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Fe/Cu双金属活化过一硫酸盐降解四环素的机制
摘要点击 3711  全文点击 1256  投稿时间:2017-09-26  修订日期:2017-12-25
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中文关键词  Fe/Cu双金属  非均相催化  过一硫酸盐  四环素(TC)  降解机制
英文关键词  Fe/Cu oxides  heterogeneous catalysis  peroxymonosulfate  tetracycline(TC)  degradation mechanism
作者单位E-mail
李晶 中国地质大学(武汉)环境学院, 武汉 430074 1522283346@qq.com 
鲍建国 中国地质大学(武汉)环境学院, 武汉 430074 bjianguo@cug.edu.cn 
杜江坤 中国地质大学(武汉)环境学院, 武汉 430074  
冷一非 中国地质大学(武汉)环境学院, 武汉 430074  
孔淑琼 中国地质大学(武汉)环境学院, 武汉 430074  
中文摘要
      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pH的提高,TC降解效率明显增加;无机阴离子(H2PO4-、HCO3-、Cl-)均对TC的降解有不同程度的促进作用,而NO3-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.
英文摘要
      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 pH of the coupled Fe-Cu-400/PMS system. Anions including H2PO4-, HCO3-, and Cl- promoted TC degradation, whereas NO3- 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.

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