新型光催化超滤膜反应器降解4BS偶氮染料
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摘要
偶氮染料多含有苯环或萘环,降解不彻底会生成致癌致畸的苯胺类化合物,排放到环境中会产生巨大的危害。本实验采用悬浮光催化-超滤膜反应器处理偶氮染料直接耐酸大红4BS,系统地研究了溶液pH值、TiO_2和4BS浓度对光催化过程的影响以及进水流速、操作时间对PAN700和PVDF700两种超滤膜分离TiO_2过程的影响,得出悬浮光催化-超滤膜反应器的最佳操作条件。
     实验结果表明,pH为5.5时,TiO_2对4BS的吸附性最好,吸附过程符合Langmuir等温吸附规律。在UV=100W、T=20℃、染料初始浓度为50mg·L~(-1)以及催化剂TiO_2浓度为1.0g·L~(-1)的最佳光催化操作条件下反应60min后,染料4BS脱色率可达到97.9%,染料矿化速率与脱色率基本一致。超滤膜回收TiO_2的过程中,随着进水流速增加,产水通量增加,出水水质维持稳定;且PAN700比PVDF700性能更好,其出水浊度更低,产水通量更大。PAN700膜在0.12MPa、40L·h~(-1)的进水流速下连续运行120min后,通量仅衰减28%,为214.00L·m~(-2)h~(-1)。通过滤饼模型计算分离过程的污染常数β值表明,PAN700比PVDF700膜更适合用于耦合分离过程。
Azo dyes usually compose of aromatic or naphthalene rings which can not be degraded completely by conventional technologies.The discharge of incompletely degraded azo dyes wastewater would easily lead to tremendous danger because of its carcinogenic and teratogenic to aquatic lives and human being.Performance of novel slurry photocatalytic ultrafiltration membrane reactor on degradation of direct scarlet 4BS in dying wastewater was studied in this paper.Influence of operating parameters such as pH value,dose of titanium dioxide(TiO_2) and initial concentration of 4BS on photocatalysis process,as well as effect of feed velocity and operating time on PAN700 and PVDF700 ultrafiltration membrane separation,was investigated in detail.To analyze the adsorption and photocatalytic process of the 4BS,Langmuir model was introduced.
     Results indicated that a maximal adsorption of dye on TiO_2 occurred at pH 5.5 and the adsorption character was accorded with Langmuir model. Under the optimal condition of UV=100W,T=20℃,dose of TiO_2 at 1.0g·L~(-1) and initial concentration of 4BS of 50 mg·L~(-1),the decoloration rate of 4BS after irradiation of 60min was up to 97.9%,and the mineralization rate showed a similar rate by UV-Visible spectrum and TOC value.Effect of the feed velocity and operating time on two kinds of membranes was also checked.PAN700 showed a larger permeate flux and better anti-pollution behavior than PVDF700.The characteristic constantβfor each membrane was calculated according to the cake filtration model and found that PAN700 was more suitable than PVDF700 for coupling system.
引文
[1]Janus M,Morawski A.W.New method of improving photocatalytic activity of commercial degussa P25 for azo dyes decomposition[J],Journal of Applied Catalysis B:Environmental.2007,75(1-2):118-123.
    [2]Gomes S.C,Faria J.L.Photochemical and photocatalytic degradation of an azo dye in aqueous solution by UV irradiation[J].Journal of Photochemistry and Photobiology A:Chemistry,2003,155(1-3):133-143.
    [3]崔鹏,赵先治.周民杰,等.光催化-膜分离集成反应器及其应用[J].催化学报.2006,27(09):752-754.
    [4]刘妙丽.基础化学(下册)[M].北京:中国纺织出版社,2005.
    [5]章杰.禁用染料和环保型染料[M].北京:中国化学工业出版社,2001:117.
    [6]杨超,柯丽霞,龚仁敏,等.花生壳粉作为生物吸附剂去除水溶液中偶氮染料的研究[J].生物学杂志.2005,22(02):45-48.
    [7]彭书传,崔康平,王诗生,等.坡缕石对直接耐酸大红4BS的吸附动力学特征[J].矿物学报.2006,26(03):267-261.
    [8]阎存仙,周红,李世雄.粉煤灰对染料废水的脱色研究[J].环境污染与防治.2000,05(02):3-5.
    [9]李庄,曾光明,高兴斋.偶氮染料废水处理研究现状及其发展方向[J].湖南化工.2000,30(06):12-15.
    [10]Hunter J.V.The effect of dyes on aerobic systems.In dyes and environment[M].ADMI,New York,NY,chap.6.1973
    [11]Michaels G.B,Lewis D.L.Sorption and toxicity of azo and triphenylmethane dyes to aquatic miCrobial populations[J].Environmental.Toxicology and Chemistry.1985,4:45-50.
    [12]Fujishima A,Honda K.K.Electrochemical photolysis of water at a semiconductor electrode[J].Nature.1972,238(5358):37-38.
    [13]Augugliaro V,Litter M,L.Palmisano,et al.The combination of heterogeneous photocatalysis with chemical and physical operations:A tool for improving the photoprocess performance[J].Journal of Photochemistry and Photobiology C:Photochemistry Reviews.2003,157(03):111-116.
    [14]刘守新,刘鸿.光催化及光电催化基础与应用[M].北京:化学工业出版社.2005.08
    [15]Linsebigler A,Lu G.Q,et al.Photocatalysis on TiO_2 surfaces:Principles,Mechanisms,and Selected results[J],Chemical Review.1995,95:755-758.
    [16]Daneshvar N,Sslari D,Khataee A.R.Photocatalytic degradation of azo dye acid red 14 in water:investigation of the effect of operational parameters[J].Journal of Photochemistry and Photobiology A:Chemistry.2003,157(03) 111-116.
    [17]顾松球,刘继华.纳米TiO_2的改性及其在废水处理中的应用[J].新技术新工艺.2007,10:19-20.
    [18]Mounir B,Pons M.N,Zahraa O,et aI.Discoloration of a red cationic dye by supported TiO_2photocatalysis[J].Journal of Hazardous Materials.2007,148:513-520.
    [19]Zhang H,Chen J,Zhang G,et al.Organic dyeing wastewater treatment with photocatatysis and membrane separation hybrid system[J].IWA Regional Conference Membrane Technologies in Water and Waste Water Treatment,2-4 June 2008,Moscow,Russia.
    [20]Tanala K,Padermpole K,Hisanaga T.Photocatalytic degradation of commercial azo dyes[J].Water Research,2000,34:327-333.
    [21]苗慧,范少华,崔玉民.5种偶氮染料溶液的光催化降解实验[J].河南科技大学学报:自然科学版.2006,27(3):93-96.
    [22]Kl(o|¨)pffer W.Photochemical degradation of pesticides and other chemicals in the environment:a critical assessment of the state of the art[J].Science of the Total Environment.1992,123-124:145-159.
    [23]李梅金,邱彬,郭光美,等.纳米TiO_2光催化转化下有机氯农药与AgNO_3的光谱特性研究[J].光谱学与光谱分析.2008,28(6):1364-1367.
    [24]陈士大.赵梦月,陶跃武.光催化降解有机磷农药废水的可行性[J].环境工程.1996,14(3):10-13.
    [25]Pelizzetti E,Pramauro E,Minero C,et al.Photocatalysis and Environment[M],Trend s and Application(Ed.Do rdrech t SM.),Kluw er A cadem ic Publishers,1988,469-497.
    [26]赵进才,张丰雷.二氧化钛微粒存在下表面活性剂光催化分解机理的研究[J].感光科学与光化学.1996,14(3),269-273.
    [27]Hidaka H,Horikoshi S,Ajisaka K,et al.Fate of amino acids upon exposure to aqueous titania irradiated with UV-A and UV-B radiation Photocatalyzed formation of NH_3,NO_3~- and CO_2[J]. Journal of Photochemistry and Photobiology A:Chemistry.1997,108(2-3):197-205.
    [28]Serpone N,Texier I,Emeline A.V,et al.Post-irradiation effect and reductive dechlorination of chlorophenols at oxygen-free TiO_2/water interfaces in the presence of prominent hole scavengers[J].Journal of Photochemistry and Photobiology A:Chemistry.2000,136(3):145-155.
    [29]Pelizzetti E,Minero C,Maurino V,et al.Photocatalytic degradation of nonylphenol ethoxylated surfactants[J].Environmental Science and Technology,2006,40(12):3775-3781.
    [30]Berry R.J,Mueller M.R.Photocatalytic Decomposition of Crude Oil Slicks Using TiO_2 on a Floating Substrate[J].Microchemical Journal.1994,50(1):28-32.
    [31]方佑龄,赵文宽,尹少华等.纳米TiO_2在空心陶瓷微球上的固定化及光催化分解辛烷[J].应用化学.1997,14(2):81-83
    [32]方佑龄,赵文宽,尹少华等.用浸涂法制备飘浮负载型TiO_2薄膜光催化降解辛烷[J].环境化学.1997,16(5):413-417.
    [33]肖俊霞,胡记杰.阎虹等.光电催化氧化技术中光电反应器的研究与发展[J].化工进展.2007,26(3):331-335.
    [34]刘秀华,傅依备,许云书.水处理中多相光催化反应器的研究进展[J].催化学报.2005,21(5):433-439.
    [35]Dijkstra M.F.J,Koerts E.C.B,Beenackers A.A.C.M,et al.Performance of immobilized photocatalytic reactor in continuous mode[J].AIChE Journal.2003,49(3):734-744.
    [36]Rizzo L,Koch J,Belgiorno V,et al.Removal of methylene blue in a photocatalytic reactor using polymethylmethacrylate supported TiO_2,nanofilm[J].Desalination.2007,211(1-3):1-9.
    [37]Xu N,Shi Z,Fan Y,et al.Effect of particles size of TiO_2 on photocatalytic degradation of methylene blue in aquies suspension[J].Ind.Eng.Chem.Res.1999,38:373-379.
    [38]Rosana M,Alberici,Wilson F,et al.Photocatalytic degradation of phenol and chlorinated phenols using Ag-TiO_2 in a slurry reactor[J].Water research.1994,28(8):1845-1849.
    [39]武杰灵,刘有智,李裕.纳米粒子固液分离实验研究[J].山西化工.2003,23(2):17-19.
    [40]周邵萍,洪磊,王刚,等.钛白颗粒离心沉降分离研究[J].流体机械.2006,34(2):10-12.
    [41]邢铁良,葛晓陵,洪磊.亚微米颗粒的离心沉降实验[J].中国非金属矿工业导刊.2005,01:27-28.
    [42]黄河,蒋展鹏.杨宏伟等.溶胶-凝胶法制备磁载光催化剂[J].环境污染治理技术与设 备.2004,5(1):65-68.
    [43]包淑娟.张校刚,刘献明.磁载WO_3-TiO_2/SiO_2/Fe_3O_4复合光催化剂的制备及其光催化活性[J].催化学报.2003,24(12):909-913.
    [44]Kagaya S,Shimizu K,Arai R,et al.Separation of titanium dioxide photocatalyst in its aqueous suspensions by coagulation with basic aluminium chloride[J].Water Research.1999,33(7):1753-1755.
    [45]赵宜江,邢卫红,徐南平.聚电解质对TiO_2悬浮体系微滤过程的影响[J].水处理技术.2005,31(8):7-9.
    [46]西蒙·贾德,布鲁斯·杰斐逊.膜技术与工业废水回用[M].北京:化学工业出版色.2006.2.
    [47]程五良.工业废水中膜技术应用与研究[J].韶关学院学报(自然科学版),2004,25(12):60-64
    [48]王湛.膜分离技术基础[M].北京,化学工业出版社,2000.
    [49]汪洪生,陆雍森.国外膜技术进展及其在水处理中的应用[M],膜科学与技术,1999,19(4):17-22
    [50]张雯.国外膜技术概述[J].化工装备技术.1995,16(1):48-51.
    [51]邵刚.膜法水处理技术及工程实例[M].北京:化学工业出版社,2002.3
    [52]Purkait M.K,Dasgupta S,De S.Removal of dye from wastewater using micellar-enhanced ultrafiltration and recovery of surfactant[J].Separation and Purification Technology,2004,37(1):81-92.
    [53]Abroad A.L,Puasa S.W,Zulkali M.M.D.Micellar-enhanced ultrafiltration for removal of reactive dyes from an aqueous solution[J].Desalination,2006,191(1-3):153-161.
    [54]Tan Y,Kyaw N.N,Teo W.K,et al.Decolorization of dye-containing aqueous solutions by the polyelectrolyte-enhanced ultrafiltration(PEUF) process using a hollow fiber membrane module [J].Separation and Purification Technology,2006,52:110-116.
    [55]M(?)tivier-Pignon H,Faur-Brasquet C,Cloirec P.L.Adsorption of dyes onto activated carbon cloths:approach of adsorption mechanisms and coupling of ACC with ultrafiltration to treat coloured wastewaters[J].Separation and Purification Technology,2003,31(1):3-11.
    [56]Al-Bastaki N,Banat F,Combining ultrafiltration and adsorption on bentonite in a one-step process for the treatment of colored waters[J].Resources,Conservation and Recycling,2004,41(2):103-113.
    [57]Banat F,AI-Bastaki N.Treating dye wastewater by an integrated process of adsorption using activated carbon and ultrafiltration[J].Desalination,2004,170(1):69-75.
    [58]Choo K.H,Choi S.J,Hwang E.D.Effect of coagulant types on textile wastewater reclamation in a combined coagulation/ultrafiltration system[J].Desalination,2007,202(1-3):262-270.
    [59]曾杭成,张国亮;孟琴等.超滤/反渗透双膜技术深度处理印染废水[J].环境工程学报,2008,2(8):1021-1025.
    [60]黄霞,桂萍.膜生物反应器废水处理工艺的研究进展[J],环境科学研究,1998,11(1):40-44.
    [61]黄涛,蒋华兵,张国亮等.悬浮态光催化超滤膜反声器处理4BS染料废水[J].水处理技术.2009,35(2):72-75.
    [62]Jiang H,Zhang G,Huang T,et al.Photocatalytic membrane reactor for degradation of acid red B wastewater[J].Chemical Engineering Journal,2009,doi:10.1016/j.cej.2009.04.011.
    [63]Fu J,Ji M,Wang Z,et al,A new submerged membrane photocatalysis reactor(SMPR) for fulvic acid removal using a nano-structured photocatalyst[J].Journal of Hazardous Materials,2006,131:238-242.
    [64]Xi W,Geissen S.Separation of titanium dioxide from photocatalytically treated water by cross-flow microfiltration[J].Water Research.2001,35(5):1256-1262
    [65]Fu J,Ji M,Zhao Y,et al.Kinetics of aqueous photocatalytic oxidation of fulvic acids in a photocatalysis-ultrafiltration reactor(PUR)[J].Separation and Purification Technology.2006,50:107-113.
    [66]Hisao H,Suzuki Y,Nohara K,et al.Photocatalyzed degradation of polymers in aqueous semiconductor suspensions I:Photooxidation of solid particles of polyvinylchloride[J],Journal of Polymer Science Part A:Polymer Chemistry.1996,34:1311.
    [67]傅平丰,栾勇,戴学刚.光催化水质净化反应器的研究进展[J].环境污染治理技术与设备,2004,5(9):18-24.
    [68]董文庚,白天雄,曹跟华,等.提高TiO_2光催化反应器氧化效率出的途径[J].河北科技大学学报,2003,24(1):86-90.
    [69]Vincenzo A,Marta L,Leonardo P,et al.The combination of heterogeneous photocatalysis with chemical and physical operations:A tool for improving the photoprocess performance[J].Journal of Photochemistry and Photobiology C:Photochemistry Reviews,2006,7:127-145.
    [70]崔鹏,赵先治,周民杰,等.光催化-膜分离集成反应器及其应用[J].催化学报,2006,27(9):52-754.
    [71]Chin S.S,Chiang K,Fane A.G.The stability of polymeric membranes in a TiO_2 photocatalysis process[J].Journal of Membrane Science,2006,275:202-211
    [72]张爱勇,肖羽堂,吕晓龙,高冠道.光催化膜反应器在污废水处理中的应用研究进展[J].现代化工,2006,26(10):25-30.
    [73]Azrague K,Aimar P,Benoit-Marquie F,et al.A new combination of a membrane and a photocatalytic reactor for the depollution of turbid water[J].Applied Catalysis B:Environmental,2007,72:97-204.
    [74]Poulios I,Avrana A,Rekliti E,et al.Photocatalytic oxidation of Auramine in the presence of semiconducting oxides[J].Journal of Chemical Technology and Biotechnology,2000,75:205-212.
    [75]尹晓红,辛峰,张凤宝.4BS染料光催化降解动力学[J].化工学报.2002,53(5):528-532.
    [76]傅剑锋,季民,金洛楠.影响光催化超滤膜反应器降解Acid Blue 7的因素研究[J].化工进展.2005,24(8):916-924.
    [77]朱长乐.膜科学技术[M].北京:高等教育出版社.2004.6.
    [78]Hlavacek M,Bouchet F.Constant flowrate blocking laws and an example of their application to dead-end microfiltration of protein solutions[J].Journal of membrane science,1993,82:285-295.
    [79]Bickley R.I,Ez-Carreno T.G,Lees J.S,et al.A structural investigation of titanium dioxide photocatalysts[J].Journal of solid state chemistry.1991,92:178-190.
    [80]赵振国.吸附作用应用原理[M].北京:化学工业出版社.2005.
    [81]Sauer T,Neto G.C,Jos(?) H.J,et al.Kinetics of photocatalytic degradation of reactive dyes in a TiO_2 slurry reactor[J].Journal of photochemistry and photobiology A:Chemistry.2002,149:147-154.
    [82]Bizani E,Fytianos K,Poulios I,et al.Photocatalytic decolorization and degradation of dye solution and wastewaters in the presence of titanium dioxide[J].Journal of hazardous materials.2006,136:85-94.
    [83]华耀祖.超滤技术与应用[M].北京:化学工业出版社.2003.
    [84]王怡中.二氧化钛悬浆体系中八种染料的太阳光催化氧化降解[J].催化学报.2000,21(4):327-331.
    [85]Kamble S.P,Sawant S.B,Pangarkar V.G.Batch and continuous photocatalytic degradation of benzenesulfonic acid using concentrated solar radiation [J]. Ind Eng Chem Res. 2003, 42:6705-6713.
    [86] Lee S.A, Choo K..H, Lee C.H, et al. Use of ultrafiltration membrane for the separation of TiO_2 photocatalysts in drinking water treatment[J]. Ind. Eng. Chem. Res. 2001,40: 1712-1719.

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