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高稳定性锌铝层状双氧化物复合材料上阿特拉津的催化臭氧氧化:效果与机制

Facilitated catalytic ozonation of atrazine over highly stabilized Zn-Al layered double oxides composites: efficacy and mechanism.

作者信息

Li Shangkun, Li Yangang, Sun Lei, Pan Fei, Yuan Xiangjuan, Xia Dongsheng

机构信息

School of Environmental Engineering, Wuhan Textile University, Wuhan, People's Republic of China.

Research and Development Center of Beijing Drainage Group Technology, Beijing, People's Republic of China.

出版信息

Environ Technol. 2023 Apr;44(10):1478-1492. doi: 10.1080/09593330.2021.2005687. Epub 2021 Nov 28.

DOI:10.1080/09593330.2021.2005687
PMID:34762002
Abstract

A series of Zn-Al Layered Double Oxides (ZnAl-LDO) composites were prepared by the hydrothermal and calcination method via employing the Zn-Al Layered Double Hydroxide (ZnAl-LDH) as the precursors in the present study. The structural properties and the catalytic ozonation activity of ZnAl-T composites synthesized with different Zn/Al molar ratios and calcination temperatures were systematically investigated. Diversified characterizations were applied to analyze the phase structure and chemical composition of ZnAl-T composites. As the calcination temperature increased, the layered ZnAl-LDH structure could be entirely destroyed and the crystallinity gradually improved. With the Zn/Al mole ratio of 4.0 and calcination temperature of 500°C, the Zn4Al-500 composite obtained the outstanding catalytic ozonation performance for atrazine (ATZ) degradation with the pseudo-first-order constant of 0.5080 min, which was 5 times more than that in O alone. Meanwhile, the ATZ degradation efficiency was gradually enhanced from 44.1% to 99.9% within 3.0 min when the solution pH ranged from 3.0 to 10.0. Besides, the ZnAl-500 composite exhibited splendid stability over multiple reaction cycles. In addition, the radical scavenging test and electron spin resonance measurement demonstrated that superoxide radical and hydroxyl radical are the dominant reactive species in O/ZnAl-500 process. Moreover, nineteen and ten transformation products were detected in O alone and O/ZnAl-500 process, and possible degradation pathways of ATZ were further elucidated. Overall, the ZnAl-500 composite would provide a potential alternative for pollutants removal due to its high catalytic ozonation efficiency, stability, and reusability.

摘要

在本研究中,通过水热和煅烧方法,以锌铝层状双氢氧化物(ZnAl-LDH)为前驱体制备了一系列锌铝层状双氧化物(ZnAl-LDO)复合材料。系统研究了不同锌铝摩尔比和煅烧温度合成的ZnAl-T复合材料的结构性能和催化臭氧化活性。采用多种表征手段分析了ZnAl-T复合材料的相结构和化学成分。随着煅烧温度的升高,层状ZnAl-LDH结构可被完全破坏,结晶度逐渐提高。在锌铝摩尔比为4.0、煅烧温度为500℃时,Zn4Al-500复合材料对阿特拉津(ATZ)降解具有优异的催化臭氧化性能,其准一级反应常数为0.5080 min,是单独臭氧氧化时的5倍。同时,当溶液pH值在3.0至10.0范围内时,ATZ降解效率在3.0 min内从44.1%逐渐提高到99.9%。此外,ZnAl-500复合材料在多个反应循环中表现出良好的稳定性。此外,自由基清除试验和电子自旋共振测量表明,超氧自由基和羟基自由基是O/ZnAl-500体系中的主要活性物种。而且,在单独臭氧氧化和O/ZnAl-500体系中分别检测到19种和10种转化产物,并进一步阐明了ATZ可能的降解途径。总体而言,ZnAl-500复合材料因其高催化臭氧化效率、稳定性和可重复使用性,可为污染物去除提供一种潜在的替代方案。

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