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还原-ZPF催化氧化降解2,4-DNT效果及其机制
摘要点击 2316  全文点击 1609  投稿时间:2010-11-12  修订日期:2011-02-28
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中文关键词  硝基苯类化合物  α-FeOOH柱撑人造沸石  pH值  地下水修复  2,4-二硝基甲苯  还原-ZPF催化氧化
英文关键词  nitro aromatic compounds  zeotileartificial pillared by α-FeOOH  pH value  remediation of groundwater  2,4-dinitrotoluene  reduction-ZPF catalytic oxidation
作者单位
张进保 常州大学环境与安全工程学院 常州 213164中国环境科学研究院城市环境系统工程研究室 北京 100012 
席北斗 中国环境科学研究院城市环境系统工程研究室北京 100012 
姜永海 中国环境科学研究院城市环境系统工程研究室北京 100012 
李定龙 常州大学环境与安全工程学院常州 213164 
邓飞 常州大学环境与安全工程学院常州 213164 
马志飞 常州大学环境与安全工程学院常州 2131642.中国环境科学研究院城市环境系统工程研究室北京 100012 
王燕飞 中国环境科学研究院城市环境系统工程研究室北京 100012 
中文摘要
      以实验室制备的α-FeOOH柱撑人造沸石(zeotileartificial pillared by α-FeOOH, ZPF)为催化剂,并利用FTIR与XRD技术进行表征,采用批式实验研究其催化H2O2氧化去除地下水中难降解有机污染物2,4-二硝基甲苯(2,4-DNT)的效能,对比分析不同pH条件下Fe0还原、ZPF催化氧化及还原-ZPF催化氧化3种修复技术对2,4-DNT的去除效果,分析ZPF/H2O2催化氧化作用机制.结果表明,低pH利于2,4-DNT还原,pH=5时,反应120 min后,其还原率为96.6%,分别为pH 7、pH 9时还原率的1.2、2.0倍,最终还原产物为2,4-二硝基甲苯(2,4-DAT);不同pH时,ZPF/H2O2催化氧化降解2,4-DNT的能力存在如下关系:pH=7> pH=9> pH=5,且反应体系pH值接近α-FeOOH零电点时, 2,4-DNT催化氧化降解效果较好,其降解数据符合拟一级反应动力学模型.还原-催化氧化技术可先将2,4-DNT还原降解为易于催化氧化去除的2,4-DAT.pH=7时,2,4-DNT还原-ZPF催化氧化一级表观动力学常数kobs为0.0027 min-1,2,4-DNT的相对去除率提高为57.4%.反应体系中溶出Fe离子的浓度远小于0.07 mmol/L,作用机制主要为非均相芬顿反应,最终将2,4-DNT矿化降解为CO2和H2O.因此,还原-催化氧化组合技术去除地下水中2,4-DNT效果明显优于单一处理。
英文摘要
      ZPF(zeoliteartificial pillared by α-FeOOH) which prepared in the laboratory and characterized by FTIR and XRD was used as catalyst, and was tested for its activity in catalytic H2O2 of 2,4-DNT, which is persistent and difficult to be degraded in groundwater. The degradation of 2,4-DNT was examined at different pHs in the reduction, catalytic oxidation and combination technology of reduction-catalytic oxidation reaction systems. Moreover, the removal effect of 2,4-DNT was compared by these three approaches and the catalytic oxidation mechanism was analyzed. The results demonstrated that the removal effect of 2,4-DNT reduced to 2,4-DAT was up to 96.6% in 120 min at pH=5, which was 1.2, 2.0 times of the rate at pH 7, pH 9 respectively. The catalytic effect was various at different pHs and more significant when the pH close to the zero point of charge of α-FeOOH. The order of removal effect of 2,4-DNT at different pHs was pH=7> pH=9> pH=5.Compared to single reduction or catalytic oxidation, the removal effect of combination technology was 57.4%, which was evidently improved on the base of 2,4-DNT reduced to 2,4-DAT. The degradation of 2,4-DNT in the presence of ZPF/H2O2 follows a first-order kinetic model and the kobs was 0.0027 min-1. Due to the concentration of dissolved Fe ion was far less than 0.07 mmol/L, the mechanism was heterogeneous Fenton reaction acting on the surface of the catalyst. Therefore the combination technology was superior to the single treatment of reduction or catalytic oxidation.

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