Fe(Ⅱ)活化O_2高级氧化降解罗丹明B染料
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摘要
基于传统Fenton体系中H_2O_2利用率低,修复费用高,对环境副作用大的缺点,通过向溶液中投加三聚磷酸钠(STPP),形成Fe(II)-STPP配合物,氧气替代H_2O_2作为氧化剂,构建Fe(II)/O_2/STPP的新型高级氧化体系,研究了该反应体系对模拟罗丹明B染料废水的降解性能.结果表明该体系对于罗丹明B具有良好的降解效果,并且在较广泛p H值(5-9)条件下罗丹明B降解率均在70%以上,废水中常见金属阳离子对降解效果基本没有影响.通过自由基掩蔽实验证明体系中对罗丹明B起降解作用的主要是·OH.该新型高级氧化体系更加绿色、可持续,在难降解染料等废水的处理中具有广泛的应用前景.
Traditional Fenton system has the disadvantages of low H_2O_2 utilization efficiency, high remediation cost and great environmental side effect. A new type of advanced oxidation system Fe(II)/O_2/sodium tripolyphosphate(STPP) was proposed to ease these disadvantages. Oxygen gas was used,as the oxidant to replace H_2O_2.STPP, an inorganic ligand, has the ability to form complexation with Fe(II), which could greatly activates O_2 to form reactive oxygen species. This studyinvestigated the degradation rhodamine B decreased by >70%at p H between 5~9. No remarkable effect was observed on the degradation of rhodamine B by common metal ions. The results of scavenger experiments show that ?OH was the main reactive oxygen species for contaminant degradation. This new reaction system is more green sustainable, and has a wide application prospect in refractory wastewater treatment.
Traditional Fenton system has the disadvantages of low H_2O_2 utilization efficiency, high remediation cost and great environmental side effect. A new type of advanced oxidation system Fe(II)/O_2/sodium tripolyphosphate(STPP) was proposed to ease these disadvantages. Oxygen gas was used,as the oxidant to replace H_2O_2.STPP, an inorganic ligand, has the ability to form complexation with Fe(II), which could greatly activates O_2 to form reactive oxygen species. This studyinvestigated the degradation rhodamine B decreased by >70%at p H between 5~9. No remarkable effect was observed on the degradation of rhodamine B by common metal ions. The results of scavenger experiments show that ?OH was the main reactive oxygen species for contaminant degradation. This new reaction system is more green sustainable, and has a wide application prospect in refractory wastewater treatment.
引文
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[3]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.
[4]Jia L,Shen Z,Guo W,et al.QSAR models for oxidative degradation of organic pollutants in the Fenton process[J].Journal of the Taiwan Institute of Chemical Engineers,2015,46:140-147.
[5]Keenan C R,Sedlak D L.Factors affecting the yield of oxidants from the reaction of nanoparticulate zero-valent iron and oxygen[J].Environmental Science&Technology,2008,42:1262-1267.
[6]Lee C,Sedlak D L.Enhanced formation of oxidants from bimetallic nickel-iron nanoparticles in the presence of oxygen[J].Environmental Science&Technology,2008,42(22):8528.
[7]Hug S J,Leupin O.Iron-catalyzed oxidation of arsenic(III)by oxygen and by hydrogen peroxide:p H-Dependent formation of oxidants in the Fenton reaction[J].Environmental Science&Technology,2003,37(12):2734-2742.
[8]Welch K D,Davis T Z,Aust S D.Iron Autoxidation and Free Radical Generation:Effects of Buffers,Ligands,and Chelators[J].Archives of Biochemistry&Biophysics,2002,397(2):360-369.
[9]Guan X,Dong H,Ma J.Influence of phosphate,humic acid and silicate on the transformation of chromate by Fe(II)under suboxic conditions[J].Separation&Purification Technology,2011,78(3):253-260.
[10]Keenan C R,Sedlak D L.Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen[J].Environmental Science&Technology,2008,42:6936-6941.
[11]高志婷.低价铁活化分子氧降解典型有机污染物的研究[D].武汉:华中师范大学,2013.
[12]Wang L,Wang F,Li P,et al.Ferrous-tetrapolyphosphate complex induced dioxygen activation for toxic organic pollutants degradation[J].Separation and Purification Technology,2013,120:148-155.
[13]Wang L,Cao M,Ai Z,et al.Design of a Highly Efficient and Wide p H Electro-Fenton Oxidation System with Molecular Oxygen Activated by Ferrous–Tetrapolyphosphate Complex[J].Environmental Science&Technology,2015,49(5):3032-9.
[14]Smith L A,Simmons S L,Mckeith F K,et al.Effects of Sodium Tripolyphosphate on Physical and Sensory Properties of Beef and Pork Roasts[J].Journal of Food Science,2010,49(6):1636-1637.
[15]姚群峰,徐顺清,周宜开,等.邻菲啰啉分光光度法测定铁的价态[J].中国卫生检验杂志,2000,10(1):3-5.
[16]Garciasegura S,Centellas F,Brillas E.Unprecedented Electrochemiluminescence of Luminol on a Boron-Doped Diamond Thin-Film Anode.Enhancement by Electrogenerated Superoxide Radical Anion[J].Journal of Physical Chemistry C,2012,116(29):15500–15504.
[17]Kim J,Lee C W,Choi W.Platinized WO3 as an environmental photocatalyst that generates OH radicals under visible light[J].Environmental Science&Technology,2010,44(17):6849-6854.
[18]Biaglow J E,Kachur A V.The generation of hydroxyl radicals in the reaction of molecular oxygen with polyphosphate complexes of ferrous ion[J].Radiation Research,1997,148(2):181-187.
[19]Minotti G,Aust S D.Redox cycling of iron and lipid peroxidation[J].Lipids,1992,27(3):219-226.