) exhibits better PET and higher photoexcited electron density than CeO2 with a relatively higher Ov (17.62%), suggesting that the PET properties of CeO2 are crucial for the Ov regeneration and O3 activation and conversion for OA removal. Electric energy per order (EEO) for VLD-PO using CeOx(7 0 0) was 6.94 kWh m−3 order−1. Additionally, bioassay experiments with Daphnia Magna showed toxicity reduction in the PO-treated effluent and continuous-flow experiments (CFEs) proved that VLD-PO could effectively remediate the toxic and refractory micropollutants containing water. The study findings can promote the application of PO systems in water treatment for treating organic pollutants. © 2023

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