引用本文:张晓薇,甘国强.Fe3O4/CeO2复合材料催化降解橙黄G的效能及降解途径[J].环境科学研究,2017,30(9):1455-1463.
ZHANG Xiaowei,GAN Guoqiang.OG Degradation Efficiency and Pathway Using Fe3O4/CeO2 Composite[J].Reserrch of Environmental Science,2017,30(9):1455-1463.]
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Fe3O4/CeO2复合材料催化降解橙黄G的效能及降解途径
张晓薇1,2, 甘国强3
1.辽宁工程技术大学环境科学与工程学院, 辽宁 阜新 123000 ;2.东北大学资源与土木工程学院, 辽宁 沈阳 110819 ;3.中国科学院沈阳应用生态研究所, 辽宁 沈阳 110016
摘要:
为研究磁性纳米Fe3O4/CeO2复合材料在高浓度难降解有机废水处理中的应用,利用共沉淀法制备Fe3O4/CeO2复合材料,并将其作为非均相类Fenton催化剂降解橙黄G染料废水,利用单因素法优化出最佳降解工艺,同时利用TOF-MS/MS(飞行时间质谱)检测降解中间产物,推测出可能降解途径. 结果表明,当Ce/Fe为1∶1(质量比)时制备的Fe3O4/CeO2复合材料催化效果最佳. 最佳降解工艺条件:初始pH为2.0,温度为30 ℃,H2O2投加量为30 mmol/L,Fe3O4/CeO2复合材料的投加量为2.0 g/L,初始ρ(橙黄G)为50 mg/L. 在最佳降解工艺条件下反应120 min后,橙黄G去除率为96.2%,TOC去除率为65.0%,Fe3O4/CeO2复合材料至少可重复利用6次. 研究显示,橙黄G降解主要有三条可能的降解途径,包括偶氮键断裂、偶氮键与苯环断开、脱磺酸基、羟基化以及开环等过程,共检测出八种可能的降解中间产物,主要有苯胺、苯酚、萘酚以及羧酸等.
关键词:  Fe3O4/CeO2  橙黄G  类芬顿法  降解效能  降解途径
DOI:
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基金项目:辽宁省教育厅项目(L2014143)
OG Degradation Efficiency and Pathway Using Fe3O4/CeO2 Composite
ZHANG Xiaowei1,2, GAN Guoqiang3
1.College of Environmental Science and Technology, Liaoning Technical University, Fuxin 123000, China ;2.College of Resources and Civil Engineering, Northeastern University, Shenyang 110819, China ;3.Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China
Abstract:
Abstract: In recent years, environmental pollution has become more and more serious. High concentration refractory organic wastewater is highly toxic and difficult to decompose. Therefore, developing a new high efficient wastewater treatment process is extremely urgent. Fe3O4/CeO2 composite was synthesized using the co-precipitation method. The composite was used for the degradation of Orange G as Fenton-like heterogeneous catalyst. The process parameters were investigated by the single factor experiment. The degradation intermediate products were determined by TOF-MS/MS. The possible degradation pathway of OG by heterogeneous Fenton-like process was attained. The results indicated that the optimal conditions were pH value 2.0, H2O2 concentration 30 mmol/L, initial dye concentration 50 mg/L, catalyst dosage 2.0 g/L and temperature 30 °C. Under the optimal conditions, the degradation percentage of OG was 96.2% within 120 min, and the TOC removal rate was 65.0%. Mass spectrometry analysis results showed that the OG degradation was mainly through three possible degradation pathways, including the process of azo bond rupture, desulfonation, hydroxylation and ring opening process. Eight possible degradation intermediate productions were measured, including aniline, phenol, naphthol and carboxylic acid.
Key words:  Fe3O4/CeO2  Orange G  Fenton-like  degradation efficiency  degradation pathway