制备条件对硅胶负载氧化锆吸附除氟的影响

应用浸渍法制备了硅胶负载氧化锆除氟吸附剂,研究了焙烧温度、硅胶粒度、浸渍时间、浸渍温度、浸渍液浓度、浸渍固液比和浸渍次数等制备参数对吸附剂吸附容量的影响.实验发现焙烧温度有较大影响,450℃焙烧有最大的吸附量,再升高温度吸附量迅速下降.浸渍可在2h内达到平衡.浸渍温度越高,浸渍液浓度越高,则吸附容量越大.采用较高浓度一次浸渍优于低浓度多次浸渍.硅胶粒度和浸渍固液比也影响吸附量,粒度越大吸附量越小,粒度小于0.25mm后吸附量趋于稳定.     

负载镧镁活性氧化铝的制备及除氟性能研究

采用浸渍法制备负载镧镁活性氧化铝改性除氟剂,用于去除溶液中氟离子。通过正交实验考察镧镁摩尔比、焙烧温度和焙烧时间对改性活性氧化铝吸附性能的影响,得出最佳合成条件为镧、镁物质的量比1∶2,焙烧温度300℃,焙烧时间2.0 h。研究吸附时间、投加量、p H值和共存阴离子对氟离子吸附效果的影响。结果表明:吸附时间为3.0 h、投加量为3.6 mg/L,p H值在6~9,除氟效果最好,氟离子去除率为94.5%;对比不同阴离子对除氟性能的影响,除氟性能受阴离子影响力大小为:CO2-3>SO2-4>Cl->NO-3;吸附剂对氟离子的吸附过程符合伪二级动力学模型,吸附等温线满足Langmuir吸附等温式,其饱和吸附量为7.663 mg/g;不同温度下的热力学结果表明该反应为自发吸热反应。     

不同沉淀pH值条件下制备的水合氧化锆对水中磷酸盐的吸附作用

研究了沉淀pH值分别为4.8、8.0和10.6条件下制备的水合氧化锆对水中磷酸盐的吸附作用,结果表明,共存的Na~+仅仅略微促进了沉淀pH值为4.8和8.0时所得水合氧化锆对水中磷酸盐的吸附,却明显促进了沉淀pH值为10.6时所得水合氧化锆对磷酸盐的吸附.共存的Ca~(2+)仅仅略微促进了沉淀pH值为4.8时水合氧化锆对磷酸盐的吸附,却极大地促进了沉淀pH值为8.0和10.6时水合氧化锆对磷酸盐的吸附.共存的HCO_3~-和SO_4~(2-)抑制了水合氧化锆对磷酸盐的吸附,且它们对沉淀pH值为4.8时水合氧化锆吸磷的抑制作用明显大于对沉淀pH值为8.0和10.6时水合氧化锆的抑制作用.不同沉淀pH值条件下制备的水合氧化锆对水中磷酸盐的吸附能力均随着溶液pH值的增加而降低.不同沉淀pH值条件下所得水合氧化锆对水中磷酸盐的吸附平衡数据可以采用Langmuir、Freundlich和Dubinin-Redushckevich(D-R)等温吸附模型加以描述.存在Na+而不存在Ca~(2+)情况下,3种不同沉淀pH值条件下所得水合氧化锆对中性溶液中磷酸盐的最大单层吸附容量差别不大;存在Ca~(2+)情况下,沉淀pH值为8.0和10.6时所得水合氧化锆对中性溶液中磷酸盐的最大单层吸附容量远远高于沉淀pH值为4.8时制备的水合氧化锆.沉淀pH值为4.8和8.0时所得水合氧化锆的吸磷机制主要是表面氯和羟基基团与磷酸盐之间的配位体交换作用,而沉淀pH值为10.6时所得水合氧化锆的吸磷机制主要是表面羟基基团与磷酸盐之间的配位体交换作用.以上研究结果显示,与沉淀pH值为4.8时制备的水合氧化锆相比,沉淀pH值为8.0和10.6时制备的水合氧化锆更加适合作为吸附剂去除废水中的磷酸盐.     

活化赤泥除氟剂的制备及除氟性能试验研究

分别采用(NH4)2HPO4,NH4HCO3,NaHCO3等对赤泥进行活化处理,并制备成球形颗粒,同时研究了活化剂浓度、焙烧温度、焙烧时间等对赤泥除氟剂吸附性能的影响。结果表明：在活化剂质量浓度为10%左右、焙烧温度500℃,焙烧时间2 h时制备的除氟剂具有较好的除氟效果,且采用(NH4)2HPO4,NH4HCO3,NaHCO3对赤泥进行活化处理制备的除氟剂能分别使溶液中氟离子的质量浓度从19 mg/L分别降低到0.085,0.13及0.19 mg/L,相应地除氟剂的吸附容量均达0.94 mg/g以上。     

纳米氢氧化钛及焙烧产物对磷酸根的吸附特性研究

以纳米氢氧化钛(NTH)作为吸附水溶液中磷酸根的吸附剂,考察了NTH不同焙烧温度下的分子式及其对PO43-吸附效果的影响.选择PO43-初始浓度为50 mg/L,通过正交试验确定在pH=2、吸附剂用量为0.1g、吸附时间为40min、温度25℃时,NTH吸附效果达到最佳,吸附量为55.5 mg/g,经200、300、400及500℃焙烧后的NTH对磷酸根的吸附量逐渐减小;吸附量分别为494、40.6、25.5及16.8 mg/g;NTH经800℃焙烧后,焙烧产物TiO2不具有吸附性.TG、XRD分析表明随着焙烧温度的升高,NTH的表面活性基团(-OH)数量逐渐减少.结果表明,吸附剂的吸附性与吸附剂表面羟基的数量有直接关系.     

新型材料磁性氧化锆的除氟效能

采用一步共沉淀法制备了磁铁矿纳米颗粒为核和水合氧化锆为壳的磁性氧化锆材料,研究了其除氟性能.结果表明,磁性氧化锆对氟的Langmuir最大吸附量为35. 46 mg·g~(-1),远高于磁铁矿、活性氧化铝和活性炭.磁性氧化锆对氟的吸附过程较快且吸附动力学数据符合准二级动力学模型,吸附过程为吸热反应.磁性氧化锆对氟的吸附量随pH升高而降低. Cl~-、NO_3~-和SO_4~(2-)的共存对磁性氧化锆除氟没有明显影响,而HCO_3~-和CO_3~(2-)明显抑制氟的吸附.磁性氧化锆吸附的氟可通过1mol·L~(-1)NaOH成功脱附,脱附率99. 5%～99. 6%.脱附后的磁性氧化锆经过再生处理可继续使用.磁性氧化锆对实际井水中的氟的去除效果低于纯水,但适当增加投加量仍可以达到饮用水标准对氟浓度的要求.磁性氧化锆制备简单、使用后可从水中磁分离从而可反复使用,因此是一种有较好应用前景的除氟材料.     

稀土吸附剂对废水深度除磷研究

通过浸渍——干燥——焙烧法制备预载镧氧化物稀土吸附剂，探讨了该吸附剂对水中磷的吸附性能。研究表明在镧离子浓度为0．025mol／1、pH为10-11的溶液中浸渍，于500℃温度下焙烧制得的稀土吸附剂，其除磷效果可达95％。     

纳米氢氧化钛及焙烧产物对磷酸根的吸附特性研究

以纳米氢氧化钛(NTH)作为吸附水溶液中磷酸根的吸附剂,考察了NTH不同焙烧温度下的分子式及其对PO4吸附效果的影响。选择PO4初始浓度为50mg/L,通过正交试验确定在pH=2、吸附剂用量为0.1g、吸附时间3-3-为40min、温度25℃时,NTH吸附效果达到最佳,吸附量为55.5mg/g,经200、300、400及500℃焙烧后的NTH对磷酸根的吸附量逐渐减小;吸附量分别为49.4、40.6、25.5及16.8mg/g;NTH经800℃焙烧后,焙烧产物TiO2不具有吸附性。TG、XRD分析表明随着焙烧温度的升高,NTH的表面活性基团(-OH)数量逐渐减少。结果表明,吸附剂的吸附性与吸附剂表面羟基的数量有直接关系。     

微波辐射香草醛交联壳聚糖对镉(Ⅱ)的吸附性能

采用微波辐射技术合成了香草醛交联壳聚糖(V-CTS)希夫碱,用红外光谱和扫描电镜对产物结构进行了表征,研究了该吸附剂对镉离子的吸附性能。结果表明,香草醛改性壳聚糖粒径约在5~40μm之间,吸附剂对镉离子的的吸附条件是:pH为6.0,100 mg/LCd2+溶液50 mL,吸附剂投加量为0.02 g,吸附震荡时间5 h,温度20℃,吸附量为39.7 mg/g。与水浴法制备的吸附剂以及其他壳聚糖改性产品相比,该吸附剂的吸附量大大提高,且操作方法简单,工艺条件易于控制。     

类水滑石Mg/Zn/Al焙烧产物对高氯酸盐的吸附

利用类水滑石Mg/Zn/Al的焙烧产物对ClO-4进行吸附性能研究,通过类水滑石表面结构X射线衍射分析并探讨其吸附等温、动力学模型,并研究了焙烧温度、Mg/Zn/Al质量比、溶液pH值、吸附时间及吸附剂投加量等因素对类水滑石Mg/Zn/Al吸附ClO-4的性能影响.结果表明在500℃下焙烧4 h,Mg/Zn/Al质量比为2∶1∶1的类水滑石对ClO-4去除效果较好,吸附容量最大且对溶液pH值有较好的适用范围.经500℃焙烧的类水滑石吸附ClO-4的动力学拟合结果符合二级反应动力学模型,吸附等温线符合Langmuir及Freundlich吸附等温模型.     

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.     

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.     

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.     

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.     

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.     

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.     

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.     

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.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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