超声辅助制备的LaFeO_(3)/PS催化可见光芬顿降解盐酸四环素  

Study of the degradation of tetracycline by visible photo-Fenton catalyzed by ultrasound-assisted LaFeO_(3)/PS

作　　者：戈晓东 孟冠华 刘宝河 张林森 杨建华 程洛闻 GE Xiaodong;MENG Guanhua;LIU Baohe;ZHANG Linsen;YANG Jianhua;CHENG Luowen(School of Energy and Environment,Anhui University of Technology,Ma'anshan 234002,China)

机构地区：[1]安徽工业大学能源与环境学院,马鞍山234002

出　　处：《复合材料学报》2023年第1期255-269,共15页Acta Materiae Compositae Sinica

基　　金：安徽高校自然科学研究重点项目(KJ2017A065);2017年度高校优秀骨干青年人才国内外访学研修项目(gxfx2017019)。

摘　　要：粉末状LaFeO_(3)材料具有易团聚、分离困难等缺点,规模化应用中受到限制。聚苯乙烯树脂(PS)上沉积粉末状催化剂,弥补了以上粉末材料的不足。为此,本文采用超声辅助溶胶-凝胶和水热法,在PS上沉积了自组装形成的LaFeO_(3)凝胶微球,制得了LaFeO_(3)/PS催化剂,并对其结构和性能进行了系统的研究。LaFeO_(3)凝胶微球在PS上的分散分布使LaFeO_(3)的禁带宽度变宽,从而增加了氧化还原能力,并解决了催化剂团聚等问题,提高了LaFeO_(3)的光芬顿催化活性。在La∶Fe∶柠檬酸(CA)摩尔比=1∶1∶2、超声40 min、水热时间18 h、水热温度90℃、LaFeO_(3)起始剂/PS质量比=32∶1的制备条件制得的复合材料,在可见光下催化芬顿降解盐酸四环素(TC),TC的去除率可达96.51%(降解速率k=0.0160 min^(-1))。自由基捕获实验表明,·O_(2)^(−)是主要活性物种。结合捕获实验提出了TC的降解机制。通过LC/MS分析,得到了TC的降解路径。该技术提高了催化剂的稳定性,高效利用了太阳能,是一种很有前途的有机污染物降解技术。The powdered LaFeO_(3) material had shortcomings such as easy agglomeration and difficult separation,so it was limited in large-scale applications.The deposition of powdered catalysts in polystyrene resin(PS)made up for the above shortcomings of powdered materials.Therefore,in this study,the self-assembled LaFeO_(3) gel was deposited on the PS through ultrasound-assisted sol-gel and hydrothermal methods.The dispersion and distribution of LaFeO_(3) on PS broadens the forbidden band width of LaFeO_(3),improves its redox ability,solves the problem of agglomeration,and consequently improves its photo-Fenton catalytic activity.The LaFeO_(3)/PS composite prepared under the following experimental conditions shows the highest photocatalytic activity:La∶Fe∶Citric acid(CA)molar ratio=1∶1∶2,ultrasonic time 40 min,hydrothermal temperature 90℃,hydrothermal time 18 h,LaFeO_(3) initiator/polystyrene mass ratio=32∶1.The removal rate of tetracycline hydrochloride(TC)is up to 96.51%(rate of degradation k=0.0160 min^(-1))under visible light irradiation in the Fenton process catalyzed by LaFeO_(3)/PS.Free radical capture experiments show that·O_(2)^(−)is the main active species.According to the capture experiment,the degradation mechanism of TC was proposed.Through LC/MS analysis,the degradation path of TC was obtained.The photo-Fenton process catalyzed by LaFeO_(3)/PS is a promising technology for the degradation of organic pollutants due to the high stability of the catalyst and the efficient use of solar energy.

关 键 词：盐酸四环素 可见光芬顿 聚苯乙烯树脂 铁酸镧 催化降解 

分 类 号：TB333[一般工业技术—材料科学与工程]