钴负载型磁石墨烯耦合过氧单硫酸盐去除橙红7分析
Analysis on the Removal of Acid Orange 7 by Magnetic Graphene-supported Cobalt and Peroxymonosulfate Coupling
作者：杨颖(四川大学 建筑与环境学院, 四川 成都 610065)；邓钦祖(中国市政工程西南设计研究总院, 四川 成都 610065)；王如梦(四川大学 建筑与环境学院, 四川 成都 610065)；张永丽(四川大学 建筑与环境学院, 四川 成都 610065)；郭洪光(四川大学 建筑与环境学院, 四川 成都 610065)；张鹏(四川大学 建筑与环境学院, 四川 成都 610065)；蒋玮炜(四川大学 建筑与环境学院, 四川 成都 610065)；孙泽宇(四川大学 建筑与环境学院, 四川 成都 610065)
Author：YANG Ying(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；DENG Qinzu(Southwest Municipal Eng. Design & Research Inst. of China, Chengdu 610065, China)；WANG Rumeng(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；ZHANG Yongli(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；GUO Hongguang(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；ZHANG Peng(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；JIANG Weiwei(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)；SUN Zeyu(College of Architecture & Environment, Sichuan Univ., Chengdu 610065, China)
收稿日期：2016-08-29 年卷（期）页码：2017,49(1):132-137
期刊名称：工程科学与技术
Journal Name：Advanced Engineering Sciences
关键字：磁石墨烯;过渡金属;硫酸自由基;橙红7;去除率
Key words：magnetic graphene;transition metal;sulfate radical;acid orange 7;removal rate
基金项目：国家自然科学基金资助项目（51508354）；中国博士后基金资助项目（2016M590888）；成都市科技局项目资助项目（2015-HM01-00502-SF）
中文摘要
为充分利用过渡金属对过氧单硫酸盐（PMS）的催化活性，同时解决残余金属所带来的水体二次污染问题，实现催化剂的重复利用，将磁性Fe3O4颗粒和Co负载在还原氧化石墨烯（RGO）表面合成新型多相复合磁性材料（CF-RGO），对比了PMS、RGO、CF-RGO、RGO/PMS、Co/PMS和CF-RGO/PMS等6种体系去除橙红7（AO7）的效果，并考察了不同初始pH、CF-RGO初始投量、AO7初始浓度对CF-RGO激活PMS去除水中AO7的影响。试验结果显示：PMS、RGO、CF-RGO和RGO/PMS体系基本不能去除水中AO7，而CF-RGO/PMS和Co/PMS体系则能有效去除AO7，且CF-RGO/PMS体系去除AO7的能力显著高于Co/PMS体系。对于CF-RGO/PMS体系，随着pH的增加，AO7的去除率先增大后减小，并在pH=5.0时达到最大去除率；CF-RGO初始投量对体系去除AO7的影响差异不大，总体呈正相关性；AO7初始浓度的不断增加会减弱体系的去除能力，从而降低AO7的去除率。同时，叔丁醇（TBA）和乙醇（ETOH）的投加证实了CF-RGO/PMS体系的自由基在pH=5.0时以硫酸自由基（·SO4-）为主，说明·SO4-对AO7的去除占主导作用。此外，重复使用该催化剂3次后发现其催化活性和稳定性均较好，Co、Fe等残留金属的检测结果也表明该催化剂对水体的二次污染极小。研究表明：CF-RGO作为催化剂可快速、高效地激活PMS去除水中AO7，且重复利用效果好、二次污染小；在pH=5.0，AO7、PMS初始浓度分别为0.03、0.2 mmol/L，CF-RGO初始投量为0.003 g的条件下，CF-RGO/PMS体系去除AO7效果最佳，去除率最高达95.8%。
英文摘要
Magnetic Fe3O4and Co were loaded on the face of reduced graphene oxide (RGO) to form newly multiphase composite magnetic materials (CF-RGO),taking the advantage of the ability of transition metals to activate peroxymonosulfate (PMS),and decreasing the secondary pollution of residual metal.The efficiency of PMS,RGO,CF-RGO,RGO/PMS,Co/PMS,and CF-RGO/PMS systems on removing acid orange 7 (AO7) were compared,and the effects of different initial pHs,CF-RGO dosages and AO7 concentraions on removal of AO7 were investigated by CF-RGO-activated PMS.Results suggested that AO7 could hardly be removed by PMS RGO,CF-RGO and RGO/PMS systems,while the systems of CF-RGO/PMS and Co/PMSPMS could remove efficiently,and the removal capacity of CFRGO/PMS system was apparently higher than Co/PMS system.For the system of CF-RGO/PMS,the removal efficiency of AO7 increased first and then decreased with the increase of pH,and the removal rate reached a maximum at pH=5.0.The effect of CF-RGO dosage on AO7 removal showed a positive correlation basically.The increase of AO7 initial concentration would reduce the removal capacity of system,with the decrease of the removal rate of AO7.The dosing of tertiary butanol (TBA) and ethyl alcohol (ETOH) confirmed that the major radical formed was sulfate radical (·SO4-) at pH=5.0,which suggested a major role of ·SO4-in degrading AO7. In addition,the catalytic activity and stability were good after using three times repeatedly.The investigation of residual Co and Fe showed that this kind of catalyst had little secondary pollution on water.The study indicated that CF-RGO could activate PMS quickly and remove AO7 efficiently as a catalyst,with good reutilization and little secondary pollution. On the conditions of pH of 5.0,initial concentrations of AO7 and PMS of 0.03 mmol/L and 0.2 mmol/L,and the dosage of CF-RGO of 0.003 g,CF-RGO PMS system could remove AO7 efficiently,with the maximum rate reaching 95.8%.
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