铜锌铝水滑石制备及活化过氧单硫酸盐对水中土霉素降解性能  

Synthesis of CuZnAl layered double hydroxide and degradation of oxytetracycline in water by activated peroxymonosulfate

作　　者：闫旭 李旭光 宋雯 朱宝存 YAN Xu;LI Xuguang;SONG Wen;ZHU Baocun(School of Water Conservancy and Environment,University of Jinan,Jinan 250022,China)

机构地区：[1]济南大学水利与环境学院,山东济南250022

出　　处：《中国粉体技术》2025年第2期59-70,共12页China Powder Science and Technology

基　　金：国家自然科学基金项目,编号:22206057。

摘　　要：【目的】利用水滑石(layered double hydroxide,LDH)粉体材料催化能力强、结构可调、制备难度低、分散性良好等优点及其在高级氧化技术中的应用潜能,研究铜锌铝水滑石(CuZnAl-LDH)的制备方法,以及活化过氧单硫酸盐(peroxymonosulfate,PMS)降解水中难降解污染物的性能。【方法】采用共沉淀法制备并表征CuZnAl-LDH-x;选择水中土霉素(oxytetracycline,OTC)进行降解实验,确定CuZnAl-LDH-x的较优制备条件,研究水化学条件对催化体系中OTC降解率的影响;探究CuZnAl-LDH-x活化PMS的催化机制和降解途径;在不同水体样本中进行催化体系的实际应用性能评估。【结果】制得的CuZnAl-LDH-x具有致密的六边形层状结构;当Cu、Zn、Al元素的物质的量比为5∶1∶2时,CuZnAl-LDH-1-PMS体系对OTC降解效果最佳;在CuZnAl-LDH-1-PMS体系初始pH为6、CuZnAl-LDH-1质量浓度为20 mg/L、PMS浓度为1.0 mmol/L、OTC质量浓度为10 mg/L时降解效果最佳,降解时间为40 min时降解率高达96.25%;CuZnAl-LDH-1-PMS体系具有良好的抗干扰性,pH、无机阴离子和腐殖酸等因素的影响较小;在CuZnAl-LDH-1-PMS体系降解OTC过程中存在自由基和非自由基2种途径,其中羟基自由基对降解率的贡献最大;CuZnAl-LDH-1-PMS体系在4种实际水体中对OTC的降解率仍能达到74%~95%。【结论】CuZnAl-LDH-x制备过程简便,具备高效活化PMS并降解抗生素类污染物的能力,可以作为基于过硫酸盐的高级氧化水处理技术的催化剂。Objective Layered double hydroxide(LDH)is a widely available and cost-effective material known for its unique structure,large specific surface area,controllable interlayer ion exchange,and stability.LDH is capable of activating peroxymonosulfate(PMS)in advanced oxidation processes,offering advantages such as high efficiency,abundant surface hydroxyl groups,and a range of active species.In this study,CuZnAl-LDH was synthesized using the co-precipitation method.The structure and properties of CuZnAl-LDH were characterized using scanning electron microscopy(SEM),high-resolution transmission electron microscopy(HRTEM),X-ray diffraction(XRD),and Fourier-transform infrared(FTIR)spectroscopy.The synthesis of CuZnAl-LDH was explored leveraging the favorable attributes of LDHs,such as robust catalytic activity,customizable structure,simple synthesis process,excellent dispersibility,and potential application in advanced oxidation processes.Furthermore,the effectiveness of activated PMS in degrading recalcitrant pollutants in water was investigated,highlighting the potential of CuZnAl-LDH as a catalyst in advanced oxidation applications.Methods The CuZnAl-LDH-x(x=1,2,…,5)was prepared by the co-precipitation method using CuCl2·2H2O,ZnCl2 and AlCl3·6H2O at various molar ratios of Cu,Zn,and Al elements.The obtained powder was characterized by SEM,FTIR and XRD.The degradation experiments in CuZnAl-LDH-PMS system were conducted using OTC as a typical antibiotic in water.The experimental conditions,including the molar ratio of Cu,Zn,and Al elements,catalyst and PMS dosage,solution pH,and environmental factors such as inorganic anions and humic acid,were optimized.The mechanisms were also investigated by a quenching experiment and electron paramagnetic resonance(EPR)spectroscopy,and high performance liquid chromatography-mass spectrometry(HPLC-MS)was used to determine the degradation products of OTC in CuZnAl-LDH-1-PMS system.With distilled water as a control,tap water,Yellow River water,a city landscape lake water,and a campu

关 键 词：铜锌铝水滑石 活化过氧单硫酸盐 土霉素 降解 高级氧化水处理技术 

分 类 号：TB4[一般工业技术] TB34