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Fe-Ce协同改性MCM-41高效催化臭氧氧化四环素的特性与机理    

Characteristics and Mechanism of Efficient Degradation of Tetracycline by Fe-Ce Bimetallic Synergistically Modified MCM-41 in Catalytic Ozonation

文献类型:期刊文献

中文题名:Fe-Ce协同改性MCM-41高效催化臭氧氧化四环素的特性与机理

英文题名:Characteristics and Mechanism of Efficient Degradation of Tetracycline by Fe-Ce Bimetallic Synergistically Modified MCM-41 in Catalytic Ozonation

作者:马玮钰[1];张东平[1];孙贤波[1];蔡正清[1,2];刘勇弟[1]

机构:[1]华东理工大学资源与环境工程学院,工业废水无害化与资源化国家工程研究中心,200237;[2]上海污染控制与生态安全研究院,200092:上海

年份:2025

卷号:51

期号:10

起止页码:240

中文期刊名:水处理技术

外文期刊名:Technology of Water Treatment

收录:;北大核心:【北大核心2023】;

基金:国家自然科学基金(22176061)。

语种:中文

中文关键词:催化臭氧氧化;Fe-Ce-MCM-41;抗生素

外文关键词:catalytic ozonation;Fe-Ce-MCM-41;antibiotics

摘要:本文通过Fe、Ce双金属掺杂制备了Fe-Ce-MCM-41材料,并应用于催化臭氧氧化四环素(TC)。在最佳条件下(pH 4.5、催化剂投加量0.4 g/L、O_(3)投加速率6 mg/min),Fe-Ce-MCM-41/O_(3)对TC的降解和矿化率分别达到98.0%和66.1%,矿化率提升至无催化剂系统的6.3倍。体系的主要活性氧物种(ROS)为·OH和O_(2)·^(-)。表面暴露的Fe和Ce是电子转移的活性位点,材料比表面积的提升及路易斯酸位点的增加有利于O_(3)分解。MCM-41良好的吸附性以及Fe^(3+)/Fe^(2+)与Ce^(4+)/Ce^(3+)氧化还原偶联共同促进了Fe-Ce-MCM-41的催化性能,显著改善了传统金属基催化剂比表面积低、团聚烧结和离子浸出等问题。通过构建Fe-Ce双金属活性中心与MCM-41载体协同体系,实现了臭氧催化氧化能力的显著提升,研究结果可为合成高效臭氧氧化催化剂提供参考。
In this paper,Fe-Ce-MCM-41 materials were prepared by Fe and Ce bimetallic doping and applied to catalytic ozonation of tetracycline(TC).Under the optimal conditions(pH 4.5,catalyst dosage 0.4 g/L,O_(3) dosage 6 mg/min),the degradation and mineralization rates of TC by Fe-Ce-MCM-41/O_(3) reached 98.0%and 66.1%,respectively,and the mineralization rate was 6.3 times higher than that of the O_(3) system(without catalysts).The main reactive oxygen species(ROS)of the system are?OH and O_(2)?^(-).The exposed Fe and Ce on the surface are the active sites for electron transfer,the increased surface area and surface Lewis acid sites are beneficial to O3 decomposition.The good adsorption of MCM-41 and the redox coupling of Fe^(3+)/Fe^(2+)and Ce^(4+)/Ce^(3+)jointly promoted the catalytic performance of Fe-Ce-MCM-41,which significantly improved the problems of low specific surface area,agglomeration sintering and ion leaching of traditional metal-based catalysts.This work dramatically improved the catalytic ozonation performance by constructing the synergistic system of Fe-Ce bimetallic active center and MCM-41 carrier,and provided reference for the synthesis of efficient ozone oxidation catalysts.

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