可见光协同CuO高效活化过二硫酸盐降解四环素  

Visible light-assisted copper oxide efficient activation of peroxydisulfate for tetracycline degradation

作　　者：李世嘉 庞尔楠[2] LI Shi-jia;PANG Er-nan(Institute of Traffic Engineering,Shanxi Vocational University of Engineering Science and Technology,Taiyuan 030619,China;School of Materials Science and Engineering,North University of China,Taiyuan 030051,China)

机构地区：[1]山西工程科技职业大学交通工程学院,山西太原030619 [2]中北大学材料科学与工程学院,山西太原030051

出　　处：《中国环境科学》2025年第3期1298-1307,共10页China Environmental Science

基　　金：山西工程科技职业大学校科技创新基金(202229);山西工程科技职业大学横向项目(2023HX021)。

摘　　要：基于CuO活化过二硫酸盐(PDS)的高级氧化技术已成为降解有机污染物的有效策略之一,但仍存在活化PDS效率较低、Cu O比表面积小和Cu(Ⅱ)/Cu(Ⅱ)转换效率低等问题,本文采用低温水热-煅烧两步法成功制备了具有高催化活性和大比表面积(32.8m^(2)/g)的片状氧化铜(CCB-300).通过X射线粉末衍射仪(XRD)、比表面及孔径分析仪(BET)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱仪(XPS)等表征分析了CCB-300的晶体结构、形貌和元素组成等理化性质.研究其在可见光(Vis)协同作用下活化PDS降解四环素(TC)的性能.在不调整初始p H值、催化剂用量为0.05g/L、PDS浓度为0.5mmol/L、TC浓度为50mg/L条件下,反应60min后TC去除率达到96.9%.电子顺磁共振谱(EPR)和自由基淬灭实验表明非自由基途径产生的^(1)O_(2)和自由基途径生成的SO_(4)^(i-)和·OH均参与了降解反应.紫外可见漫反射光谱及光电化学测试结果表明CCB-300具有优异的可见光吸收能力和电荷传输性能,在可见光激发下产生的光生电子加速了Cu(Ⅱ)/Cu(Ⅱ)的氧化还原循环,促进了PDS向SO_(4)^(i-)和·OH的转化,从而进一步提高其降解TC的效率.重复性实验结果表明CCB-300具有较好的重复使用性和稳定性.最后,提出了CCB-300协同可见光活化PDS降解TC的可能反应机理.本研究为可见光协同非均相催化剂活化过硫酸盐降解四环素类抗生素提供一种新的方法和思路.The advanced oxidation technology of persulfate (PDS) activation by Cu O have been hotly sought as one of the effective strategies for degrading organic pollutants in water.However,there are still certain issues such as the low efficiency of PDS activation,the small specific surface area of Cu O,and the low conversion efficiency of Cu(II)/Cu(I).Herein,the flake copper oxide(CCB-300) with high activity and large specific surface area (32.8m^(2)/g) was successfully synthesized through a two-step hydrothermal-calcination method.Multiple characterization analysis,such as X-ray powder diffractometry (XRD),N_(2) adsorption-desorption analysis,Scanning electron microscopy (SEM),Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS),were utilized to analyze crystal structure,morphology and element composition of CCB-300.Furthermore,the performance of the CCB-300 for degradation of tetracycline (TC) via peroxydisulfate activation under visible light(Vis) was investigated.The findings revealed that the TC removal rate reached 96.9% within 60 minutes under the circumstances of 0.05g/L CCB-300,0.5 mmol/L PDS,50mg/L TC and unadjusted initial p H.Electron paramagnetic resonance spectroscopy (EPR) and radical quenching experiments indicated that both ^(1)O_(2) produced by the non-radical pathways and SO_(4)^(i-)and·OH generated via the radical pathways were involved in the degradation reaction.Ultraviolet-visible diffuse reflectance spectroscopy and photoelectrochemical tests confirmed that CCB-300 exhibited excellent visible light absorption capacity and charge transfer performance.The photogenerated electrons excited by visible light accelerate the redox cycle of Cu(II)/Cu(I),facilitating the conversion of PDS to SO_(4)^(i-)and·OH,and further enhancing the efficiency of TC degradation.The repeatable experiments demonstrated that CCB-300 exhibited favorable reusability and stability.Finally,the possible reaction mechanism was proposed.This study provided a novel method for tetracycline degradation

关 键 词：高级氧化法 氧化铜 可见光 过二硫酸盐 四环素 

分 类 号：X703[环境科学与工程—环境工程]