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活化过硫酸盐技术降解二苯甲酮-9动力学研究
论文作者:童鞋论文网  论文来源:www.txlunwenw.com  发布时间:2019/10/29 7:56:55  

摘要:近年来,高级氧化技术被广泛应用于难降解有机物的处理,而基于硫酸根自由基的高级氧化技术以其氧化能力强、应用范围广等优点在废水、地下水以及土壤修复等方面得到水处理研究学者们越来越多的关注。硫酸根自由基的产生有多种途径,其中紫外活化、零价铁活化以及热活化过硫酸盐产生硫酸根自由基以其温和的反应条件和简便的操作成为目前应用较多的活化方式。本文选用二苯甲酮-9(BP-9)为目标污染物,通过探讨基于硫酸根自由基的高级氧化技术氧化降解二苯甲酮-9的过程,以期对废水中二苯甲酮类有机污染物的降解提供理论依据和技术基础。

本研究采用紫外、零价铁及加热三种方式活化过硫酸钠产生硫酸根自由基降解二苯甲酮-9,分别研究了这三种方法降解有机物的一级反应动力学,探讨了污染物初始浓度、氧化剂投加量、温度、pH值等一系列因素对降解过程的影响,同时还考察了降解反应过程中三维荧光变化以及毒性变化等。研究结果表明:三种方式活化过硫酸钠降解二苯甲酮-9均能达到较好的降解效果,且均符合降解反应一级反应动力学规律;反应过程中增加氧化剂投加量均能提高降解反应效率,而增加污染物初始浓度均能抑制降解反应的进行;采用热活化方式时,升高温度能有效提高污染物的去除效率,采用零价铁活化方式时,在一定范围内,去除效果随着零价铁的投加量增加而增加。

水中常见的阴离子以及pH值是影响降解反应的重要因素,在紫外/过硫酸钠体系中,酸性和碱性条件降解效果都优于中性条件,且pH值为7时降解效果最差;在零价铁/过硫酸钠与热/过硫酸钠体系中碱性和中性条件下,二苯甲酮-9的去除率较低,而酸性条件下二苯甲酮-9去除效果最佳。在紫外/过硫酸钠与热/过硫酸钠反应体系中溶液中阴离子都会抑制二苯甲酮-9降解反应的进行,同离子浓度下,碳酸氢根离子抑制作用最明显。在零价铁/过硫酸钠体系中CO32-、HCO3-、SO42-的存在抑制了二苯甲酮-9降解,而Cl-的存在则有利于二苯甲酮-9的降解。

Advanced oxidation technology was widelyused in the treatment of refractory organic matter, and advanced oxidationtechnology based on sulfate radicals was a new technology developed in recentyears. Sulfate radicals had gained much attention of water treatmentresearchers in wastewater, groundwater and soil remediation due to the strongoxidizing ability and pervasive application. The production of sulfate radicalshas multiple ways such as UV activation, zero valent iron activation andheating activation. In this study, benzophenone-9 (BP-9) was selected as thetarget contaminant to discuss the process of BP-9 degradation by advancedoxidation technology. Therefore, this study can provide the theoretical andtechnical basis to the degradation of organic pollutants in aquaticenvironment.

In this study, BP-9 was degradated bysulfate radicals whith generated from activated persulfate. The reactionkinetics and factors such as initial concentration, amount of oxidant dosing,temperature and pH values during the degradation process were considered.Meanwhile, the three-dimension fluorescence spectroscopy and the toxicitychange during the degradation process had also proposed. The results indicatedthat the degradation of benzophenone-9 by activated persulfate can achieve gooddegradation effect, and all of them was found to fit first order reactionkinetics. The degradation rates increased with the increasing of oxidantdosage, while decreased with the initial concentration of pollutants. Theelevated temperature can effectively improve the efficiency of pollutantremoval in thermal activation. The removal efficiency increased with theincrease of zero valence iron dosage within certain limits.

The common anions in aquatic environmentand pH values are important factors in the degradation process. In terms of UV/persulfatesystem, acid and alkaline conditions are favorable for BP-9 degradationcompared with neutral conditions, which means the degradation efficiency is theworst when the pH value was 7. However, during the Fe0 and heating process, thedegradation rate was low under alkaline and neutral conditions, and the removalefficiency of BP-9 was the best under acid condition. Besides, in UV andheating process, anions could inhibit the degradation of BP-9, and theinhibition of bicarbonate ions was the most obvious at the same ionconcentration. The presence of CO32-, HCO3-, SO42- inhibited the degradation ofBP-9 in the Fe0 system, while the presence of Cl- are favorable the degradationof BP-9.

关键词:过硫酸钠;硫酸根自由基;二苯甲酮-9;活化;降解;影响因素

Sodium persulfate; Sulfate radicals;Benzophenone-9; Activation; Degradation; Influencing factor

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