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超声空化及其组合技术降解焦化废水的研究【作者】徐金球 【导师】徐晓军; 宁平

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作者徐金球导师徐晓军; 宁平
[q)c:]6T6s q0【作者基本信息】昆明理工大学,矿物加工工程,2002年,博士

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8qu+\y0eBB8F$D0【中文摘要】 利用超声空化技术降解水中的有机污染物已经引起了世界各国水处理专家的广泛关注,但目前主要是研究低浓度单组分模拟废水的降解。本文以高浓度难降解的实际焦化废水为研究对象,详细研究了超声空化及其组合技术对其中的氨氮、有机氮和有机物(CODcr)的降解效果、作用机理和反应过程动力学。以焦化废水中的有机物苯酚为代表,深入研究了超声空化对苯酚的降解效果、作用机理、降解途径和反应过程动力学。较详细地研究了联合应用超声空化与Fenton试剂氧化法降解焦化废水的效果。特别是将超声空化技术与生物法联合用于降解高浓度难降解的焦化废水,考查了在不同条件下该组合工艺对焦化废水中的有机物(CODcr)的降解效果,并采用新型的水质模型对超声空化预处理降解焦化废水中各有机物组分的作用进行了分析解释,同时考查了催化剂在该组合工艺中的作用。 超声空化效应对焦化废水中的氨氮和有机氮有不同程度的降解作用,其对氨氮的降解效果优于对有机氮的降解效果。溶液的初始pH值、初始浓度、饱和气体的存在与否及其作用方式和超声波的声能密度是影响其降解效果的主要因素。废水中氨氮和有机氮降解的作用机理是以高温热解反应为主,氨氮和有机氮被...更多超声降解以后以氮气的形式释放到大气中,氨氮和有机氮的超声降解反应服从二级化学反应动力学。 超声空化效应对焦化废水中的有机物(CODcr)有很好的降解作用。溶液的初始pH值、饱和气体的存在与否及其作用方式、有机物(CODcr)的初始浓度和超声波的声能密度是影响其降解效果的主要因素。焦化废水经超声空化处理以后,其中的萘和吡啶等生物难降解有机物得到了有效降解,而苯酚、甲酚等有机物的浓度亦有较大程度的降低。有机物(CODcr)超声降解的作用机理是以·OH自由基的氧化反应为主,废水中有机物的超声空化降解反应服从一级化学反应动力学。 超声空化对苯酚水溶液的降解试验结果表明,各种试验条件对苯酚超声降解效果的影响规律与其对焦化废水中的有机物(CODcr)超声降解效果的影响规律相一致。苯酚超声降解的作用机理是,超声空化在水溶液中产生的·OH自由基进攻苯酚苯环上羟基的邻位或对位而使苯环断裂生成己二烯酸、顺式丁烯二酸和乙二酸小分子有机物而使苯酚得以降解,这些小分子有机物在·OH自由基的进一步作用下最终被氧化成CO2和H2O。根据苯酚超声降解的反应途径,提出了苯酚超声降解各基元反应的反应方程式,从理论上推导出苯酚的超声降解反应服从一级化学反应动力学。焦化废水中的大多数亲水性有机物(如苯酚及其同系物等)的超声降解机理为超声空化效应在水中产生的·OH自由基进攻苯环而将其氧化成小分子有机物,小分子有机物在·OH自由基的作用下进一步被氧化成CO2和H2O。 超声空化与Fenton试剂联合处理焦化废水对其中的有机物(CODcr)有较好的降解效果,二者对废水中有机物的降解作用存在正的协同效应。超声波的作用条件、溶液的初始pH值和Fenton试剂的用量是影响其降解效果的主要因素*enton试剂可以弥补超声波在水中产生的*H自由基产额的不足。 与单独活性污泥法相比,超声空化.活性污泥法联合能显著提高焦化废水中有机物的降解效果。COD*初始浓度 807 mg/L的焦化废水经超声波和活性污泥分别作用240 min后,CODcr降解率为 80.54%,比单独活性污泥法作用时 CODcr的降解率提高 48.29%。 超声空化-湿式催化氧化·活性污泥法联合能进一步提高焦化废水中有机物的降解效果。当在超声波辐照废水的过程中加入催化剂硫酸亚铁3刀 mmoVL时,超声波和活性污泥联合处理使废水中 CODcr的降解率达到 97.54%,比单独活性污泥法处理废水时的 COD*降解率提高 63.49%。  还原

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:Oyd@-Q*H,VyKs0【英文摘要】 Since the late of 1980's, the effectiveness of using ultrasonic technology to degrade organic pollutants of wastewater has caught the attention of research fellows worldwide concerned; as a result, intensive research work has been devoted to this approach. Nevertheless, most of the work to date has focused on the sonochemical degradation of single model organic pollutant with lower initial concentration in the simulated wastewater. By contrast, as for the treatment of the real wastewater of a coke plant, co-approach of combining ultrasonic cavitation with other technology was carried out, meanwhile, the degradation efficiency, mechanism, and reaction kinetics of the compounds, such as ammonia, nitrogen-bearing organic compounds, and CODcr-bearing organic compounds, were investigated in this thesis. The degradation efficiency, mechanism, pathway, and kinetics were investigated by taking phenol as the representative of the organic components in the coking wastewater. A combined approach ...更多of both ultrasonic cavitation and Fenton reagent was attempted. Particularly, by combining ultrasonic cavitation with oxic microbe, the degradation efficiency of CODcr-bearing organic compounds under various conditions was studied in detail so as to examine the degradability of the coke plant wastewater, which was regarded as a kind of wastewater of difficult-to-treat due to its higher initial concentration of organic compounds. And the explanation of the sonochemical decomposition of the organic pollutants in the wastewater was given by using a new water quality model. Catalysts was introduced to improve the degradation efficiency of CODcrbearing organic compounds in the ultrasonic process.To begin with, as demonstrated by the test results of single ultrasonic approach, ultrasonic cavitation has a stronger degradation effect on ammonia than on the rest nitrogen-bearing organic compounds. The initial pH value, the initial concentration of organic components, the presence of saturated gas, and the energy density of ultrasound consisted of the four key factors to affect the degradation efficiency. The sonochemical decomposition of ammonia and those containing nitrogen element took place via the reactions of thermal decomposition in cavitation bubbles. Consequently, nitrogen gas (Na), which would evaporate to air, was formed by the nitrogen elements coming from ammonia and those organic compounds containing nitrogen elements. The decomposition process follows pseudo second-order kinetics.Secondly, ultrasonic cavitation can also effectively degrade the CODcrbearing organic compounds of the coking wastewater. Again, the four key factors played a key rolein the process of degradation. The refractory substances such as naphthalene and pyridine were degraded considerably. Meanwhile, the concentration of phenol and cresols also fairly decreased. The mechanism was dominated by the reactions between CODCr-bearing organic compounds and -OH radicals of the bulk solution. While, thermal decomposition in cavitation bubbles or in the interfacial region (between the bubbles and bulk solution) played a less important role in the mechanism. The decomposition process is in line with the equation of pseudo first-order kinetics.Thirdly, tests of phenol solution have revealed that impacts of experimental parameters on phenol are as same as the impacts on CODCr of the coking wastewater. The mechanism of ultrasonic degradation of phenol is that -OH radicals produced by ultrasound in aqueous solution attack phenolic cycle at adjacent or para position of the hydroxyl on phenol so that phenol is changed into small organic molecules such as muconic acid, maleic acid and ethane diacid. These small organic molecules will be oxidized to form carbon dioxide and water by -OH radical eventually. According to the reaction pathway of the ultrasonic degradation of phenol, its reaction equation is in line with the equation of first-order kinetics. The mechanism of ultrasonic degradation of most hydrophilic organic compounds such as phenol, cresols in t  还原水利论文%w e K&G e%OG} \0n

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【中文关键词】 超声空化; 焦化废水; 苯酚; Fenton试剂; 活性污泥法; 催化剂; 水质模型
h tPQ%x {(Q]8c0【英文关键词】 ultrasonic cavitation; coking wastewater; phenol; Fenton reagent; activated-sludge process; catalyst; water quality model水利论文p4ucJ-]6{
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