An ultrafast carrier dynamics system from oxygen vacancies modified SnO2 QDs and Zn2SnO4 heterojunction for deeply photocatalytic oxidation of NO

doi:10.1016/j.jmst.2023.04.043

Abstract

Abstract: Deeply photocatalytic oxidation of NO-to-NO₃^- holds great promise for alleviating NO_x pollution. The major challenge of NO photo-oxidation is the highly in-situ generated NO₂ concentration, and the formation of unstable nitrate species causes desorption to release NO₂. In this study, SnO₂ quantum dots and oxygen vacancies co-modified Zn₂SnO₄ (ZSO-SnO₂-OVs) were prepared by a one-step hydrothermal procedure, the NO photo-oxidation was investigated by a combination of solid experimental and theoretical support. Impressively, spectroscopic measurements indicate that fast carrier dynamics can be achieved due to the electron transfer efficiency of ZSO-SnO₂-OVs reaching 99.99%, far outperforming the counterpart and previously reported photocatalysts. During NO oxidation, molecular NO/O₂ and H₂O are efficiently adsorbed/activated around OVs and SnO₂ QDs, respectively. In-situ infrared measurements and calculated electron localized function disclose two main findings: (1) richly electrons enable NO promptly form NO^- instead of toxic NO₂ or NO⁺; (2) the generation of stable and undecomposed bidentate NO₃^- rather than bridging or monodentate one benefits the deep oxidation of NO via shifting reaction sites from O terminals for original ZSO to Sn ones for ZSO-SnO₂-OVs. The synergistic action of SnO₂ QDs and OVs positively contributes to the NO oxidation performance enhancement (60.6%, 0.1 g of sample) and high selectivity of NO to NO₃^- (99.2%). Results from this study advance the mechanistic understanding of NO photo-oxidation and its selectivity to NO₃^- over photocatalysts.

Key words: Zn₂SnO₄, Modification, NO photo-oxidation, Charge transfer efficiency, Reaction mechanism

Yuhan Li, Min Zhang, Bangfu Chen, Ping Ouyang, Youyu Duan, Kangle Lv, Fan Dong. An ultrafast carrier dynamics system from oxygen vacancies modified SnO₂ QDs and Zn₂SnO₄ heterojunction for deeply photocatalytic oxidation of NO[J]. J. Mater. Sci. Technol., 2023, 165: 85-93.

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An ultrafast carrier dynamics system from oxygen vacancies modified SnO₂ QDs and Zn₂SnO₄ heterojunction for deeply photocatalytic oxidation of NO

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