悬浮填料负载氧化铁Fenton流化床法对腈纶废水的处理
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摘要
以悬浮填料为基体,采用循环浸泡法将铁氧化物负载到填料表面制备出具有催化能力的悬浮填料载体,用于Fenton流化床工艺处理腈纶废水的研究,通过正交实验验证悬浮填料投加率、通气量、H_2O_2浓度和Fe~(2+)投加量对COD降解效率的影响。实验结果表明:悬浮填料负载氧化铁后密度由0.9627g/cm~3略增至1.0216g/cm~3,填料表面铁氧化物覆盖均匀,载体表面负载的氧化物中铁元素含量达到47.17%;正交实验及模拟结果表明各因素影响处理效果的主次顺序为H_2O_2>Fe~(2+)>通气量>填料投加率,以及当实验最佳参数条件为:H2O2浓度为75mmol/L,Fe~(2+)投加量为3.25mmol/L,通气量0.25m~3/h,悬浮填料载体投加率为40%时,COD、BOD_5、NH_3-N、TOC和氰化物的去除率分别为77.8%、44%、76%、70.6%和70%;填料载体循环使用5次后,降解120min,COD去除率从77.8%降到70.4%,性能稳定,可重复利用。
Based on suspended filler as the substrate, iron oxide was loaded onto the surface of the packing material by cyclic immersion method to prepare a catalytic packing material, which was used for the advanced treatment of acrylic fiber wastewater by Fenton fluidized bed process. The effect of addition rate of suspended filler, the amount of ventilation, the concentration of H_2O_2 and the dosage of Fe~(2+) on the degradation efficiency of COD was studied by orthogonal test. The experimental results showed that the density of suspended filler coated with iron oxide slightly increased from 0.9627 g/cm3 to 1.0216 g/cm~3, and it was evenly for the iron oxide on the surface of filler with 47.17% of iron content. The results of orthogonal test and simulation showed that the factors influenced order processing effect was H_2O_2>Fe~(2+)>ventilatory capacity>filling rate of catalytic carriers. The optimum parameters conditions were that the concentration of H_2O_2 was 75 mmol/L, Fe~(2+) dosage was 3.25 mmol/L, volume 0.25 m3/h, suspended carrier dosage rate of 40%, the COD, BOD_5, NH_3-N, TOC and cyanide were 77.8%, 44%, 76%, 70.6% and 70%, respectively. After 5 cycles of packing carrier recycling with 120 min of reaction time, the COD removal efficiencies were reduced from the 77.8% to 70.4% that proved it could be reused with stable performance.
Based on suspended filler as the substrate, iron oxide was loaded onto the surface of the packing material by cyclic immersion method to prepare a catalytic packing material, which was used for the advanced treatment of acrylic fiber wastewater by Fenton fluidized bed process. The effect of addition rate of suspended filler, the amount of ventilation, the concentration of H_2O_2 and the dosage of Fe~(2+) on the degradation efficiency of COD was studied by orthogonal test. The experimental results showed that the density of suspended filler coated with iron oxide slightly increased from 0.9627 g/cm3 to 1.0216 g/cm~3, and it was evenly for the iron oxide on the surface of filler with 47.17% of iron content. The results of orthogonal test and simulation showed that the factors influenced order processing effect was H_2O_2>Fe~(2+)>ventilatory capacity>filling rate of catalytic carriers. The optimum parameters conditions were that the concentration of H_2O_2 was 75 mmol/L, Fe~(2+) dosage was 3.25 mmol/L, volume 0.25 m3/h, suspended carrier dosage rate of 40%, the COD, BOD_5, NH_3-N, TOC and cyanide were 77.8%, 44%, 76%, 70.6% and 70%, respectively. After 5 cycles of packing carrier recycling with 120 min of reaction time, the COD removal efficiencies were reduced from the 77.8% to 70.4% that proved it could be reused with stable performance.
引文
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[16]颜金利,汪晓军,黎玉香,等.负载氧化铁石英砂用于Fenton-流化床体系处理印染废水的研究[J].水处理技术,2012,38(2):76-78.YAN J L,WANG X J,LI Y X,et al.Study on dying wastewater treatment by Fenton-fluidized bed process with iron oxide coated sand[J].Technology of Water Treatment,2012,38(2):76-78.
[17]BANDARA J,MORRISON C,KIWI J,et al.Degradation/decoloration of concentrated solutions of OrangeⅡ.Kinetics and quantum yield for sunlight induced reactions via Fenton type reagents[J].Journal of Photochemistry and Photobiology A:Chemistry,1996,99(1):57-66.
[18]MATIRA E M,CHEN T C,LU M C,et al.Degradation of dimethyl sulfoxide through fluidized-bed Fenton process[J].Journal of Hazardous Materials,2015,300(30):218-226.
[2]王亚娥,白帆,赵炜,等.我国腈纶废水物化处理技术研究进展[J].水处理技术,2017(3):1-3.WANG Y E,BAI F,ZHAO W,et al.Research progress on physicochemical treatment of acrylic fiber wastewater in China[J].Technology of Water Treatment,2017(3):1-3.
[3]马克存,邵正宏,杜龙弟,等.Fenton氧化-接触氧化工艺处理聚合废水的试验[J].化工进展,2011,30(s1):859-863.MA K C,SHAO Z H,DU L D,et al.Study on Fenton-contact oxidation process for polymerization wastewater treatment[J].Chemical Industry and Engineering Progress,2011,30(s1):859-863.
[4]张潇逸,蒋进元,周岳溪,等.响应曲面法优化聚硅酸铁混凝剂处理腈纶废水[J].环境工程学报,2017,11(2):721-726.ZHANG X Y,JIANG J Y,ZHOU Y X,et al.Optimization on poly-silicic-ferric congulant treatment of acrylic fiber wastewater using response surface methodology[J].Chinese Journal of Environmental Engineering,2017,11(2):721-726.
[5]CAI M,SU J,ZHU Y,et al.Decolorization of azo dyes Orange Gusing hydrodynamic cavitation coupled with heterogeneous Fenton process[J].Ultrasonics Sonochemistry,2016,28:300-302.
[6]叶友胜,万新军,程乐华,等.微电解-Fenton-BAF组合工艺深度处理腈纶废水[J].工业水处理,2017,37(1):65-68.YE Y S,WAN X J,CHENG Y H,et al.Advanced treatment of acrylic fiber wastewater by the combined process microelectrolysisFenton-biological aerated filter[J].Industrial Water Treatment,2017,37(1):65-68.
[7]JING X,LONG Y,SHEN D,et al.Optimization of Fenton treatment process for degradation of refractory organics in pre-coagulated leachate membrane concentrates[J].Journal of Hazardous Materials,2017,323(B):674-680.
[8]LI W H,LI G W,SEBASTIEN R,et al.Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst[J].Journal of Hazardous Materials,2016,302:458-67.
[9]范东,丁丽丽,耿金菊,等.Fenton流化床陶瓷膜反应器处理造纸废水的膜污染与清洗[J].化工环保,2017,37(2):200-206.FAN D,DING L L,GENG J J,et al.Membrane fouling and cleaning regeneration of Fenton fluidized bed-ceramic membrane reactor for treatment of papermaking wastewater[J].Environmental Protection of Chemical Industry,2017,37(2):200-206.
[10]FAN D,DING L L,HUI H,et al.Fluidized-bed Fenton coupled with ceramic membrane separation for advanced treatment of flax wastewater[J].Journal of Hazardous Materials,2017,340:390-398.
[11]ANOTAI J,SAKULKITTIMASAK P,BOONRATTANAKIJ N,et al.Kinetics of nitrobenzene oxidation and iron crystallization in fluidized-bed Fenton process[J].Journal of Hazardous Materials,2009,165(3):874-880.
[12]POURAN S R,RAMAN A A A,WAN M A W D.Review on the application of modified iron oxides as heterogeneous catalysts in Fenton reactions[J].Journal of Cleaner Production,2014,64:24-35.
[13]LO S L,JENG H T,LAI C H.Characteristics and adsorption properties of iron-coated sand[J].Water Science and Technology,1997,35(7):63-70.
[14]LI S,ZHANG G,WANG P,et al.Microwave-enhanced Mn-Fenton process for the removal of BPA in water[J].Chemical Engineering Journal,2016,294:371-379.
[15]KASIRI M B,ALEBOYEH H,ALEBOYEH A.Degradation of Acid Blue 74 using Fe-ZSM5 zeolite as a heterogeneous photo-Fenton catalyst[J].Applied Catalysis B:Environmental,2008,84(1):9-15.
[16]颜金利,汪晓军,黎玉香,等.负载氧化铁石英砂用于Fenton-流化床体系处理印染废水的研究[J].水处理技术,2012,38(2):76-78.YAN J L,WANG X J,LI Y X,et al.Study on dying wastewater treatment by Fenton-fluidized bed process with iron oxide coated sand[J].Technology of Water Treatment,2012,38(2):76-78.
[17]BANDARA J,MORRISON C,KIWI J,et al.Degradation/decoloration of concentrated solutions of OrangeⅡ.Kinetics and quantum yield for sunlight induced reactions via Fenton type reagents[J].Journal of Photochemistry and Photobiology A:Chemistry,1996,99(1):57-66.
[18]MATIRA E M,CHEN T C,LU M C,et al.Degradation of dimethyl sulfoxide through fluidized-bed Fenton process[J].Journal of Hazardous Materials,2015,300(30):218-226.