温度对厌氧氨氧化与反硝化耦合脱氮除碳的影响

采用ASBR反应器,研究了温度对厌氧氨氧化与反硝化耦合反应的短期影响.试验结果表明:耦合反应的活化能要小于单纯厌氧氨氧化反应的活化能,厌氧氨氧化与反硝化耦合反应可在一定程度上缓解低温对单纯厌氧氨氧化反应造成的消极影响,温度降低对厌氧氨氧化反应的影响大于对反硝化反应的影响.温度与耦合反应最大比反应速率的关系符合Arrhenius方程,在25~35℃时,耦合反应活化能为49.56kJ/mol,小于厌氧氨氧化反应的活化能66.18kJ/mol,且厌氧氨氧化反应为主导反应,对脱氮的贡献率约为61.29%.9~25℃时耦合反应的活化能为74.91kJ/mol,小于此温度梯度下厌氧氨氧化的活化能106.40kJ/mol,反硝化反应对脱氮的贡献率随温度的降低逐渐升高,9℃时,反硝化反应成为主导反应,对脱氮的贡献率约为75.10%.温度低于25℃时,反应器的容积氮去除速率(NRR)会受温度的影响.     

钙化合物的种类对脱氯特性的影响

以PVC为HCl的释放源，采用热重法对不同气氛下各种钙化合物的脱氯特性进行了研究，探讨了各种钙化物的脱氯机理以及脱氯效率。结果表明和PVC作为氯化氢的释放源是可行的。3种钙化物中氢氧化钙的脱氯效果最好。氧化钙与氢氧化钙的脱氯机理基本相似。各种钙化物在不同气氛下的脱氯机理是不同的。燃烧状态下，在高温段钙化物脱氯产物氯化钙有分解迹象。     

二甲胺盐酸盐与氯胺生成NDMA动力学研究

研究了二甲胺盐酸盐与氯胺反应生成N,N-亚硝基二甲胺（NDMA）的动力学.采用隔离法测定得到反应物浓度与时间的变化关系,进而采用尝试法求解反应级数、速率常数、速率方程和活化能.结果表明：对于二甲胺盐酸盐与氯胺反应生成中间体的第一步过程,反应物两者的反应级数均为一级,反应速率常数在5,15和25℃下分别为1.5361×10^-3,1.8707×10^-3,7.7217×10^-3mol^-1·min^-1,反应活化能Ea为51.27kJ/mol.由反应速率常数和活化能数值可以看出温度高有利于反应的进行.所得结果可为含二甲胺基及其同系物与氯胺整体反应的动力学研究,以及原水处理过程中消毒副产物NDMA生成风险的判定提供实验依据.     

低环多环芳烃(萘、苊)在活性炭上的热脱附行为

利用SETSYS Evolution 16型热重分析仪,在氮气气氛下分别研究了萘和苊在活性炭(AC)上的热脱附行为,并采用多升温速率法和单升温速率法相结合的方法,得到萘和苊在AC上的热脱附反应动力学方程及其动力学参数,结果表明:萘在AC上的热脱附反应动力学模型为Avrami-Erofeev方程,反应级数为1.5,脱附活化能(E)均值为63.38kJ/mol, lnA均值为11.75;苊在AC上的热脱附反应动力学模型亦为Avrami-Erofeev方程,反应级数为2, E均值为95.49kJ/mol, lnA均值为16.80.     

纳米Pd/Fe双金属对2,4-二氯酚的脱氯机理及动力学

采用纳米Pd Fe双金属对2,4 二氯酚(2,4 DCP)进行了催化还原脱氯处理.结果表明,纳米Pd Fe双金属具有较高的比表面积和反应活性,对2,4 DCP具有较好的脱氯效率.当纳米Pd Fe用量在6g·L-1时,2,4 DCP脱氯率达到90%以上;脱氯效率与pH值、温度、钯化率、Pd Fe投加量等因素有关.2,4 DCP在脱氯过程中先生成邻氯酚和对氯酚,而后继续脱氯生成苯酚,或由2,4 DCP直接降解成苯酚.2,4 DCP降解符合拟一级反应动力学.2,4 DCP催化还原脱氯反应的活化能为139 7kJ·mol-1.     

负载型纳米Pd/Fe对氯代烃脱氯机理研究

采用实验室制备的负载型纳米Pd/Fe对几种常见的挥发性氯代烃:四氯乙烯(ICE)、三氯乙烯(TCE)、1,1-二氯乙烯(1,1-DCE)、氯乙烯(VC)和林丹(γ-HCH)进行了还原脱氯研究.负载型纳米Pd/Fe对PCE、TCE、1,1-DCE、VC和γ-HCH的还原脱氯符合准一级反应动力学方程,其反应速率常数分别为2.79 h-1、2.35 h-1、1.12 h-1、2.14 h-1和4.02 h-1.氯代烃降解过程中几乎没有中间产物生成,终产物主要为C2 H6和C2 H4,如对TCE进行降解时,生成的C2H6和C2 H4分别占总碳质量比的70%和10%.采用暴露在空气中24 h的负载型纳米Pd/Fe对PCE进行脱氯,8次循环后仍能对PCE快速完全降解,表明负载型纳米Pd/Fe的稳定性能良好.以γ-HCH为目标污染物对负载型纳米Pd/Fe的反应持久性进行了研究,200 h后负载型纳米Pd/Fe的反应性没有明显降低,表明负载型纳米Pd/Fe反应持久性能良好.温度对负载型纳米Pd/Fe的脱氯反应影响较大,测得各氯代烃脱氯反应的活化能均高于29 kJ·mol-1.对PCE、TCE进行了脱氯动力学模拟,模拟结果与试验数据基本吻合,表明负载型纳米Pd/Fe对氯代烃的脱氯,是连串、平行及多步骤反应的结合.     

铬渣中六价铬水浸动力学研究

采用连续反应器,考察了铬渣水浸工艺参数,研究了铬渣中Cr(VI)的水浸动力学。结果表明,铬渣水浸过程速率为通过固膜的扩散所控制,通过对整个过程分阶段分别进行拟合,建立了Cr(VI)水浸过程的动力学模型,后阶段反应模型在α=0.05上显著,两个反应阶段表观活化能分别为18 kJ/mol和10.25 kJ/mol。     

高温煤气中氯化氢脱除反应动力学研究

在此对自制脱氯剂GH1与高温煤气中的氯化氢反应等温动力学与高温脱氯过程反应动力学进行了研究。等温动力学得出反应的反应级数为1,表观活化能为10.9kJmol。基于固定床反应器恒定模式行为,采用化学反应控制、产物层扩散控制及两种混合控制对脱氯过程的研究结果表明:自制脱氯剂GH1与高温煤气中的氯化氢气体的反应主要受化学反应控制,同时产物层的扩散控制是不容忽视的。     

粉煤灰碱浸出体系反应过程分析:Ⅱ反应动力学

文章利用Jander方程,对粉煤灰在强碱性条件下的反应动力学进行了研究。研究内容包括:动力学反应阶段的划分;温度对各动力学反应阶段的影响;动力学反应阶段与理论模型的关系以及各阶段反应活化能的计算等。研究结果表明:粉煤灰在碱浸出体系下的反应分为3个阶段,即表明反应阶段,早期扩散阶段以及中后期扩散阶段。各阶段的持续时间与反应温度有密切关系。根据热力学计算,表明反应阶段的活化能为102 kJ/mol,早期扩散阶段的活化能为66 kJ/mol。     

均相阳离子隔离阴阳极室电化学降解含酚废水实验及其动力学研究

在隔离阴阳极室的条件下进行电化学法降解含酚废水实验 ,结果表明 ,在 2 5～ 4 5℃的低温范围内 ,苯酚的转化率能达到 95 %以上。反应动力学研究揭示 ,其活化能Ea =12 75～ 16 0 6kJ mol,与一般化学反应的活化能Ea =6 0～2 5 0kJ mol相比 ,本实验的活化能很低 ,即反应所要克服的势能垒很低 ,反应更易进行 ,这是电化学脱酚速率快 ,降解彻底的重要原因 ;另外 ,不同电解液对比实验显示 ,降解苯酚时在碱性电解液中更为有效     

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.     

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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Organochlorine pesticides in soils under different land usage in the Taihu Lake region, China

A field study was conducted in the Taihu Lake region, China in 2004 to reveal the organochlorine pesticide concentrations in soils after the ban of these substances in the year 1983. Thirteen organochlorine pesticides (OCPs) were analyzed in soils from paddy field, tree land and fallow land. Total organochlorine pesticide residues were higher in agricultural soils than in uncultivated fallow land soils. Among all the pesticides, ΣDDX (DDD, DDE and DDT) had the highest concentration for all the soil samples, ranging from 3.10 ng/g to 166.55 ng/g with a mean value of 57.04 ng/g and followed by ΣHCH, ranging from 0.73 ng/g to 60.97 ng/g with a mean value of 24.06 ng/g. Dieldrin, endrin, HCB and α-endosulfan were also found in soils with less than 15 ng/g. Ratios of p,p'-(DDD DDE)/DDT in soils under three land usages were: paddy field ＞ tree land ＞ fallow land, indicating that land usage inlfuenced the degradation of DDT in soils. Ratios of p,p'-(DDD DDE)/DDT ＞1, showing aged residues of DDTs in soils of the Taihu Lake region. The results were discussed with data from a former study that showed very low actual concentrations of HCH and DDT in soils in the Taihu Lake region, but according to the chemical half-lives and their concentrations in soils in 1980s, the concentration of DDT in soils seemed to be underestimated. In any case our data show that the ban on the use of HCH and DDT resulted in a tremendous reduction of these pesticide residues in soils, but there are still high amounts of pesticide residues in soils, which need more remediation processes.     

Single and joint effects of pesticides and mercury on soil urease

The influence of two pesticides including chlorimuron-ethyl and furadan and mercury （Hg） on urease activity in 4 soils （meadow burozem and phaeozem） was investigated. The soils were exposed to various concentrations of the two pesticides and Hg individually and simultaneously. Results showed that there was a close relationship between urease activity and organic matter content in soil. Chlorimuron-ethyl and furadan could both activate urease in the 4 soils. The maximum increment of urease activity by chlorimuronethyl was up to 14%-18%. There was almost an equal increase （up to 13%-21%） in the urease activity by furadan. On the contrary, Hg markedly inhibited soil urease activity. A logarithmic equation was used to describe the relationship （P〈0.05） between the concentration of Hg and the activity of soil urease in the 4 tested soils. Semi-effect dose （ED50） values by the stress of Hg based on the inhibition of soil urease in the 4 soils were 88, 5.5, 24 and 20 mg/kg, respectively, according to the calculation of the corresponding equations. The interactive effect of chlorimuron-ethyl or furadan with metal Hg on soil urease was mainly synergic at the highest tested concentrations.