Efficient catalytic ozonation via Mn-loaded C-SiO2 Framework for advanced wastewater treatment: Reactive oxygen species evolution and catalytic mechanism

Abstract

Heterogeneous catalytic ozonation (HCO) is attractive for water decontamination and catalyst is a core element. However, it is difficult to maintain high efficiency and stability of catalysts under stern conditions. In this study, we proposed Mn-loaded C-SiO2-Framework (Mn-CSF) which contained stable silica core and robust carbon shell for efficient catalytic ozonation. The pseudo-first-order kinetic rate constant for oxalic acid removal of Mn-CSF catalytic ozonation was 160 % and 875 % higher than those of Mn-SiO2 and pristine CSF, respectively. Mn-CSF was also proven effective in gasification wastewater treatment, where the COD was decreased to 46 mg·L−1, 37 % lower than that of Mn-SiO2. These results indicated that the graphitization carbon layer and Mn significantly enhanced the activity of the catalyst. Furthermore, a fulvic-like component and a protein-like component were recognized through 3D-EEM in coal gasification wastewater. It was proven that Mn-CSF catalytic ozonation exhibited higher fulvic-like component and protein-like component removal compared with ozonation. Moreover, O2− and 1O2 were identified to be responsible for organic degradation in this research. Sufficient external specific surface area and porous structure were important for complex wastewater treatment. Specifically, external specific surface area could enhance the degradation of macromolecular organics while porous structures were vital for smaller molecular pollutant removal. The results highlighted that Mn-CSF was a promising HCO catalyst for advanced wastewater treatment, and this study provided evidence of relationship between structure of catalysts and HCO efficiency.