Epsilon-MnO_(2)/MnFe_(2)O_(4)复合催化剂活化过一硫酸盐降解水中四环素的研究  

Catalytic Degradation of Tetracycline in Water by Activation of Peroxymonosulfate Using Epsilon-MnO_(2)/MnFe_(2)O_(4) as Composite Catalyst

作　　者：李晓燕 张国珍[1] LI Xiaoyan;ZHANG Guozhen(School of Environment and Municipal Engineering,Lanzhou Jiaotong University,Lanzhou 730070,China;School of Civil Engineering,Lanzhou University of Technology,Lanzhou 730050,China)

机构地区：[1]兰州交通大学环境与市政工程学院,兰州730070 [2]兰州理工大学土木工程学院,兰州730070

出　　处：《兰州交通大学学报》2024年第6期144-154,164,共12页Journal of Lanzhou Jiaotong University

基　　金：甘肃省科技厅自然科学基金(22JR5RA306);兰州交通大学重大科技成果培育项目(2022CG07)。

摘　　要：开发高效、可持续利用的催化剂是过硫酸盐高级氧化技术发展的重点。将铁锰尖晶石MnFe_(2)O_(4)与ε-MnO_(2)复合制备ε-MnO_(2)/MnFe_(2)O_(4)复合催化剂,利用XRD、SEM、FTIR和XPS等方法对ε-MnO_(2)/MnFe_(2)O_(4)的微观结构和形貌进行表征,并将其作为过一硫酸盐(PMS)催化剂来探究对四环素(TC,10 mg/L)的催化降解性能。结果表明:在催化剂投加0.1 g/L,PMS用量为0.05 g/L,25℃,pH不做调整时,90 min内对四环素的催化降解达到90.4%。实验经5次循环后TC的降解效率为76.3%,说明催化剂有较好的循环稳定性。自由基捕获实验表明降解涉及活性氧物种有:催化剂表面-OH,SO_(4^(·))^(-),·OH,O_(2^(·))^(-)和^(1)O_(2),其中催化剂表面-OH基团作起主导作用。研究制备的催化剂活化PMS对水中的抗生素有较好去除效能,具备应用潜力。Exploring efficient and sustainable catalysts is the focus of the development of persulfate advanced oxidation process.Epsilon-MnO_(2)/MnFe_(2)O_(4) complex was synthesized with Fe-Mn spinel MnFe_(2)O_(4) and ε-MnO_(2),the microstructure and morphology were characterized by XRD,SEM,FTIR and XPS.The catalytic degradation performance of ε-MnO_(2)/MnFe_(2)O_(4) was investigated by activating peroxymonosulfate(PMS)as a catalyst to degrade tetracycline(TC).The results showed that the catalytic degradation of TC could reach 90.4% in 90 min when 0.1 g/L catalyst was added,PMS dosage was 0.05 g/L,pH was not adjusted and temperature was 25 ℃.After 5 cycles of experiments,the degradation efficiency of ε-MnO_(2)/MnFe_(2)O_(4) activated PMS for TC was still 76.3%,which indicated that the catalyst had good cycle stability.The free radical capture experiments showed that a variety of reactive oxygen species co-contributed to the degradation of TC,such as-OH on the catalyst surface,SO_(4~·)^(-),·OH,O_(2~·)^(-) and ~1O_(2),in which the-OH group on the catalyst surface played a leading role.The prepared catalyst activated PMS had good removal efficiency for antibiotics in water,and therefore had potential for application.

关 键 词：ε-MnO_(2)/MnFe_(2)O_(4) 过一硫酸盐 催化降解 四环素 

分 类 号：X522[环境科学与工程—环境工程]