材料科学与技术 ›› 2023, Vol. 165 ›› Issue (0): 85-93.DOI: 10.1016/j.jmst.2023.04.043

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  • 收稿日期:2023-02-07 修回日期:2023-03-30 接受日期:2023-04-16 出版日期:2023-12-01 发布日期:2023-06-07

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

Yuhan Lia,b, Min Zhanga, Bangfu Chena, Ping Ouyanga, Youyu Duanc,*, Kangle Lvd, Fan Donga,*   

  1. aEngineering Research Center for Waste Oil Recovery Technology and Equipment, Ministry of Education, Chongqing Key Laboratory of Catalysis and New Environmental Materials, Chongqing Technology and Business University, Chongqing 400067, China;
    bNanchang Institute of Technology, Nanchang 33044, China;
    cCollege of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China;
    dKey Laboratory of Resources Conversion and Pollution Control of the State Ethnic Affairs Commission, College of Resources and Environmental Science, South-Central Minzu University, Wuhan 430074, China
  • Received:2023-02-07 Revised:2023-03-30 Accepted:2023-04-16 Online:2023-12-01 Published:2023-06-07
  • Contact: *E-mail addresses: . youyuduan@cqu.edu.cn (Y. Duan), dongfan@uestc.edu.cn (F. Dong)

Abstract: Deeply photocatalytic oxidation of NO-to-NO3- holds great promise for alleviating NOx 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