超声—光Fenton组合工艺处理垃圾渗滤液的研究
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摘要
垃圾渗滤液特性取决于处置的固体废物的类型、稳定性、含水率及填埋场的水文、气象、温度、填埋时间和固体废物的分解阶段,具有显著地地域性和特异性；《生活垃圾填埋场污染控制标准》(GB16889-2008)严格规定了填埋场水污染物的排放浓度,这些因素都给生化处理技术处理垃圾渗滤液提出了挑战。而Fenton工艺可在温和条件下无选择性地将污染物降解或矿化成无害物质,被认为是一种可供选择的替代技术。
为研究超声、光与Fenton组合工艺对垃圾渗滤液的处理效果,以超声处理和Fenton法处理的一般规律出发,采用光和超声作为辅助技术来提升渗滤液的处理效果,并对各种组合工艺进行优化和比较,寻找最佳组合工艺,为垃圾渗滤液处理提供了一种新的处理方法,并建立了符合该水质特性的Fenton法处理垃圾渗滤液的反应动力学模型。
采用超声处理垃圾渗滤液,发现80KHz超声获得最高的COD去除率；COS和AOS的变化表明有机物矿化主要集中于超声前60min。低初始pH值、低初始浓度、较高反应温度和辅助曝气可提高渗滤液COD去除率。50KHz超声的NH3-N去除率最高；高初始pH值和辅助曝气可提高渗滤液NH3-N去除率；NH3-N初始浓度对去除效果影响不明显。对超声处理后的UV-vis光谱和EEM分析发现光谱强度增强,认为渗滤液中的大分子有机物裂解成小分子有机物；对特征参数和EEM的峰位移及Pi，n。的变化分析结果一致；且受渗滤液浓度、初始pH值、超声频率和时间等因素影响。
Fenton、US-Fenton、光Fenton和US-光Fenton法均能很好地处理垃圾渗滤液,且具有很多相似点：COD去除率均大于TOC去除率；有机物去除主要集中在前30min内,其中前10min变化最明显；AOS和COS值也是在前10min剧烈变化,30min后变化范围较小,说明有机物矿化和剧烈化学反应形成氧化反应中间体主要集中在反应前30min；初始pH值为3时,渗滤液获得最好的去除率；对所有处理工艺而言,均存在一个最佳H202用量,超过这个用量后,再增加H202用量对TOC去除率增加效果不明显；对光Fenton而言,发现[H2O2]/[Fe2+]摩尔比为4时,其氧化去除率最佳；而对其余工艺最佳试剂比为5；多次投加H202均可提高渗滤液TOC去除率,还发现Fe2+的投加方式和次数也影响TOC的去除率,不过在不同的工艺中呈现不同的效果；渗滤液初始浓度的提高,渗滤液TOC去除率也升高的趋势；反应温度的提高对各种处理工艺处理垃圾渗滤液的处理效果有一定的正面影响,不过对去除率的提升影响较小；研究发现各种工艺对UV254的去除效果均好于TOC。
US/Fe2+预处理渗滤液相当于一个投加微量H202的Fenton反应,其处理效果受初始pH值,Fe2+和反应温度影响；对光Fenton而言,TOC去除率随着S/V值的增加呈增加趋势。对同一浓度水样采用相同的操作参数,比较Fenton相关多种工艺对渗滤液的处理效果,发现渗滤液TOC去除率大小顺序为：US-光Fenton>US/光Fenton>US-Fenton>光Fenton>Fenton>US/Fe2+>US> UV。
在H2O23655-10965mg·L-1, FeSO4600-2800mgFe·L-1,温度12-30℃,初始pH值为3.0的条件下,Fenton;法处理垃圾渗滤液在5-30mmin内的反应动力学模型为：
The characteries of landfill leachate, with a significant specificity, depend on type of disposal, stability and moisture of solid waste, hydrology, meteorology and temperature of landfill site, landfill age and decomposition stages of solid waste;"Standard for pollution control on the landfill site of municipal solid waste"(GB16889-2008) regulate strict controlling over effluent concentration of leachate pollutants, those factors pose a challenge for landfill leachate to be treated by biological technology. The Fenton process, non-selectively reacted with organic compounds, can be used to degrade pollutants into harmless substances under mild conditions and considered to be an alternative technology for landfill leachate treatment.
To study effect of combined technology of sonication, photo and Fenton, the optimization of sonication and Fenton were firstly studied, then the technologies assisted by sonication and photo were used to improve removal of leachate, the aim of this research was found to a new approach to get best removal by comparison of various combinations process and the kinetic model of treatment leachate effluents by Fenton process was built finally.
The highest COD removal was achieved by80KHz sonication in this study and the mineralization of organic matter mainly achieved at the first60min according to the variation of COS and AOS. Low initial pH, low initial concentration, higher temperature and assisted aeration were beneficial for improving COD removal efficiency. The highest NH3-N removal was achieved by50KHz sonication in this research. Higher pH and assisted aeration can improve the NH3-N removal, the initial concentration have little influence on NH3-N removal. The higher intensities of UV-vis and EEM spectra were induced from breaking down high molecular weight organics into lower ones by sonication. That the variation of special parameters of UV-vis were in accord with the shift of peaks in EEM spectra or Pi,n by FRI were affected by initial pH, initial concentration, ultrasound frequency and reaction time.
The Fenton, US-Fenton, photo-Fenton and US-photo-Fenton processes were proved to be highly effective for treatment of landfill leachate. And they are similar in the following points:The degradation of leachate were got in the first30min, especially dramatically changed in the first10min and slowly after30min; the same phenomenon were appeared for AOS and COS, which meant that the dramatic chemical reaction were reacted and reaction intermediates were generated in the first30min. The best TOC removal was got at pH3. The economic TOC removal was existed for all researched Fenton-related processes. That the TOC removal were affected slightly when the dosage of H2O2excess2Dth for Fenton process and1Dth for the other. The best oxidation removal of leachate were got at [H2O2]/[Fe2+] molar ratio of4for photo-Fenton and5for the other. The TOC removal were increased with dosing times of H2O2while there are slight different in different process of dosing times of Fe2+. The TOC removal were increased with the initial concentration of leachate. The temperature had a slight effect on TOC removal for all process. The UV254removal were higher than TOC removal for all processes.
The leachate pretreated by US/Fe2+was equal to be treated by Fenton process containing little amount of H2O2. The TOC removal were affected by initial pH, initial concentration of Fe2+and temperature. The TOC removal was increased with S/V value increase in photo-Fenton. The order of TOC removal for the same leachate under unified parameters were US-photo-Fenton> US/photo-Fenton> US-Fenton> photo-Fenton>Fenton>US/Fe2+>US>UV.
Under the following conditions:H2O23655-10965mg·L-1, FeSO41200-28800mgFe·L-1,12-30℃and pH3.0, the kinetic reaction equation of leachate treatment by Fenton process between5min and30min of reaction was fitted as follows:
为研究超声、光与Fenton组合工艺对垃圾渗滤液的处理效果,以超声处理和Fenton法处理的一般规律出发,采用光和超声作为辅助技术来提升渗滤液的处理效果,并对各种组合工艺进行优化和比较,寻找最佳组合工艺,为垃圾渗滤液处理提供了一种新的处理方法,并建立了符合该水质特性的Fenton法处理垃圾渗滤液的反应动力学模型。
采用超声处理垃圾渗滤液,发现80KHz超声获得最高的COD去除率；COS和AOS的变化表明有机物矿化主要集中于超声前60min。低初始pH值、低初始浓度、较高反应温度和辅助曝气可提高渗滤液COD去除率。50KHz超声的NH3-N去除率最高；高初始pH值和辅助曝气可提高渗滤液NH3-N去除率；NH3-N初始浓度对去除效果影响不明显。对超声处理后的UV-vis光谱和EEM分析发现光谱强度增强,认为渗滤液中的大分子有机物裂解成小分子有机物；对特征参数和EEM的峰位移及Pi，n。的变化分析结果一致；且受渗滤液浓度、初始pH值、超声频率和时间等因素影响。
Fenton、US-Fenton、光Fenton和US-光Fenton法均能很好地处理垃圾渗滤液,且具有很多相似点：COD去除率均大于TOC去除率；有机物去除主要集中在前30min内,其中前10min变化最明显；AOS和COS值也是在前10min剧烈变化,30min后变化范围较小,说明有机物矿化和剧烈化学反应形成氧化反应中间体主要集中在反应前30min；初始pH值为3时,渗滤液获得最好的去除率；对所有处理工艺而言,均存在一个最佳H202用量,超过这个用量后,再增加H202用量对TOC去除率增加效果不明显；对光Fenton而言,发现[H2O2]/[Fe2+]摩尔比为4时,其氧化去除率最佳；而对其余工艺最佳试剂比为5；多次投加H202均可提高渗滤液TOC去除率,还发现Fe2+的投加方式和次数也影响TOC的去除率,不过在不同的工艺中呈现不同的效果；渗滤液初始浓度的提高,渗滤液TOC去除率也升高的趋势；反应温度的提高对各种处理工艺处理垃圾渗滤液的处理效果有一定的正面影响,不过对去除率的提升影响较小；研究发现各种工艺对UV254的去除效果均好于TOC。
US/Fe2+预处理渗滤液相当于一个投加微量H202的Fenton反应,其处理效果受初始pH值,Fe2+和反应温度影响；对光Fenton而言,TOC去除率随着S/V值的增加呈增加趋势。对同一浓度水样采用相同的操作参数,比较Fenton相关多种工艺对渗滤液的处理效果,发现渗滤液TOC去除率大小顺序为：US-光Fenton>US/光Fenton>US-Fenton>光Fenton>Fenton>US/Fe2+>US> UV。
在H2O23655-10965mg·L-1, FeSO4600-2800mgFe·L-1,温度12-30℃,初始pH值为3.0的条件下,Fenton;法处理垃圾渗滤液在5-30mmin内的反应动力学模型为：
The characteries of landfill leachate, with a significant specificity, depend on type of disposal, stability and moisture of solid waste, hydrology, meteorology and temperature of landfill site, landfill age and decomposition stages of solid waste;"Standard for pollution control on the landfill site of municipal solid waste"(GB16889-2008) regulate strict controlling over effluent concentration of leachate pollutants, those factors pose a challenge for landfill leachate to be treated by biological technology. The Fenton process, non-selectively reacted with organic compounds, can be used to degrade pollutants into harmless substances under mild conditions and considered to be an alternative technology for landfill leachate treatment.
To study effect of combined technology of sonication, photo and Fenton, the optimization of sonication and Fenton were firstly studied, then the technologies assisted by sonication and photo were used to improve removal of leachate, the aim of this research was found to a new approach to get best removal by comparison of various combinations process and the kinetic model of treatment leachate effluents by Fenton process was built finally.
The highest COD removal was achieved by80KHz sonication in this study and the mineralization of organic matter mainly achieved at the first60min according to the variation of COS and AOS. Low initial pH, low initial concentration, higher temperature and assisted aeration were beneficial for improving COD removal efficiency. The highest NH3-N removal was achieved by50KHz sonication in this research. Higher pH and assisted aeration can improve the NH3-N removal, the initial concentration have little influence on NH3-N removal. The higher intensities of UV-vis and EEM spectra were induced from breaking down high molecular weight organics into lower ones by sonication. That the variation of special parameters of UV-vis were in accord with the shift of peaks in EEM spectra or Pi,n by FRI were affected by initial pH, initial concentration, ultrasound frequency and reaction time.
The Fenton, US-Fenton, photo-Fenton and US-photo-Fenton processes were proved to be highly effective for treatment of landfill leachate. And they are similar in the following points:The degradation of leachate were got in the first30min, especially dramatically changed in the first10min and slowly after30min; the same phenomenon were appeared for AOS and COS, which meant that the dramatic chemical reaction were reacted and reaction intermediates were generated in the first30min. The best TOC removal was got at pH3. The economic TOC removal was existed for all researched Fenton-related processes. That the TOC removal were affected slightly when the dosage of H2O2excess2Dth for Fenton process and1Dth for the other. The best oxidation removal of leachate were got at [H2O2]/[Fe2+] molar ratio of4for photo-Fenton and5for the other. The TOC removal were increased with dosing times of H2O2while there are slight different in different process of dosing times of Fe2+. The TOC removal were increased with the initial concentration of leachate. The temperature had a slight effect on TOC removal for all process. The UV254removal were higher than TOC removal for all processes.
The leachate pretreated by US/Fe2+was equal to be treated by Fenton process containing little amount of H2O2. The TOC removal were affected by initial pH, initial concentration of Fe2+and temperature. The TOC removal was increased with S/V value increase in photo-Fenton. The order of TOC removal for the same leachate under unified parameters were US-photo-Fenton> US/photo-Fenton> US-Fenton> photo-Fenton>Fenton>US/Fe2+>US>UV.
Under the following conditions:H2O23655-10965mg·L-1, FeSO41200-28800mgFe·L-1,12-30℃and pH3.0, the kinetic reaction equation of leachate treatment by Fenton process between5min and30min of reaction was fitted as follows:
引文
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