基于硫酸根自由基的高级氧化技术对典型有机污染物降解的研究
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摘要
氯苯胺诸如苯胺和对氯苯胺(PCA)是水中常见的污染物，广泛应用于许多行业，例如染料制造、杀虫剂、橡胶助剂、抗氧化剂、药物、农药和除草剂等行业。PCA和苯胺对动物和人类具有毒性和致癌性，基于它们的这些危险性质，需要处理被其污染的废水以避免其对环境的有害影响。
基于产生硫酸根自由基(SO_4~-)的高级氧化技术是去除非生物降解的有机污染物的最有效方法之一。由于SO_4~-的强氧化性，其在治理废水方面受到了越来越多的关注，过硫酸盐活化技术由于其方法简单以及反应条件温和而成为了一项有效产生SO_4~-的技术。在本论文的研究中，利用零价铁(ZVI)活化过硫酸盐降解废水中的PCA和苯胺。零价铁(ZVI)能活化过硫酸盐产生硫酸根自由基，利用硫酸自由基的强氧化性可降解有机污染物。
在零价铁(ZVI)活化过硫酸盐(S_2O_8~(2-))降解对氯苯胺(PCA)的实验研究中，讨论了不同pH、温度、ZVI用量等条件对PCA降解的影响。实验结果表明：随着ZVI含量的增加，ZVI可以活化过硫酸盐产生更多的强氧化性的活性基团（如：硫酸自由基），使PCA的降解效率也随之加快。与碱性条件相比，PCA在酸性条件下(pH2.0和4.0)的降解效率更高，在pH为4.0时，PCA在12分钟即可完全降解。PCA的矿化作用非常显著，TOC在30分钟内去除效率就达到了69%，且随着时间的增长而增加，在pH为4.0的条件下，TOC在3小时后的去除率达到了94%。反应温度从15℃增加到50℃可显著增强PCA的降解效率。苯胺、对氯硝基苯、对苯醌、1-(4氯苯)-3苯基脲和5-氯-2-(4氯苯二氮烯)苯酚被认为是过硫酸盐氧化PCA的主要中间产物。
在实验室条件下，本文研究了零价铁(ZVI)活化过硫酸盐(S_2O_8~(2-))氧化降解水中的苯胺，讨论了不同pH、ZVI浓度、苯胺浓度、过硫酸盐浓度和反应温度等条件对苯胺降解效果的影响。结果表明：苯胺的降解效率随着温度的升高而增加；ZVI的最佳用量为0.4g/L，且有85%的苯胺得到降解；在pH为4.0时苯胺的降解效率最大，当pH大于或小于4.0时，苯胺的降解效率降低。在PS-ZVI系统中，苯胺降解的表观活化能是14.85kJmol~(-1)。在乙醇和叔丁醇等自由基捕获剂实验中，证明了苯胺降解过程中同时硫酸自由基和羟基自由基。通过GC-MS检测苯胺降解的中间产物有硝基苯、亚硝基苯和对苯醌，通过及基于这些中间物阐明了苯胺降解可能的反应途径。
Chloroanilines such as aniline and p-chloroaniline (PCA) are common water pollutantswhich are widely used in many industries such as dye manufacturing, pesticides, rubberchemicals, antioxidants, pharmaceuticals, pesticides and herbicides. PCA and aniline areconsidered to be toxic and carcinogenic to animals and human beings. These hazardousproperties of PCA and aniline require the treatment of contaminated wastewater to preventany deleterious effect to the environment.
Advanced oxidation processes based on the generation of sulfate radicals (SO_4~-) is oneof the most effective ways to remove the nonbiodegradable organic pollutants. Due to its highoxidation ability, SO_4~-is getting more and more attention for the treatment of wastewater.Persulfate activation is a promised technique to produce SO_4~-due to the simplicity of methodand mildness of reaction conditions. In this study zero valent iron (ZVI) was used to activatepersulfate for the degradation of PCA and aniline in wastewater. Zero valent iron (ZVI) canactivate persulfate to generate sulfate free radicals which are a strongest oxidant to degradeorganic pollutants
The degradation of p-chloroaniline (PCA) by persulfate (S_2O_8~(2-)) activated with zero-valent iron (ZVI) was investigated through batch experiments. Effects of pH, temperature anddosages of ZVI on PCA degradation were also examined. The degradation of PCA increasedwith higher dosage of ZVI due to increased activation of persulfate by zero-valent iron whichgenerates strong oxidizing species (sulfate radicals) in aqueous solution. The PCAdegradation was higher under acidic conditions (pH2.0and4.0) when compared to alkalineconditions. Complete degradation of PCA was obtained by ZVI-activated persulfate at pH4.0in12minutes. PCA mineralization was significant, where69%TOC removal efficiency wasachieved within30min. TOC removal efficiency increased with increasing time, so that94%TOC was removed after3h reaction time at pH4.0. An increase in reaction temperature from15to50℃significantly enhanced the PCA degradation. The aniline, N-(4-chlorophenyl)-p-phenylene di-imine,1-(4-chlorophenyl)-3-phenylurea and5-chloro-2-(4-chlorophenyl diazenyl) phenol were identified as the major intermediates of PCA oxidationby persulfate
The oxidative degradation of aniline in aqueous solution by persulfate activated withzero valent iron was studied under laboratory conditions. Batch experiments were conductedto investigate the effects of different parameters such as pH, ZVI concentration, aniline concentration, persulfate concentration and reaction temperature on aniline degradation. Theresults showed that aniline degradation increased with increasing temperature. The optimumdosage of ZVI was0.4g/L, and85%aniline degradation was observed. Maximum anilinedegradation was observed at pH4.0, whereas at pH above or below4.0, aniline degradationefficiency was decreased. In persulfate-ZVI system, the apparent energy of activation foraniline degradation was14.85kJ mol~(-1). The existence of persulfate radicals and hydroxylradicals produced during the degradation of aniline were identified with scavenger ethanoland tert-butyl alcohol. The reaction intermediates nitrobenzene, nitroso-benzene and p-benzoquinone were detected by gas chromatography–mass spectrometry. Based on theseintermediates observed a probable pathway of aniline degradation has been proposed.
基于产生硫酸根自由基(SO_4~-)的高级氧化技术是去除非生物降解的有机污染物的最有效方法之一。由于SO_4~-的强氧化性，其在治理废水方面受到了越来越多的关注，过硫酸盐活化技术由于其方法简单以及反应条件温和而成为了一项有效产生SO_4~-的技术。在本论文的研究中，利用零价铁(ZVI)活化过硫酸盐降解废水中的PCA和苯胺。零价铁(ZVI)能活化过硫酸盐产生硫酸根自由基，利用硫酸自由基的强氧化性可降解有机污染物。
在零价铁(ZVI)活化过硫酸盐(S_2O_8~(2-))降解对氯苯胺(PCA)的实验研究中，讨论了不同pH、温度、ZVI用量等条件对PCA降解的影响。实验结果表明：随着ZVI含量的增加，ZVI可以活化过硫酸盐产生更多的强氧化性的活性基团（如：硫酸自由基），使PCA的降解效率也随之加快。与碱性条件相比，PCA在酸性条件下(pH2.0和4.0)的降解效率更高，在pH为4.0时，PCA在12分钟即可完全降解。PCA的矿化作用非常显著，TOC在30分钟内去除效率就达到了69%，且随着时间的增长而增加，在pH为4.0的条件下，TOC在3小时后的去除率达到了94%。反应温度从15℃增加到50℃可显著增强PCA的降解效率。苯胺、对氯硝基苯、对苯醌、1-(4氯苯)-3苯基脲和5-氯-2-(4氯苯二氮烯)苯酚被认为是过硫酸盐氧化PCA的主要中间产物。
在实验室条件下，本文研究了零价铁(ZVI)活化过硫酸盐(S_2O_8~(2-))氧化降解水中的苯胺，讨论了不同pH、ZVI浓度、苯胺浓度、过硫酸盐浓度和反应温度等条件对苯胺降解效果的影响。结果表明：苯胺的降解效率随着温度的升高而增加；ZVI的最佳用量为0.4g/L，且有85%的苯胺得到降解；在pH为4.0时苯胺的降解效率最大，当pH大于或小于4.0时，苯胺的降解效率降低。在PS-ZVI系统中，苯胺降解的表观活化能是14.85kJmol~(-1)。在乙醇和叔丁醇等自由基捕获剂实验中，证明了苯胺降解过程中同时硫酸自由基和羟基自由基。通过GC-MS检测苯胺降解的中间产物有硝基苯、亚硝基苯和对苯醌，通过及基于这些中间物阐明了苯胺降解可能的反应途径。
Chloroanilines such as aniline and p-chloroaniline (PCA) are common water pollutantswhich are widely used in many industries such as dye manufacturing, pesticides, rubberchemicals, antioxidants, pharmaceuticals, pesticides and herbicides. PCA and aniline areconsidered to be toxic and carcinogenic to animals and human beings. These hazardousproperties of PCA and aniline require the treatment of contaminated wastewater to preventany deleterious effect to the environment.
Advanced oxidation processes based on the generation of sulfate radicals (SO_4~-) is oneof the most effective ways to remove the nonbiodegradable organic pollutants. Due to its highoxidation ability, SO_4~-is getting more and more attention for the treatment of wastewater.Persulfate activation is a promised technique to produce SO_4~-due to the simplicity of methodand mildness of reaction conditions. In this study zero valent iron (ZVI) was used to activatepersulfate for the degradation of PCA and aniline in wastewater. Zero valent iron (ZVI) canactivate persulfate to generate sulfate free radicals which are a strongest oxidant to degradeorganic pollutants
The degradation of p-chloroaniline (PCA) by persulfate (S_2O_8~(2-)) activated with zero-valent iron (ZVI) was investigated through batch experiments. Effects of pH, temperature anddosages of ZVI on PCA degradation were also examined. The degradation of PCA increasedwith higher dosage of ZVI due to increased activation of persulfate by zero-valent iron whichgenerates strong oxidizing species (sulfate radicals) in aqueous solution. The PCAdegradation was higher under acidic conditions (pH2.0and4.0) when compared to alkalineconditions. Complete degradation of PCA was obtained by ZVI-activated persulfate at pH4.0in12minutes. PCA mineralization was significant, where69%TOC removal efficiency wasachieved within30min. TOC removal efficiency increased with increasing time, so that94%TOC was removed after3h reaction time at pH4.0. An increase in reaction temperature from15to50℃significantly enhanced the PCA degradation. The aniline, N-(4-chlorophenyl)-p-phenylene di-imine,1-(4-chlorophenyl)-3-phenylurea and5-chloro-2-(4-chlorophenyl diazenyl) phenol were identified as the major intermediates of PCA oxidationby persulfate
The oxidative degradation of aniline in aqueous solution by persulfate activated withzero valent iron was studied under laboratory conditions. Batch experiments were conductedto investigate the effects of different parameters such as pH, ZVI concentration, aniline concentration, persulfate concentration and reaction temperature on aniline degradation. Theresults showed that aniline degradation increased with increasing temperature. The optimumdosage of ZVI was0.4g/L, and85%aniline degradation was observed. Maximum anilinedegradation was observed at pH4.0, whereas at pH above or below4.0, aniline degradationefficiency was decreased. In persulfate-ZVI system, the apparent energy of activation foraniline degradation was14.85kJ mol~(-1). The existence of persulfate radicals and hydroxylradicals produced during the degradation of aniline were identified with scavenger ethanoland tert-butyl alcohol. The reaction intermediates nitrobenzene, nitroso-benzene and p-benzoquinone were detected by gas chromatography–mass spectrometry. Based on theseintermediates observed a probable pathway of aniline degradation has been proposed.
引文
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