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新型芬顿法降解持久性多环芳烃有机污染物研究

Study on Degradation of Persistent Polycyclic Aromatic Hydrocarbon by Employing New Fenton Method

【作者】 伊茜

【导师】 ?忱?;

【作者基本信息】 重庆大学 , 分析化学, 2007, 硕士

【摘要】 有机污染物是环境中最主要的污染物之一,其中持久性难降解有机污染物危害大,处理困难。而持久性难降解有机物多为多环芳烃类物质。持久性难降解有机污染物在水中存在时间长、范围广、危害大、处理难度大,一直是环境保护领域的一个研究重点,其处理技术的研究一直深受国内外科学家的关注。Fenton氧化法是一种典型的高级氧化技术。它能产生氧化能力极强的羟基自由基·OH,羟基自由基能够有效的降解有机物,甚至彻底地将有机物转化为无害的无机物。本研究将微波引入Fenton反应体系促进降解多环芳烃类有机物--孔雀石绿和罗丹明B,研究内容包括:微波-Fenton试剂协同效应研究;在单因素试验的基础上利用正交实验设计得到最优化实验条件;通过控制性试验得到微波-Fenton氧化反应降解目标有机物的动力学方程;同时,用Cr(Ⅵ)离子溶液代替Fe(Ⅱ)离子溶液作为催化剂,进行上述试验降解目标有机物。实验结果表明:微波-Fenton试剂联用具有协同效应,能有效地加快孔雀石绿的降解速率,对于100mg/L孔雀石绿溶液的优化试验条件是:pH=3.4、1.00ml30%H2O2溶液、4.00ml0.020mol L-1Fe(Ⅱ)离子溶液、微波作用8min。此时,孔雀石绿去除率达到99.0%,COD去除率达到89.7%。初始pH=3.4条件下,微波辐射Fenton反应降解孔雀石绿的动力学方程为: V=0.033716×[Malachite Creen]0.986×[Fe2+]0.8234×[H2O2]0.1663。微波-类Fenton试剂联用具有协同效应,能有效地加快孔雀石绿的降解速率,对于100mg/L孔雀石绿溶液的优化试验条件是:pH=3.2、1.00ml30%H2O2溶液、5.00ml0.040mol L-1Cr(Ⅵ)离子溶液、微波作用8min。此时,孔雀石绿去除率达到90.0%,COD去除率达到67.0%。初始pH=3.2条件下,微波辐射类Fenton反应降解孔雀石绿的动力学方程为: V=0.004574×[Malachite Creen]1.153×[Cr6+]0.6712×[H2O2]0.2951。微波-Fenton试剂联用具有协同效应,能有效地加快罗丹明B的降解速率,对于100mg/L罗丹明B溶液的优化试验条件是:pH=3.0、0.70ml30%H2O2溶液、4.00ml0.020mol/LFe(Ⅱ)溶液、微波作用8min。此时,罗丹明B去除率达到99.9%,COD去除率达到90.2%。初始pH=3.0条件下,微波辐射Fenton反应降解罗丹明B的动力学方程为: V=0.064085×[Rhodamine B]0.4089×[Fe2+]1.4655×[H2O2]0.2562。微波-类Fenton试剂联用具有协同效应,能有效地加快罗丹明B的降解速率,对于100mg/L罗丹明B溶液的优化试验条件是:pH=3.4、1.0ml 30%H2O2溶液、4.00ml0.040 mol L-1Cr(Ⅵ)离子溶液、微波作用8min。此时,罗丹明B去除率达到99.0%,COD去除率达到80.4%。初始pH=3.4条件下,微波辐射类Fenton反应降解罗丹明B的动力学方程为: V=8.29182×10-5×[Rhodamine B]0.8763×[Cr6+]1.3719×[H2O2]0.5975

【Abstract】 Organic contaminants are the uppermost pollutants in environments; of that the kind of persistent organic pollutants (POPs) poses the largest harm due to they are difficult to be disposed. Being mostly polycyclic aromatic hydrocarbons, POPs have wide distribution, long-time existence and difficult disposal in water, thus arising considerable interests by scientists in many countries.Fenton hydrocarbonylation, being a senior oxidation technique, brings about hydroxyl free radical(·OH) which is efficacious to deCrade organic compounds, even to completely transforming organic compounds into harmless inorganic substances. In this paper, microwave is introduced into Fenton reaction system, aiming to improving deCradation of polycyclic aromatic hydrocarbon organics—malachite Creen and rhodamine B. the following contents are included: investigations on microwave-Fenton synergistic effects; deriving the optimum experimental condition from orthogonal experimental design based on single-factor experiment; via controlling experiment, kinetic equation for microwave-Fenton oxidizing reaction to deCrade target organics is obtained. Meanwhile, taking the place of ion Fe(Ⅱ), ion Cr(Ⅵ)is utilized as catalytic agent to implement above-mentioned experiments to deCrade target organics.By experiments, it is suggested that the couple of microwave-Fenton possess of synergistic effects which enable quick deCradation velocity of malachite Creen; for the malachite Creen solution with the concentration of 100mg/L, the optimum experimental condition is resulted; pH=3.4, 1.00ml30%H2O2, 4.00ml 0.020mol L-1Fe(Ⅱ) and 8min microwave interactions. Then, 99.0% of malachite Creen is removed and 89.7% for COD. On original condition that pH=3.4, kinetic equation for Fenton reaction in case of microwave radiation to deCrade malachite Creen is as: V=0.033716×[Malachite Creen]0.986×[Fe2+]0.8234×[H2O2]0.1663.Combination of microwave and Fenton-like agents possess of synergistic effects which enable quick deCradation velocity of malachite Creen; for the malachite Creen solution with the concentration of 100mg/L, the optimum experimental condition is as these: pH=3.2, 1.00ml30%H2O2, 5.00ml0.040mol L-1Cr(Ⅵ)and 8min microwave interaction. Then, 90.0% of malachite Creen is removed and 67.0% for COD. On original condition that pH=3.2, kinetic equation for Fenton reaction in case of microwave radiation to deCrade malachite Creen is as the following: V=0.004574×[Malachite Creen]1.153×[Cr6+]0.6712×[H2O2]0.2951.Couple of microwave-Fenton possesses of synergistic effects which enable quick deCradation velocity of rhodamine B; for the rhodamine B solution with the concentration of 100mg/L, the optimum experimental condition is as these: pH=3.0, 0.70ml30%H2O2, 4.00ml0.020mol/LFe(Ⅱ) and 8min microwave interactions. Then, 99.9% of rhodamine B is removed and 90.2% for COD. On original condition that pH=3.0, kinetic equation for Fenton reaction in case of microwave radiation to deCrade rhodamine B is as this: V=0.064085×[Rhodamine B]0.4089×[Fe2+]1.4655×[H2O2]0.2562.Combination of microwave and Fenton-like agents possess of synergistic effects which enable quick deCradation velocity of rhodamine B; for the rhodamine B solution with the concentration of 100mg/L, the optimum experimental condition is as these: pH=3.4, 1.00ml 30 % H2O2, 4.00ml0.040 mol L-1Cr(Ⅵ) and 8min microwave interactions. Then, 99.0% of rhodamine B is removed and 80.4% for COD. On original condition that pH=3.4, kinetic equation for Fenton reaction in case of microwave radiation to deCrade rhodamine B is as the following: V=8.29182×10-5×[Rhodamine B]0.8763×[Cr6+]1.3719×[H2O2]0.5975.

【关键词】 微波Fenton类FentonCr(Ⅵ)Fe(Ⅱ)孔雀石绿罗丹明B降解
【Key words】 MicrowaveFentonFenton-likeCr(Ⅵ)Fe(Ⅱ)Malachite CreenRhodamine BDeCradation
  • 【网络出版投稿人】 重庆大学
  • 【网络出版年期】2007年 05期
  • 【分类号】X703
  • 【被引频次】19
  • 【下载频次】1016
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