Heterogeneous catalytic ozonation of clofibric acid using Ce/MCM-48: Preparation, reaction mechanism, comparison with Ce/MCM-41

被引:37
作者
Li, Shangyi [1 ]
Tang, Yiming [1 ,2 ,3 ]
Chen, Weirui [1 ]
Hu, Zhe [1 ]
Li, Xukai [1 ,2 ,3 ]
Li, Laisheng [1 ,2 ,3 ]
机构
[1] South China Normal Univ, Sch Chem & Environm, Guangzhou 510006, Guangdong, Peoples R China
[2] Guangdong Prov Engn Technol Res Ctr Drinking Wate, Guangzhou 510006, Guangdong, Peoples R China
[3] Guangdong Prov Key Lab Funct Mat Environm Protect, Guangzhou 510006, Guangdong, Peoples R China
基金
中国博士后科学基金;
关键词
Heterogeneous catalytic ozonation; Ce/MCM-48; Clofibric acid; Mineralization; MESOPOROUS MOLECULAR-SIEVES; CARE PRODUCTS PPCPS; ROOM-TEMPERATURE; WATER; OXIDATION; SILICA; BEHAVIOR; MCM-48; OZONE; PHARMACEUTICALS;
D O I
10.1016/j.jcis.2017.05.042
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Three-dimensional mesoporous MCM-48 and Ce loaded MCM-48 (Ce/MCM-48) were synthesized by hydrothermal and impregnating methods, respectively. They were characterized by XRD, SEM, TEM, EDS, XPS, N-2 adsorption-desorption techniques, and the results showed that Ce/MCM-48 still retained a highly ordered cubic structure. A series of experiments were conducted to study the catalytic activity of Ce/MCM-48 and Ce/MCM-41 for ozonation of clofibric acid in aqueous solution. Total Organic Carbon (TOC) removal efficiency in Ce/MCM-48/O-3 can be improved to 64% at 120 min reaction time, 54% by Ce/MCM-41/O-3, only 24% by MCM-48/O-3, 23% by single ozonation. Ce/MCM-48 did not show any adsorption capacity for CA. Effect of initial pH revealed that active sites were surface protonated hydroxyl groups. The restraint of phosphate and sodium hydrogen sulfite (NaHSO3) on the mineralization of CA illustrated more hydroxyl radicals were generated by Ce/MCM-48 catalysts than Ce/MCM-41. The degradation pathway of CA was investigated by the alterations of pH under different conditions. Recycle tests of catalysts demonstrated that compared with Ce/MCM-41, Ce/MCM-48 exhibited more excellent catalytic efficiency and stability because of its unique pore systems. (C) 2017 Elsevier Inc. All rights reserved.
引用
收藏
页码:238 / 246
页数:9
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