含铁矿物与UV联合催化H_2O_2深度处理印染废水
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摘要
分别以天然含铁矿物黄铜矿、磁铁矿、磁黄铁矿为催化剂,构建了UV-异相类Fenton体系处理实际印染废水生化出水,确定了最优反应条件,并对反应机理进行了初步探讨。实验结果表明:最佳条件下,以黄铜矿、磁铁矿、磁黄铁矿为催化剂的3种异相UV-类Fenton体系对废水的COD去除率分别可达58.83%、57.41%和60.57%,UV254去除率均大于94%;3种天然矿物在重复使用5次后对废水COD的去除率仍保持在50%以上,光催化活性稳定;该体系产生·OH的途径主要有催化剂表面的Fe(Ⅱ)催化H_2O_2分解、H_2O_2光解、溶出的Fe~(2+)催化H_2O_2分解3种,以前两种方式为主。
UV-heterogeneous Fenton-like systems were exploited to treat the biochemical effluent of printing and dyeing wastewater using natural iron-bearing minerals(chalcopyrite,magnetite and pyrrhotite)as catalysts. The optimal reaction conditions were determined and the reaction mechanisms were discussed. The experimental results showed that:Under the optimal conditions,the COD removal rate by the three UV-heterogeneous Fenton-like system with chalcopyrite,magnetite and pyrrhotite as catalysts reached 58.83%,57.41% and 60.57% respectively,the UV254 removal rates were all greater than 94%;The COD removal rates remained above 50% with the three natural minerals reused for 5 times,showing their excellent stability of photocatalytic activity;The origination of ·OH could be H_2O_2 decomposition catalyzed by Fe(Ⅱ)on surface of the catalysts,H_2O_2 photolysis and H_2O_2 decomposition catalyzed by dissolved Fe~(2+),and the former two were the main ways.
UV-heterogeneous Fenton-like systems were exploited to treat the biochemical effluent of printing and dyeing wastewater using natural iron-bearing minerals(chalcopyrite,magnetite and pyrrhotite)as catalysts. The optimal reaction conditions were determined and the reaction mechanisms were discussed. The experimental results showed that:Under the optimal conditions,the COD removal rate by the three UV-heterogeneous Fenton-like system with chalcopyrite,magnetite and pyrrhotite as catalysts reached 58.83%,57.41% and 60.57% respectively,the UV254 removal rates were all greater than 94%;The COD removal rates remained above 50% with the three natural minerals reused for 5 times,showing their excellent stability of photocatalytic activity;The origination of ·OH could be H_2O_2 decomposition catalyzed by Fe(Ⅱ)on surface of the catalysts,H_2O_2 photolysis and H_2O_2 decomposition catalyzed by dissolved Fe~(2+),and the former two were the main ways.
引文
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[9]MOUSSAVI G,REZAEI M,POURAKBAR M.Comparing VUV and VUV/Fe2+processes for decomposition of cloxacillin antibiotic:degradation rate and pathways,mineralization and by-product analysis[J].Chem Eng J,2018,332:140-149.
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[20]HULING S G,ARNOLD R G,SIERKA R A,et al.Measurement of hydroxyl radical activity in a soil slurry using the spin trapα-(4-Pyridyl-1-oxide)-N-tert-butylnitrone[J].Environ Sci Technol,1998,32(21):3436-3441.
[21]CHEN J X,ZHU L Z.Heterogeneous UV-Fenton catalytic degradation of dyestuff in water with hydroxyl-Fe pillared bentonite[J].Catal Today,2007,126(3/4):463-470.
[22]DAI H W,XU S Y,CHEN J X,et al.Oxalate enhanced degradation of OrangeⅡin heterogeneous UV-Fenton system catalyzed by Fe3O4@γ-Fe2O3 composite[J].Chemosphere,2018,199:147-153.
[2]冯勇,吴德礼,马鲁铭.黄铁矿催化类Fenton反应处理阳离子红X-GRL废水[J].中国环境科学,2012,32(6):1011-1017.
[3]温沁雪,王进,郑明明,等.印染废水深度处理技术的研究进展及发展趋势[J].化工环保,2015,35(4):363-369.
[4]PIGNATELLO J J,OLIVEROS E,MACKAY A.Advanced oxidation processes for organic contaminant destruction based on the Fenton reaction and related chemistry[J].Crit Rev Env Sci Technol,2006,36(1):1-84.
[5]WANG Y,SUN Y K,LI W G,et al.High performance of nanoscaled Fe2O3 catalyzing UV-Fenton under neutral condition with a low stoichiometry of H2O2:kinetic study and mechanism[J].Chem Eng J,2015,267:1-8.
[6]GAO Y Y,GAN H H,ZHANG G K,et al.Visible light assisted Fenton-like degradation of rhodamine Band 4-nitrophenol solutions with a stable poly-hydroxyl-iron/sepiolite catalyst[J].Chem Eng J,2013,217:221-230.
[7]WANG W M,SONG J,HAN X.Schwertmannite as a new Fenton-like catalyst in the oxidation of phenol by H2O2[J].J Hazard Mater,2013,262:412-419.
[8]LI W G,WANGA Y,IRINI A.Effect of pH and H2O2dosage on catechol oxidation in nano-Fe3O4 catalyzing UV-Fenton and identification of reactive oxygen species[J].Chem Eng J,2014,244:1-8.
[9]MOUSSAVI G,REZAEI M,POURAKBAR M.Comparing VUV and VUV/Fe2+processes for decomposition of cloxacillin antibiotic:degradation rate and pathways,mineralization and by-product analysis[J].Chem Eng J,2018,332:140-149.
[10]WANG Y,LIN X H,SHAO Z Z,et al.Comparison of Fenton,UV-Fenton and nano-Fe3O4 catalyzed UV-Fenton in degradation of phloroglucinol under neutral and alkaline conditions:role of complexation of Fe3+with hydroxyl group in phloroglucinol[J].Chem Eng J,2017,313:938-945.
[11]CHE H S,BAE S J,LEE W J.Degradation of trichloroethylene by Fenton reaction in pyrite suspension[J].J Hazard Mater,2010,185(2/3):1355-1361.
[12]马冬梅,陈泉源,何晋保.异相类Fenton氧化处理T酸废母液的催化剂[J].环境工程学报,2015,9(6):2601-2606.
[13]张钰,何燕,邹彩琼,等.铁锰矿类Fenton异相光催化降解有毒有机染料[J].环境化学,2010,29(6):1032-1037.
[14]国家环境保护局标准处.水质化学需氧量的测定重铬酸盐法:GB 11914-1989[S].北京:中国标准出版社,1990.
[15]国家环境保护总局科技标准司.水质铁的测定邻菲啰啉分光光度法:HJ/T 345-2007[S].北京:中国环境科学出版社,2007.
[16]姜成春,庞素艳,马军,等.钛盐光度法测定Fenton氧化中的过氧化氢[J].中国给水排水,2006,22(4):88-91.
[17]王维明.非均相光芬顿深度处理焦化废水的研究[D].哈尔滨:哈尔滨工业大学,2012.
[18]HERNEY-RAMIREZ J,VICENTE M A,MADEIRAL M.Heterogeneous photo-Fenton oxidation with pillared clay-based catalysts for wastewater treatment:a review[J].Appl Catal B,2010,98(1/2):10-26.
[19]BIANCHI D,BERTOLI M,TASSINARI R,et al.Ligand effect on the iron-catalysed biphasic oxidation of aromatic hydrocarbons by hydrogen peroxide[J].JMol Catal A:Chem,2003,204/205:419-424.
[20]HULING S G,ARNOLD R G,SIERKA R A,et al.Measurement of hydroxyl radical activity in a soil slurry using the spin trapα-(4-Pyridyl-1-oxide)-N-tert-butylnitrone[J].Environ Sci Technol,1998,32(21):3436-3441.
[21]CHEN J X,ZHU L Z.Heterogeneous UV-Fenton catalytic degradation of dyestuff in water with hydroxyl-Fe pillared bentonite[J].Catal Today,2007,126(3/4):463-470.
[22]DAI H W,XU S Y,CHEN J X,et al.Oxalate enhanced degradation of OrangeⅡin heterogeneous UV-Fenton system catalyzed by Fe3O4@γ-Fe2O3 composite[J].Chemosphere,2018,199:147-153.
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