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实验室规模下卫生填埋渗滤液氧化过程中太阳能光芬顿反应参数的洞察

Insights into solar photo-Fenton reaction parameters in the oxidation of a sanitary landfill leachate at lab-scale.

作者信息

Silva Tânia F C V, Ferreira Rui, Soares Petrick A, Manenti Diego R, Fonseca Amélia, Saraiva Isabel, Boaventura Rui A R, Vilar Vítor J P

机构信息

LSRE - Laboratory of Separation and Reaction Engineering - Associate Laboratory LSRE/LCM, Departamento de Engenharia Química, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal.

LSRE - Laboratory of Separation and Reaction Engineering - Associate Laboratory LSRE/LCM, Departamento de Engenharia Química, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal.

出版信息

J Environ Manage. 2015 Dec 1;164:32-40. doi: 10.1016/j.jenvman.2015.08.030. Epub 2015 Sep 3.

Abstract

This work evaluates the effect of the main photo-Fenton (PF) reaction variables on the treatment of a sanitary landfill leachate collected at the outlet of a leachate treatment plant, which includes aerated lagooning followed by aerated activated sludge and a final coagulation-flocculation step. The PF experiments were performed in a lab-scale compound parabolic collector (CPC) photoreactor using artificial solar radiation. The photocatalytic reaction rate was determined while varying the total dissolved iron concentration (20-100 mg Fe(2+)/L), solution pH (2.0-3.6), operating temperature (10-50 °C), type of acid used for acidification (H2SO4, HCl and H2SO4 + HCl) and UV irradiance (22-68 W/m(2)). This work also tries to elucidate the role of ferric hydroxides, ferric sulphate and ferric chloride species, by taking advantage of ferric speciation diagrams, in the efficiency of the PF reaction when applied to leachate oxidation. The molar fraction of the most photoactive ferric species, FeOH(2+), was linearly correlated with the PF pseudo-first order kinetic constants obtained at different solution pH and temperature values. Ferric ion speciation diagrams also showed that the presence of high amounts of chloride ions negatively affected the PF reaction, due to the decrease of ferric ions solubility and scavenging of hydroxyl radicals for chlorine radical formation. The increment of the PF reaction rates with temperature was mainly associated with the increase of the molar fraction of FeOH(2+). The optimal parameters for the photo-Fenton reaction were: pH = 2.8 (acidification agent: H2SO4); T = 30 °C; [Fe(2+)] = 60 mg/L and UV irradiance = 44 WUV/m(2), achieving 72% mineralization after 25 kJUV/L of accumulated UV energy and 149 mM of H2O2 consumed.

摘要

本研究评估了主要光芬顿(PF)反应变量对渗滤液处理厂出口处收集的卫生填埋场渗滤液处理效果的影响,该渗滤液处理厂包括曝气塘、曝气活性污泥以及最后的混凝絮凝步骤。PF实验在实验室规模的复合抛物面聚光器(CPC)光反应器中利用人工太阳辐射进行。在改变总溶解铁浓度(20 - 100 mg Fe(2+)/L)、溶液pH值(2.0 - 3.6)、操作温度(10 - 50 °C)、用于酸化的酸类型(H2SO4、HCl和H2SO4 + HCl)以及紫外线辐照度(22 - 68 W/m(2))的同时测定光催化反应速率。本研究还试图利用铁的形态分布图阐明氢氧化铁、硫酸铁和氯化铁物种在PF反应应用于渗滤液氧化效率中的作用。最具光活性的铁物种FeOH(2+)的摩尔分数与在不同溶液pH值和温度值下获得的PF准一级动力学常数呈线性相关。铁离子形态分布图还表明,大量氯离子的存在对PF反应产生负面影响,这是由于铁离子溶解度降低以及羟基自由基被清除以形成氯自由基。PF反应速率随温度的增加主要与FeOH(2+)摩尔分数的增加有关。光芬顿反应的最佳参数为:pH = 2.8(酸化剂:H2SO4);T = 30 °C;[Fe(2+)] = 60 mg/L以及紫外线辐照度 = 44 WUV/m(2),在累积25 kJUV/L的紫外线能量和消耗149 mM的H2O2后实现72%的矿化。

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