对苯二酚强化多相类-Fenton过程降解活性艳红MX-5B的效能与机理

用碱沉淀法制备的硅羟基氧化铁(Si-FeOOH)作多相类-Fenton反应的催化剂,探讨了室温条件下投加还原剂对苯二酚(HQ)对其催化H2O2降解活性艳红MX-5B的影响,同时考察了pH、H2O2浓度、催化剂Si-FeOOH投量及活性艳红浓度对活性艳红MX-5B脱色率的影响,并从溶铁量方面初步探讨了Si-FeOOH/H2O2/HQ体系降解活性艳红MX-5B的机理.结果表明,对苯二酚强化以Si-FeOOH为催化剂的多相类-Fenton反应降解活性艳红的效果显著.在pH=3,活性艳红初始浓度为10mg·L-1,对苯二酚浓度为0.55mg·L-1,Si-FeOOH投量为100mg·L-1,H2O2浓度为51mg·L-1的反应条件下,活性艳红MX-5B的脱色率达94.69%.研究还发现,活性艳红脱色率与反应体系里的铁离子浓度关系密切,表明多相类-Fenton反应中除了催化剂表面吸附催化作用外,也可能存在类似均相类-Fenton的溶液催化作用.     

Si-FeOOH催化臭氧氧化降解活性艳红MX-5B的效能研究

通过共沉淀的方法在羟基氧化铁(FeOOH)合成过程中掺入硅(Si)来制备硅羟基氧化铁(Si-FeOOH)催化剂,比较其与FeOOH在物理强度等方面的差异,同时研究Si-FeOOH催化臭氧氧化降解活性艳红的效能、推断反应机理、考察各种因素对脱色率的影响.结果表明:相对于FeOOH,Si-FeOOH的物理强度有所提高,在水溶液中不易破碎;Si-FeOOH催化臭氧氧化降解活性艳红效果显著,比单独臭氧氧化的脱色率有较大提高;催化过程遵循自由基反应机理;脱色率随着臭氧浓度的增加而升高,在应用Si-FeOOH催化臭氧对染料脱色时存在最佳催化剂投量;Si-FeOOH在中性条件下其催化活性显著,催化剂性能稳定,可重复利用.     

絮凝污泥制备光催化剂及降解活性艳红K-2BP研究

利用絮凝污泥制备复合光催化剂,研究了其对模拟染料废水活性艳红K-2BP的光催化降解效率,并采用X射线衍射仪对其进行了结果表征。详细考察了催化剂煅烧温度、催化剂中钛含量、催化剂投加量、溶液pH值等不同条件对活性艳红K-2BP染料废水的光催化降解效果。实验结果表明,聚硅硫酸钛的n(Ti)∶n(Si)=5∶1,投加量为200mg/L,絮凝pH=5时的絮凝污泥在600℃煅烧2h制得复合光催化剂具有较高活性,当复合光催化剂投加量为500mg/L,光催化反应pH为4时光催化活性最好,此时对50mg/L的活性艳红K-2BP的降解率可达到97.2%。     

UV/Si-FeOOH/H_2O_2氧化降解水中邻苯二甲酸二甲酯

通过Si掺杂方式自制无定型Si-FeOOH催化剂,并将其用于UV/Si-FeOOH/H2O2光解体系降解内分泌干扰物邻苯二甲酸二甲酯(DMP),通过XRD、IR和SEM测试研究了Si-FeOOH的晶相结构,并与普通FeOOH进行铁溶出对比,研究pH值等因素对Si-FeOOH表面吸附和对协同体系降解DMP效能的影响.结果表明,通过Si掺杂所制得的Si-FeOOH为无定型结构,比表面积大,铁溶出率低;在Si/Fe摩尔比为0.2的Si-FeOOH投量为0.5 g/L,pH=5.0,H2O2浓度为2.0 mmol/L,125 W UV365条件下,DMP的降解效果显著,30 min内DMP降解率达到97%.与单一方法相比,UV、Si-FeOOH、H2O2三者的协同作用使得光-类Fenton可有效降解水中DMP,Si-FeOOH经多次循环使用后仍有较好的催化活性.     

非均相催化氧化处理活性艳红染料废水

以粉煤灰作为载体,制备了非均相催化剂。研究了非均相催化氧化处理98mg·L^-1活性艳红模拟染料废水的实验效果。实验结果表明,在催化剂投加量40g·L^-1、30％的H2O2投加量3mL·L^-1、pH值4、处理时间10min的最佳处理条件下,非均相催化体系对活性艳红染料的脱色率达到98．21％。对比均相催化氧化法,非均相催化氧化技术提高了对活性艳红染料的脱色率,缩短了反应时间,提高了H2O2利用效率,扩大了pH值范围,改进了Fe^2＋流失的不足。     

新生MnO2对水中活性艳红K-2G的脱色作用研究

以化学法合成的新生MnO2作吸附剂，对水中活性艳红K－2G进行吸附脱色研究，探讨了影响吸附的因素和吸附机理，结果表明：新生MnO2对活性艳红K－2G的吸附符合Langmuir吸附等温式，吸附前溶液pH值是影响染料脱色效果的最主要因素，染料浓度，MnO2投加量和温度影响程度较小，在实验条件下可使活性艳红K－2G的脱色率高达96％。     

水射流空化强化光催化处理活性艳红模拟废水

采用水射流空化强化TiO2光催化处理活性艳红X-3B模拟废水3.3 L,进行了自来水与蒸馏水的效果比较并初步研究了反应温度、催化剂投加量、溶液pH、染料初始质量浓度以及空化管喉管直径对染料去除率的影响。针对模拟废水,实验结果表明:该工艺克服了传统光催化技术中催化剂容易团聚的不足,使反应能够持续进行。溶剂全部为蒸馏水的脱色率和表观反应动力学常数分别是溶剂全部为自来水的2.1倍和4.2倍。在最优条件下:染料初始质量浓度30 mg/L,pH 3.0,温度60℃,TiO2投加量150 mg/L,反应进行90 min后染料脱色率可以达到96%。而在结合实际情况优化后的推荐值下,pH 6.0,温度40℃,空化管喉管直径选用1.5mm,其它条件不变,染料脱色率及COD去除率分别为69%和54%,该结果更能指导实践。     

Fenton试剂处理水中偶氮染料的影响因素研究

以水溶液中偶氮染料活性艳红X-3B为目标物,通过废水色度的变化考察了过氧化氢、亚铁离子投加量和pH值对废水处理效果的影响。实验结果表明:当染料浓度为200mg/L,pH值为4.0,FeSO4为0.10mmol/L,H2O2为1.2mmol/L时反应30min后,活性艳红X-3B的色度去除率达到最大值,为88.9%,处理效果较好。     

以海泡石为载体的双金属多相类芬顿催化剂的制备及表征

以活性艳蓝为目标污染物,以改性海泡石为载体,以Fe(NO3)3浓度、MnSO4浓度、尿素浓度、水浴温度、煅烧温度与煅烧时间为影响因素,优化了均匀沉淀法制备双金属多相类芬顿催化剂的工艺条件,并利用SEM、XRD、FTIR对催化剂进行了表征.结果表明,随铁离子浓度的增大,所制得催化剂金属离子活性越高.少量的锰掺杂可抑制Fe2O3粒径的增长,提高催化剂的活性.尿素浓度增大,使得晶粒的生成速率愈快,有利于生成细小、均匀的金属颗粒.利用Box-Behnken实验得出催化剂制备的最佳工艺条件为:硝酸铁浓度为0.18 mol.L-1,硫酸锰浓度为0.05 mol.L-1,尿素的浓度为1.0 mol.L-1,海泡石的投加量为40 g.L-1,水浴温度为100℃,煅烧温度为370℃,煅烧时间为3 h.SEM表明本实验所采用的海泡石为α型海泡石,可作为良好的催化剂载体;在催化剂制得后,FTIR图谱显示海泡石的纯度得到提高,并出现了Fe-O的吸收峰.XRD图谱表明,在催化剂表面铁离子主要以α-Fe2O3和γ-Fe2O3的形式存在.     

凹凸棒石基复合材料处理印染废水的研究

以凹凸棒石为载体,钛酸四丁酯为原料,通过溶胶-凝胶法,制成TiO2/凹凸棒石基复合材料(TiO2/ATT),并对所制得的复合材料进行了XRD和BET表征。在波长为254 nm的16 W紫外灯光照下,以活性黑KN-B印染废水为脱色对象,分别探讨了TiO2/凹凸棒石复合材料的煅烧温度、投加量、活性黑KN-B染料的初始浓度、溶液的pH值和反应温度等因素对印染废水脱色率的影响。实验结果表明:用煅烧温度500℃的TiO2/凹凸棒石基复合材料处理活性黑KN-B印染废水,催化剂的投加量为15 g/L、活性黑KN-B的初始浓度为10 mg/L、pH小于7、反应温度为20℃时,光催化反应4 h内即能达到较高的去除率,对活性黑KN-B的脱色率可达95%以上。     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Degradation of metabolites accumulated of benzo[a]pyrene by coupling Penicillium Chrysogenum with KMnO4

Several main metabolites of benzo[a]pyrene （BaP） formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone （BP 1,6- quinone）, trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene （BP 7,8-diol）, 3-hydroxybenzo[a]pyrene （3-OHBP）, were identified by high-performance liquid chromatography （HPLC）. The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that （1） the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; （2） the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; （3） the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% （w/v）, concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.     

基于综合水质标识指数和对应分析法的校园河道水质评价

以三峡大学的校园河道求索溪为研究对象,利用综合水质标识指数法确定求索溪水质类别,分析其水质时空变化规律,并利用对应分析法得出求索溪中不同监测点的主要污染因子.研究结果表明:求索溪整体的综合水质标识指数为7.423,整体水质为劣V类(地表水环境质量标准GB 3838-2002)且黑臭.从时间变化来看,求索溪4月份的水质最差,5月份次之,4、5月份所有监测点的水质都劣于V类且黑臭;8月份水质最好,水质为Ⅳ类;从空间分布来看,8个监测点综合水质标识指数均超过6.0,水质为劣V类,其中6号监测点的水质相对最好,监测点3号的水质相对最差;对应分析法得出求索溪的整体水体污染程度受总氮因子的影响最大,其次为总磷.该研究拟为求索溪及类似校园河道的水环境治理研究提供基础依据和参考.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.