白云鄂博矿石非均相Fenton氧化技术的研究
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摘要
利用白云鄂博原矿和过氧化氢(H_2O_2)构成非均相Fenton体系产生的自由基氧化去除难降解有机污染物。考察了白云鄂博矿石投加量、pH和H_2O_2初始浓度对亚甲基蓝的催化氧化的影响。研究了亚甲基蓝(MB)在白云鄂博原矿-H_2O_2构成的非均相Fenton体系中的催化机理。结果表明,当白云鄂博矿石投加量1.2 g/L,pH=4.5,H_2O_2浓度1.06 mmol/L时,30 mg/L的亚甲基蓝去除率可达到97.33%,且亚甲基蓝的降解反应遵循准一级反应动力学。通过加入自由基捕获剂抗坏血酸、羟基自由基捕获剂甲醇和高价铁捕获剂N,N-二甲基亚砜证明了Fe3O4/改性沸石-H_2O_2体系的氧化物种为羟基自由基、过氧自由基和高价铁自由基。
The heterogeneous Fenton system about Baiyun Obo ore and H_2O_2 makes use of the free radical by H_2O_2 decomposition to remove oxide refractory organic pollutants. We study the catalytic mechanism of methylene blue with the heterogeneous Fenton system about Baiyun Obo ore and H_2O_2,and investigate the catalyst dosing quantity,pH and the initial concentration of H_2O_2 how to oxidate methylene blue. The results show that,when the catalyst dosing quantity is 1. 2 g/L,pH is 4. 5 and the initial concentration of H_2O_2 is 1. 06 mmol/L,the removal rate of methylene blue of 1. 86 mmol/L is 97. 33%. The oxidation reaction of methylene blue and the decomposition reaction of H_2O_2 follow the first order reaction kinetics equation. Joining the ascorbic acid(free radical scavenger),methanol(hydroxyl free radical scavenger)and DMSO(high iron capture agent) proves the oxidative species of Fe3O4/modified zeolite-H_2O_2 system are the hydroxyl free radicals,the oxygen free radicals and Fe(IV) = O.
The heterogeneous Fenton system about Baiyun Obo ore and H_2O_2 makes use of the free radical by H_2O_2 decomposition to remove oxide refractory organic pollutants. We study the catalytic mechanism of methylene blue with the heterogeneous Fenton system about Baiyun Obo ore and H_2O_2,and investigate the catalyst dosing quantity,pH and the initial concentration of H_2O_2 how to oxidate methylene blue. The results show that,when the catalyst dosing quantity is 1. 2 g/L,pH is 4. 5 and the initial concentration of H_2O_2 is 1. 06 mmol/L,the removal rate of methylene blue of 1. 86 mmol/L is 97. 33%. The oxidation reaction of methylene blue and the decomposition reaction of H_2O_2 follow the first order reaction kinetics equation. Joining the ascorbic acid(free radical scavenger),methanol(hydroxyl free radical scavenger)and DMSO(high iron capture agent) proves the oxidative species of Fe3O4/modified zeolite-H_2O_2 system are the hydroxyl free radicals,the oxygen free radicals and Fe(IV) = O.
引文
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[2]Mahmoodi N M,Salehi R,Aramim.Binary system dyeremoval from colored textile wastewater using activated carbon kinetic and isotherm studies[J].Desalination,2011,272(1/2/3):187-195.
[3]Glaze W H,Kang J W,Chapin G H.The chemistry of wastewater treatment processes involving ozone,hydrogen peroxide and ultraviolet radiation[J].Ozone:Science&Engineering:The Journal of the International Ozone Association,1987,9:335-341.
[4]张光明,张盼月,张信芳.水处理高级氧化技术[M].哈尔滨:哈尔滨工业大学出版社,2007:2-3.
[5]Neamtu M,Yediler A,Siminiceanu I,et al.Oxidation of commercial reactive azo dye aqueous solutions by the photo-Fenton and Fenton-like processes[J].Journal of Photoch and Photobiology A:Chemistry,2003,161(1):87-93.
[6]Lucas M S,Peres J A.Decolorization of the azo dye Reactive Black 5 by Fenton and photo-Fenton oxidation[J].Dyes and Pigments,2006,71(3):236-244.
[7]Dutta K,Bhattacharjee S,Chaudhuri B,et al.Chemical oxidation of C.I.Reactive Red 2 using Fenton-like reactions[J].Journal of Environmental Monitoring,2002(4):754-760.
[8]Kong S H,Watts R J,Choi J H.Treatment of petroleum contaminated soils using iron mineral catalyzed hydrogen peroxide[J].Chemosphere,1998,37(8):1473-1482.
[9]张娣,王懿萱,牛红云,等.纳米Fe3O4-H2O2去除诺氟沙星[J].环境科学,2011,32(10):2943-2948.
[10]Xue X F,Hanna K,Abdelmoula M,et al.Adsorption and oxidation of PCP on the surface of magnetite:Kinetic experiments and spectroscopic investigations[J].Applied Catalysis B:Environmental,2009,89(3/4):432-440.
[11]Yan Ni,Liu Fei,Xue Qiang,et al.Degradation of trichloroethene by siderite-catalyzed hydrogen peroxide and persulfate:Investigation of reaction mechanisms and degradation products[J].Chemical Engineering Journal,2015,274:61-68.
[12]邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报,2014,34(6):1436-1442.
[13]张国卿,王罗春,徐高田,等.Fenton试剂在处理难降解有机废水中的应用[J].工业安全与环保,2004,30(3):17-19.
[14]何洁,杨晓芳,张伟军,等.纳米Fe3O4-H2O2非均相Fenton反应催化氧化邻苯二酚[J].环境科学,2013,34(5):1773-1781.
[15]Xue X F,Harma K,Abdelmoula M,et al.Adsorption and oxidation of PCP on the surface of magnetite;Kinetic experiments and spectroscopic investigations[J].Applied Catalysis B-Environmental,2009,89(3/4):432-440.
[16]朱舜,姚玉元.Fenton-like催化纤维的制备及其催化氧化染料的研究[D].杭州:浙江理工大学,2013.
[17]Doorslaer X V,Heynderickx P M,Demeestere K,et al.Ti O2mediated heterogeneous photocatalytic degradation of moxifloxacin:operational variables and scavenger study[J].Applied Catalysis B:Environmental,2012,111/112:150-156.
[18]Pang S Y,Jiang J,Ma J.Response to comment on“Oxidation of sulfoxides and Arsenic(III)in corrosion of nanoscale zero valent iron by oxygen:evidence against ferryl ions(Fe(IV))as active intermediates in Fenton reaction”[J].Environmental Science&Technology,2011,45:3179-3180.