4.7 Article

Unraveling the multiple roles of Ag species incorporation into OMS-2 for efficient catalytic ozonation: Structural properties and mechanism investigation

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ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2021.106199

关键词

OMS-2; Ag doping; Heterogeneous catalytic ozonation; Oxalic acid; Lewis acid site

资金

  1. National Natural Science Foundation of China [51808412]
  2. Central Government Guidance Projects for Local Science and Technology Development of Hubei Province [2018ZYYD024, 2019ZYYD068]

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Silver incorporated manganese oxide octahedral molecular sieves (Ag-OMSX-T) exhibit superior catalytic performance in the ozonation degradation of organic compounds compared to undoped manganese oxide molecular sieves. The optimal Ag-OMS0.2-180 catalyst shows high activity, stability, and provides insights into the mechanism of oxygen vacancies cycling and reactive oxygen species.
Silver incorporated manganese oxide octahedral molecular sieves (Ag-OMSX-T) were successfully synthesized via a hydrothermal-calcination method. Due to the multiple roles of Ag species doping, the optimal Ag-OMS0.2-180 nanocatalyst with the Ag/Mn molar ratio of 0.2 had the highest TOF value (2.94 x 10(-5) mol g(-1) h(-1)), which could completely degrade 50 mg L-1 OA at pH 5.0 in 30 min much higher than those of OMS-2 (22.3%) in catalytic ozonation system. The results of systematic characterization (such as XRD, XPS, Py-IR, and O-2-TPD) and catalytic performance tests of Ag-OMS0.2-180 clearly demonstrated that the proper amount of Ag incorporation not only facilitated the electron transfer but also induced more formation of Lewis acid sites in Ag-OMS0.2-180 as well as metals (Ag and Mn) as activation sites to collectively favor the catalytic ozonation degradation of OA. In addition, the higher mineralization rate has been achieved (79.6%) and the Ag-OMS0.2-180 exhibited the satisfactory stability and reusability with low metal release during multiple consecutive cycles (>= 5). Meanwhile, the electron spin resonance spectra and radical scavenger tests confirmed that superoxide radical and singlet oxygen were the main reactive oxygen species in catalytic process. The mechanism of solid-liquid interface reaction and the pathway of cycling of oxygen vacancies were also elaborated, which present a new insight for water decontamination.

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