构建电促铁还原型芬顿氧化法降解水中4-硝基酚
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摘要
以钛基氧化物涂层材料(Ti/SnO_2-Sb_2O_5-IrO_2)为阳极,碳纳米管修饰的石墨材料(GE-CNT)为阴极构建电化学系统,促进芬顿反应过程中Fe~(3+)还原,从而减少芬顿氧化法中铁盐加量和铁泥产生量。研究表明:GE-CNT具有良好的还原Fe~(3+)性能,其优化的阴极还原电位约为0.30 V(vs.Ag/AgCl),该电位下反应120 min时Fe~(3+)还原率达到85.7%。以Fe~(3+)为催化剂降解4-硝基酚的结果,证实了电化学还原Fe~(3+)促进芬顿反应的有效性。对比考察了电促铁还原型芬顿氧化法与普通芬顿氧化法降解4-硝基酚的效果,优化的条件下两者可获得近似的降解效果,但前者优化的H_2O_2与Fe~(2+)摩尔比为40∶1,而后者为20∶1。因此,相对于普通芬顿氧化法,电促铁还原型芬顿氧化法可显著减少芬顿反应初始Fe~(2+)投加量。
The electrochemical system using the Ti-based oxide material(Ti/SnO_2-Sb_2O_5-IrO_2) as anode and the graphite modified with carbon nano-tube(GE-CNT) as cathode was developed to enhance the reduction of Fe~(3+ )in Fenton reactions, for the purposes of decreasing the ferric salt dosage and the iron sludge production. The results show that GE-CNT cathode has the high-performance for the reduction of Fe~(3+) at the optimum potential of 0.30 V(Ag/AgCl), and in this case the reduction ratio is 85.7% by the reaction of 120 min. The electrochemical reduction of Fe~(3+) can enhance Fenton reactions confirmed by the 4-nitrophenol degradation results obtained with Fe~(3+ )catalyst. The performance of 4-nitrophenol degradation was investigated comparatively by the Fenton oxidation with electrochemical reduction of Fe~(3+) and the traditional Fenton oxidation. The results show that the two oxidation processes can present an approximate degradation performance. However, for the former process the optimum mole ratio of H_2O_2/Fe~(2+) was 40 ∶1 while it was 20 ∶1 for the latter process. Therefore, the presented new Fenton oxidation process with electrochemical reduction can obviously decrease the initial dosage of Fe~(2+).
The electrochemical system using the Ti-based oxide material(Ti/SnO_2-Sb_2O_5-IrO_2) as anode and the graphite modified with carbon nano-tube(GE-CNT) as cathode was developed to enhance the reduction of Fe~(3+ )in Fenton reactions, for the purposes of decreasing the ferric salt dosage and the iron sludge production. The results show that GE-CNT cathode has the high-performance for the reduction of Fe~(3+) at the optimum potential of 0.30 V(Ag/AgCl), and in this case the reduction ratio is 85.7% by the reaction of 120 min. The electrochemical reduction of Fe~(3+) can enhance Fenton reactions confirmed by the 4-nitrophenol degradation results obtained with Fe~(3+ )catalyst. The performance of 4-nitrophenol degradation was investigated comparatively by the Fenton oxidation with electrochemical reduction of Fe~(3+) and the traditional Fenton oxidation. The results show that the two oxidation processes can present an approximate degradation performance. However, for the former process the optimum mole ratio of H_2O_2/Fe~(2+) was 40 ∶1 while it was 20 ∶1 for the latter process. Therefore, the presented new Fenton oxidation process with electrochemical reduction can obviously decrease the initial dosage of Fe~(2+).
引文
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[2] FENTON H J H.Oxidation of tartaric acid in presence of iron [J].Journal of the Chemical Society Transactions,1894,65:889-910.
[3] LI Y F,GUAN Y Z,TAO C C.Influenc-ing factors research of phenol wastewater tre-atment by cathode electro-Fenton method[C].Computational Intelligence and Industrial Application (PACIIA),2011,224:726-733.
[4] HOIGNE J.Inter-calibration of OH radicalsources and water quality parameters[J].Water Science and Technology,1997,35(4):1-8.
[5] 吴中杰,刘国强,张燕,等.类芬顿法脱除高盐废水中有机物工艺研究[J].化学工程,2017,45(5):15-18.
[6] FAN Z L,HUJ Y,AN W,et al.Detectionand occurrence of chlorinated byproducts of bisphenol A,nonyphneol,andestrogens in drink-ing water of China comparison to the parentcompounds[J].Environmental Science and Te-chnology,2013,47(19):10841-10850.
[7] LI F B,CHEN J J,LIU C S,et al.Effe-ct of iron oxides and carboxylic acids on photochemical degradation of bisphenol A[J].Biology & Fertility of Soils,2006,42(5):409-417.
[8] NGUYEN T D,PHAN N H,DO M H,et al.Magnetic Fe2MO4 (M:Fe,Mn) activated carbons:fabrication,characterization and heterogeneous Fenton oxidation of methyl orange[J].Journal of Hazardous Materials,2011,185(2):653-661.
[9] 周骏,肖九花,方长玲,等.UV/PMS体系硝基氯酚降解动力学及机理研究[J].中国环境科学,2016,36(1):66-73.
[10] YIN C,CAI J J,GAO L F,et al.Highly efficient degradation of 4-nitrophenol over the catalyst of Mn2O3/ AC by microwave catalytic oxidation degradation method[J].Journal of Hazardous Materials,2016,305:15-20.
[11] CHU Y Y,WANG W J,WANG M.Anodic oxidation process for the degradation of 2,4-dichlorophenol in aqueous solution and the enhancement of biodegradability[J].Journal of Hazardous Materials,2010,180(1):247-252.
[12] 褚衍洋,王蒙.钛基氧化物电极导致的H2O2分解及其对苯胺氧化的影响[J].化工学报,2010,61(3):761-766.
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