不同共基质条件下上流式厌氧污泥床反应器中硝基酚的降解研究

用实验室规模的2个UASB反应器,分别研究了以葡萄糖和乙酸钠为共基质条件下3-硝基酚(3-NP)和2,6-二硝基酚（2,6-DNP）的降解效果.结果表明,对3-NP的降解,用葡萄糖作共基质的效果明显好于以乙酸钠为共基质;而对2,6-DNP的降解,乙酸钠作共基质效果更好.在含3-NP废水厌氧降解实验中,保持进水COD浓度为2 500 mg/Ｌ左右,HRT为26 h,以葡萄糖为共基质时,进水3-NP浓度可提高到254.6 mg/Ｌ,3-NP的去除率保持在99.0%以上;以乙酸钠为共基质时,保持HRT为30 h,3-NP浓度可提高到71.6 mg/Ｌ,3-NP去除率在90.0%以上.在含2,6-DNP废水厌氧降解实验中,保持进水COD浓度在2 500 mg/Ｌ左右,HRT为35 h,以葡萄糖为共基质时,2,6-DNP浓度可提高到170.0 mg/Ｌ,2,6-DNP的去除率保持在98.0%以上;以乙酸钠为共基质时,保持HRT为30 h,2,6-DNP最大浓度可提高到189.5 mg/Ｌ,2,6-DNP的去除率在99.2%以上.     

以混合单氯酚驯化厌氧颗粒污泥降解2,4-DCP的研究

利用邻氯酚 (2-CP)和对氯酚 (4-MCP)的模拟废水驯化厌氧颗粒污泥并考察驯化的污泥对2,4-二氯酚 (2,4-DCP)的降解性.通过摇瓶试验和运行连续流反应器研究了将2种单氯酚驯化过的污泥混合后对混合单氯酚以及2,4-DCP的降解特性,并比较了驯化与未驯化的污泥降解2,4-DCP过程的差异.驯化与未驯化的污泥分别在50 h和180 h左右将2,4-DCP降解完全,表明混合单氯酚驯化的厌氧颗粒污泥降解2,4-DCP 比未驯化的厌氧颗粒污泥快.虽然2种污泥降解过程都出现了4-MCP积累现象,但驯化的污泥可以逐渐降解4-MCP,未驯化的污泥则无法降解.因此,混合单氯酚驯化的污泥可以强化邻、对位脱氯功能,并且提高污泥对2,4-DCP的降解性.连续流厌氧颗粒污泥-悬浮载体反应器的运行结果表明,接种混合单氯酚驯化的厌氧污泥能够同时降解2种单氯酚,可缩短启动时间,并提高了降解二氯酚效率.2-CP的去除率一直维持在80%左右,4-MCP随着进水浓度变化去除率在30%～80%波动.     

玉米芯生物炭对2,4-D在土壤中吸附性能的研究

研究了玉米芯生物炭剂对土壤中2,4-D的吸附性能,并探讨了影响吸附的因素和吸附机理.结果表明:生物炭可使土壤对2,4-D的吸附容量显著增大.吸附结果用Freundlich和Redlich-Peterson方程都可以较好地拟合(R20.95).60 h后,与对照土壤相比,添加质量分数为0.5%生物炭的土壤对2,4-D的最大吸附量从20.83μg·g-1升高到58.82μg·g-1.吸附动力学研究表明,伪二级动力学速率方程对土壤吸附2,4-D的过程拟合效果较好(R20.99),优于一级动力学速率模型;p H和温度对土壤中2,4-D的吸附影响显著,p H接近3.1和40℃的水浴环境更利于添加生物炭的土壤对2,4-D的吸附.玉米芯生物炭可作为原位修复剂吸附土壤中的2,4-D,从而降低土壤中有机污染物的迁移性和生物有效性.     

Powdered activated carbon adsorption of two fishy odorants in water: Trans,trans-2,4-heptadienal and trans,trans-2,4-decadienal

Powdered activated carbon(PAC) adsorption of two fishy odorants, trans,trans-2,4-heptadienal(HDE) and trans,trans-2,4-decadienal(DDE), was investigated. Both the pseudo first-order and the pseudo second-order kinetic models well described the kinetics curves, and DDE was more readily removed by PAC. In isotherm tests, both Freundlich and Modified Freundlich isotherms fitted the experimental data well. PAC exhibited a higher adsorption capacity for DDE than for HDE, which could be ascribed to the difference in their hydrophobicity. The calculated thermodynamic parameters(ΔG~0, ΔH~0, and ΔS~0) indicated an exothermic and spontaneous adsorption process. PAC dosage, p H, and natural organic matter(NOM) presence were found to influence the adsorption process. With increasing PAC dosage, the pseudo first-order and pseudo second-order rate constants both increased. The value of p H had little influence on HDE or DDE molecules but altered the surface charge of PAC, and the maximum adsorption capacity occurred at p H 9. The presence of NOM, especially the fraction with molecular weight less than1 k Dalton, hindered the adsorption. The study showed that preloaded NOM impaired the adsorption capacity of HDE or DDE more severely than simultaneously fed NOM did.     

Powdered activated carbon adsorption of two fishy odorants in water: Trans,trans-2,4-heptadienal and trans,trans-2,4-decadienal

Powdered activated carbon (PAC) adsorption of two fishy odorants, trans,trans-2,4-heptadienal (HDE) and trans,trans-2,4-decadienal (DDE), was investigated. Both the pseudo first-order and the pseudo second-order kinetic models well described the kinetics curves, and DDE was more readily removed by PAC. In isotherm tests, both Freundlich and Modified Freundlich isotherms fitted the experimental data well. PAC exhibited a higher adsorption capacity for DDE than for HDE, which could be ascribed to the difference in their hydrophobicity. The calculated thermodynamic parameters (ΔG⁰, ΔH⁰, and ΔS⁰) indicated an exothermic and spontaneous adsorption process. PAC dosage, pH, and natural organic matter (NOM) presence were found to influence the adsorption process. With increasing PAC dosage, the pseudo first-order and pseudo second-order rate constants both increased. The value of pH had little influence on HDE or DDE molecules but altered the surface charge of PAC, and the maximum adsorption capacity occurred at pH 9. The presence of NOM, especially the fraction with molecular weight less than 1 k Dalton, hindered the adsorption. The study showed that preloaded NOM impaired the adsorption capacity of HDE or DDE more severely than simultaneously fed NOM did.     

Cagelike mesoporous silica encapsulated with microcapsules for immobilized laccase and 2, 4-DCP degradation

In this study, cage-like mesoporous silica was used as the carrier to immobilize laccase by a physical approach, followed by encapsulating with chitosan/alginate microcapsule membranes to form microcapsules of immobilized laccase based on layer-by-layer technology. The relationship between laccase activity recovery/leakage rate and the coating thickness was simultaneously investigated. Because the microcapsule layers have a substantial network of pores, they act as semipermeable membranes, while the laccase immobilized inside the microcapsules acts as a processing plant for degradation of 2,4-dichlorophenol. The microcapsules of immobilized laccase were able to degrade 2,4-dichlorophenol within a wide range of 2,4-dichlorophenol concentration, temperature and pH, with mean degradation rate around 62%. Under the optimal conditions, the thermal stability and reusability of immobilized laccase were shown to be improved significantly, as the removal rate and degradation rate remained over 40.2% and 33.8% respectively after 6 cycles of operation. Using mass spectrometry (MS) and nuclear magnetic resonance (NMR), diisobutyl phthalate and dibutyl phthalate were identified as the products of 2,4-dichlorophenol degradation by the microcapsules of immobilized laccase and laccase immobilized by a physical approach, respectively, further demonstrating the degradation mechanism of 2,4-dichlorophenol by microcapsule-immobilized laccase.     

Fe~0-厌氧微生物降解2,4-二氯酚的效应及机理

以2,4-二氯酚(2,4-DCP)为目标污染物,采用间歇试验,接种厌氧混合微生物,考察葡萄糖共基质条件下不同pH值时零价铁(Fe)0对2,4-DCP生物降解的效应,并对Fe0与厌氧微生物联合体系的作用机理进行探讨。结果表明:Fe0与厌氧微生物联合作用可提高2,4-DCP的降解效果,且中性或偏碱性环境下联合体系对目标污染物的促进效果较酸性环境明显,初始pH值为8时目标污染物的降解效果最好。Fe0在厌氧条件下腐蚀产生的OH-可有效平衡葡萄糖发酵产生的有机酸,使体系挥发性脂肪酸(VFA)的浓度维持在较低水平(300 mg/L),同时促使联合体系pH值上升从而利于目标物2,4-DCP的降解。Fe0在酸性环境的腐蚀较强,腐蚀产物以Fe2+为主,Fe3+含量较少。不同pH值时"Fe0+微生物"体系的COD去除率与目标物降解效果有一定相关性。     

Pd/TiO2对水体中2,4-二氯酚的催化加氢脱氯研究

分别采用沉淀-沉积法和浸渍法合成了Pd/TiO2催化剂,采用透射电镜(TEM)、X射线衍射(XRD)和电感耦合等离子体发射光谱(ICP-AES)对材料进行了表征,并对2,4-二氯酚的催化加氢脱氯反应进行了研究.结果表明,2种方法制备的催化剂在加氢脱氯反应中均具有较好的效果,沉淀-沉积法制备的催化剂活性更高,当反应物初始浓度为3.11 mmol.L-1,pH为12,催化剂用量为50 mg时,45 min内2,4-二氯酚可以完成脱氯过程.酸性条件有利于反应的进行.当催化剂用量在15～80 mg时,反应初活性没有明显变化,因此催化反应过程不受传质阻力的影响.当反应物初始浓度在0.62～3.11 mmol.L-1时反应初活性随浓度的提高显著增加,但进一步增加反应物的浓度时初活性没有明显提高,因此2,4-二氯酚在催化剂上的加氢脱氯行为符合Langmuir-Hinshelwood模型,表明2,4-二氯酚的加氢脱氯受表面吸附所控制.     

预处理方式对氧化-还原联合技术修复硝基苯污染地下水的影响

为了探究氧化与还原预处理对氧化-还原联合技术修复硝基苯污染地下水的影响,选取2,4-DNT（2,4-二硝基甲苯）为研究对象,构建过硫酸盐/铁炭修复技术体系,分别设置2个试验槽,一个试验槽以过硫酸盐作为氧化预处理联合以铁炭作为还原后处理,另一个试验槽以铁炭作为还原预处理联合以过硫酸盐作为氧化后处理,对比研究构建的氧化-还原联合系统中不同氧化与还原预处理方式对2,4-DNT去除机制的影响.结果表明:①过硫酸盐氧化材料填充位置显著影响试验槽pH和ORP（氧化还原电位）的变化,在运行周期5 PV（PV为孔隙体积,1 PV时间约为4 h）内,pH可显著增至11左右,ORP值达到最高.②在运行周期5 PV内,氧化填充层S₂O₈2-浓度和还原填充层Fe2+浓度均显著降低.③在运行周期5 PV内,随运行周期的增加,以过硫酸盐作为氧化预处理联合以铁炭作为还原后处理的协同技术体系对2,4-DNT的去除效果显著降低,以铁炭作为还原预处理联合以过硫酸盐作为氧化后处理的协同技术体系对2,4-DNT的去除率维持在100%.④通过液相-质谱联用技术,识别构建的氧化-还原联合技术体系内2,4-DNT降解的主要中间产物,同时结合铁炭微电解还原机制和过硫酸盐氧化机制提出了2,4-DNT协同处理机制及其可能的降解路径.研究显示,还原预处理更有利于氧化-还原联合技术对地下水中2,4-DNT的去除,可为有效处理硝基苯化合物污染地下水提供理论支撑.      

SPE- GC/MS法测定水中对硝基氯苯和2,4- 二硝基氯苯

采用SPE-GC/MS法测定水中对硝基氯苯和2,4-二硝基氯苯,优化了试验条件.对硝基氯苯在1.00 mg/L～80.0 mg/L之间线性关系良好,2,4-二硝基氯苯在1.00 mg/L～50.0 mg/L之间线性关系良好,方法检出限对硝基氯苯为0.6 μg/L,2,4-二硝基氯苯为2.1 μg/L,回收率对硝基氯苯为86.2%～94.7%,2,4-二硝基氯苯为87.3%～95.4%.