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共存氯苯类同系物对六氯苯厌氧降解活性的影响   总被引:1,自引:0,他引:1       下载免费PDF全文
王琪  刘辉  姜林  唐军 《环境科学》2014,35(4):1358-1365
微生物厌氧降解六氯苯已经成为国内外六氯苯污染土壤修复技术研发的前沿和热点.研究了在不同的初始pH值、反应温度及固液比等环境条件下,3种共存氯苯类同系物五氯苯、1,2,4,5-四氯苯、1,2,4-三氯苯对染料厂污染土壤中六氯苯厌氧降解活性的影响.结果表明,在降解过程中,共存氯苯类同系物的累积对六氯苯的厌氧降解产生了反馈抑制作用,影响了六氯苯的降解活性,且在不同的环境条件下,累积规律不同,反馈抑制作用不同.反应的初始pH值较低时,五氯苯的的反馈抑制作用更突出,反应的初始pH值较高时,1,2,4-三氯苯的反馈抑制作用更突出;常温下,五氯苯的反馈抑制作用更突出,较高温度下,1,2,4-三氯苯的反馈抑制作用更突出;固液比越小,五氯苯的反馈抑制作用越突出.因此,针对性地采取提高低氯苯类同系物降解活性的措施,降低共存低氯苯类同系物在六氯苯厌氧降解过程中的累积,不失为提高污染土壤中六氯苯降解率的一种好的选择.  相似文献   
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Decomposition of hexachlorobenzene(HCB)was investigated over several metal oxides(i.e.,MgO,CaO,BaO,La2O3,CeO2,MnO2, Fe2O3,and Co3O4)supported on Al2O3,which was achieved in closed system at a temperature of 300°C.Catalysts were prepared by incipient wetness impregnation with different metal oxides loading and impregnating solvents.The decomposition effciency of different catalysts for this reaction depends on the nature of the metal oxide used,and Al2O3 supported La2O3 was found to be the most active one.Pe...  相似文献   
4.
金属氧化物降解六氯苯的活性比较及催化机理研究   总被引:1,自引:0,他引:1       下载免费PDF全文
以氧化铝(α-Al_2O_3、γ-Al_2O_3)、氧化钙(CaO)、过渡金属氧化物(Mn O_2、α-Fe_2O_3、γ-Fe_2O_3、Ni_2O_3、CuO)为催化剂,考察了催化剂种类、添加比例等因素对六氯苯(Hexachlorobenzene,HCB)降解效果和产物组分的影响.结果表明,催化效果随催化剂添加比例的提高显著增加.在反应温度为350℃,反应时间1 h,金属氧化物添加比例为100∶1的条件下,碱土金属氧化物CaO及过渡金属氧化物中的α-Fe_2O_3和Ni_2O_3降解活性较好,这3种氧化物对HCB的降解率分别达到65.5%、100.0%和100.0%,脱氯率D_1分别为54.4%、81.9%和77.5%.HCB降解有机产物分析结果显示,8种金属氧化物与HCB样品反应产物中均存在低氯代苯,在α-Fe_2O_3和Ni_2O_3的催化作用下有2~4氯代低氯苯检出,说明在降解过程中存在明显的逐级脱氯/加氢反应;与CaO反应后的产物中低氯代苯较少,经拉曼光谱定性分析,有无序碳的检出,说明除了脱氯/加氢还存在脱氯缩合反应.  相似文献   
5.
黄俊  杨曦  张祖麟  余刚 《环境科学》2006,27(12):2392-2395
以高压汞灯为光源,分别研究了六氯苯在正己烷和邻苯二甲酸二异辛酯(DIOP)为有机气溶胶表层模拟介质时的光解,发现六氯苯在正己烷和DIOP中的光解半衰期分别约为<5 min和5 h,相差70倍以上.研究发现蒽醌和甲氧酚类气溶胶组分对六氯苯的光解具有光敏化作用,其反应机制可能分别为能量转移和抽氢反应.六氯苯光解的主要产物是五氯酚.  相似文献   
6.
针对城市生活垃圾焚烧(MSWI)过程中二(口恶)英类的生成机制以及焚烧飞灰的组成,研究了MSWI飞灰中常见的钙化合物(CaO,Ca(OH)2,CaCl2,CaSO4及Ca(NO3)2)对前生体五氯酚(PCP)及六氯苯(HCB)生成二(口恶)英类的阻滞作用.结果表明,280℃下加热2 h,Ca(NO3)2,Ca(OH)2和CaO对PCP生成二(口恶)英类的总阻滞效率分别为93.7%,80.4%和98.9%,而CaCl2和CaSO4几乎没有效果.CaO对PCP和HCB混合物生成二(口恶)英类物质同样具有良好的阻滞效果.另外,探讨了上述钙化合物对PCP及HCB生成二(口恶)英类的阻滞作用机理.  相似文献   
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BACKGROUND, AIMS AND SCOPE: In the first part of this paper the main principles which control the dehalogenation of polychlorinated aromatic compounds on municipal waste incineration fly ash (MWI-FA) have been discussed and the model fly ash of similar dehalogenation activity has been proposed. Even if both systems show comparable dehalogenation properties, the main question concerning the postulated identical reaction mechanism in both cases is left unanswered. The other very important point is to what extent is this dechlorination mechanism thermodynamically controlled. The same problem is often discussed in the literature also for the de novo synthetic reactions. From the data it is clear that metallic copper plays a decisive role in the mechanism of the dehalogenation reaction. Although the results reported in the first part strongly support the idea that copper acts in this dechlorination as the reaction component, in contrast to its generally accepted catalytic behaviour, we believed that additional support for this conclusion can be obtained with the help of a thermodynamic interpretation of the mechanism of the reaction. RESULTS AND DISCUSSION: The pathways of hexachlorobenzene dechlorination on MWI-FA and model fly ash were studied in a closed system at 260-300 degrees C under nitrogen atmosphere. These pathways were the same for both systems, with the following prevailing sequences: hexachlorobenzene --> pentachlorobenzene --> 1,2,3,5-tetrachlorobenzene --> 1,3,5-trichlorobenzene --> 1,3-dichlorobenzene. Thermodynamic calculations were carried out by using the method of minimization total Gibbs energy of the whole system. In the calculations, the following reaction components were taken into account: all gaseous chlorinated benzenes, benzene, hydrogen chloride, a gaseous trimer Cu3Cl3, and also Cu2O and CuCl2 as solid components. The effect of the reaction temperature and the amount of copper and water vapour were considered as well. The effect of reaction temperature was determined from the data calculated for the 500 to 750 K temperature region. The effect of the initial composition was determined for the molar amounts of copper = 0.01-3 moles and water vapour = 0.2 to 3 moles per mole of chlorobenzene isomer CONCLUSIONS: The results of hexachlorobenzene dechlorination by MWI-FA and model fly ash under comparable reaction conditions allow us to conclude that both dechlorinations proceed via the same dechlorination pathways, which can be taken as an evidence of the identical dehalogenation mechanism for both systems. The relative percentual distribution of the dehalogenated products depends on the temperature, but not on the initial amount of water vapour or copper metal. On the other hand, the initial amount of copper substantially affects the conversion of the dehalogenation as well as the molar ratio of Cu3Cl3 to HCl in the equilibrium mixture. Comparison of the experimental with thermodynamic results supports the idea that dehalogenation reactions are thermodynamically controlled. RECOMMENDATIONS AND OUTLOOK: Thermodynamic analysis of the dehalogenation reactions may prove useful for a wide range of pollutants. The calculations concerning polychlorinated biphenyls and phenols are under study.  相似文献   
8.
采用批量平衡试验的方法,研究了不同初始浓度的六氯苯在红壤和黄泥土表面的吸附与解吸特征. 结果表明,六氯苯在红壤和黄泥土表面的吸附与解吸行为均可用Freundlich方程进行很好的拟合,其相关系数(R2)在0.97-0.99之间,并表现为非线性特征. 六氯苯在红壤和黄泥土上吸附的KadsF值均小于其解吸的KdesF值,说明六氯苯在这两种土壤表面的解吸表现为一定的滞后效应. 随着初始浓度的升高,其滞后效应增强,两者呈线性相关. 用不同方程对滞后系数H,ω和λ进行量化,发现不同浓度的六氯苯在土壤表面的解吸过程表现出正滞后效应.  相似文献   
9.
染料厂污染土壤中六氯苯的水淹法厌氧降解   总被引:2,自引:0,他引:2  
以乙酸为碳源,采用正交实验的方法,探讨了水淹法厌氧降解某染料厂污染土壤中六氯苯的效果,研究考察了初始pH、反应温度和固液比3个环境因素对六氯苯降解率的影响,确定了六氯苯最佳的厌氧降解条件。结果表明,初始pH对土壤中六氯苯的降解率影响最大。在初始pH为5,反应温度为45℃,固液比为1∶1的最佳反应条件下,六氯苯的降解率最高达到52.56%。  相似文献   
10.
以六氯苯作为模型化合物,建立了半挥发性有机污染物样品净化的气相色谱方法.采用进样阀切换载气吹扫的进样方式,通过保留间隙柱和溶剂放空装置实现大体积进样,经过气相色谱分离后将分析物所在的半挥发性组分选择性冷凝在收集管中.本方法对模型化合物六氯苯的制备回收率为90%,对半挥发性有机污染物样品净化方法的发展具有重要意义.  相似文献   
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