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

被引:20
作者
Chen, Shuning [1 ]
Ren, Tengfei [1 ]
Zhang, Xiaoying [1 ]
Zhou, Zuoyong [1 ]
Huang, Xia [1 ]
Zhang, Xiaoyuan [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100084, Peoples R China
关键词
Heterogeneous catalytic ozonation; C-SiO2 Framework catalysts; Reactive oxygen species; Advanced wastewater treatment; CARBON NANOTUBES; DEGRADATION;
D O I
10.1016/j.scitotenv.2022.159447
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Heterogeneous catalytic ozonation (HCO) is attractive for water decontamination and catalyst is a core element. How -ever, it is difficult to maintain high efficiency and stability of catalysts under stern conditions. In this study, we pro-posed 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 center dot 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, center dot O2- and 1O2 were identified to be respon-sible for organic degradation in this research. Sufficient external specific surface area and porous structure were impor-tant 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 high-lighted that Mn-CSF was a promising HCO catalyst for advanced wastewater treatment, and this study provided evi-dence of relationship between structure of catalysts and HCO efficiency.
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页数:11
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