Fe/Cu双金属活化过一硫酸盐降解四环素的机制  

Degradation Mechanism of Tetracycline Using Fe/Cu Oxides as Heterogeneous Activators of Peroxymonosulfate

作　　者：李晶 鲍建国[1] 杜江坤[1] 冷一非[1] 孔淑琼[1] LI Jing;BAO Jian-guo;DU Jiang-kun;LENG Yi-fei;KONG Shu-qiong(School of Environmental Studies, China University of Geoseienees, Wuhan 430074, Chin)

机构地区：[1]中国地质大学(武汉)环境学院,武汉430074

出　　处：《环境科学》2018年第7期3203-3211,共9页Environmental Science

基　　金：国家自然科学基金项目(41373083);国家自然科学基金国际(地区)合作与交流项目(41611130185)

摘　　要：利用共沉淀法成功制备出绿色、高效、具有磁性的介孔Fe/Cu双金属非均相催化剂(Fe-Cu-400),通过X射线衍射仪(XRD)、比表面积测试仪(BET)、场发射扫描电镜(FESEM)及X射线能谱仪(EDS)等表征手段对催化剂的结构、形貌等进行分析,并用制备的Fe-Cu-400催化剂活化过一硫酸盐(PMS)降解四环素(TC),研究了不同反应条件对降解效果的影响.结果表明Fe-Cu-400/PMS体系具有较好的降解效果,随着PMS浓度和初始p H的提高,TC降解效率明显增加;无机阴离子(H2PO-4、HCO-3、Cl-)均对TC的降解有不同程度的促进作用,而NO-3对TC的降解则表现出较弱的抑制作用.Fe-Cu-400在循环使用5次后仍具有较好活化性能.通过自由基抑制实验和XPS测试分析了Fe-Cu-400/PMS体系的活化机制和分解产生的主要活性物种.通过LC-MS结合TOC分析,推测出TC经水解、脱甲基、脱羟基和脱氨基作用达到降解和矿化.A green,highly efficient,and porous copper-ferrite heterogeneous catalyst（ Fe-Cu-400） with good magnetism was synthesized via a coprecipitation method. The catalysts were characterized using XRD,BET,FESEM,and EDS. The performance of Fe-Cu-400 as a catalyst was evaluated by activating peroxymonosulfate（ PMS） for degradation of tetracycline（ TC） in aqueous solution and investigating the influence of several water parameters. The Fe-Cu-400/PMS system showed a greater TC degradation ability,and the degradation rate of TC was enhanced with an increase in the PMS concentration and the initial p H of the coupled Fe-Cu-400/PMS system. Anions including H2PO4 ～-,HCO3 ～-,and Cl ～-promoted TC degradation,whereas NO-3 showed a low inhibitory influence. In addition,Fe-Cu-400 exhibited excellent reusability towards activating PMS for TC degradation after five runs of tests. Possible mechanisms of the activation of PMS by Fe-Cu-400 and the main reactive species were proposed based on radical identification tests and XPS analysis. Furthermore,a potential degradation pathway was proposed that included hydrolysis and sequential removal of N-methyl,hydroxyl,and amine functional groups according to the results of LC-MS and TOC detections.

关 键 词：Fe/Cu双金属 非均相催化 过一硫酸盐 四环素(TC) 降解机制 

分 类 号：X703.1[环境科学与工程—环境工程]