河口有机物在固-液界面迁移转化研究进展

河口复杂的水动力条件和丰富的泥沙含量,使得河口水体中固-液界面过程成为控制河口有机物迁移转化的关键环节.本文总结了有机物固-液界面吸附机理以及河口区有机物在悬浮物-水界面、沉积物-水界面的迁移转化,并对今后研究工作提出几点看法.     

固液界面吸附机制与模型——“环境水质学前沿专栏”序言

固液界面吸附是环境水化学及水处理技术研究中的一项重要内容.本文阐述了目前固液界面吸附研究方面取得的主要进展,对吸附剂表面性质、吸附络合物形态、表面反应描述中使用的一些重要实验技术、理论计算方法和模型模拟手段进行了系统的介绍,并展望了固液界面吸附研究的发展趋势.表面表征技术、理论计算及表面络合模型的发展、应用和结合有力地促进了人们对各种固液界面体系吸附机制的深入理解,对于阐明污染物在水环境中迁移转化规律,及开发新型吸附剂有着重要的科学意义.     

土壤环境微界面过程与污染控制

土壤环境微界面是土壤组分(矿物和有机质)、植物根系、微生物等微界面的集合体和动态变化的连续体.土壤胶体微界面可理解为土壤固/液界面的双电层结构.这些动态变化的异质微界面,按其表面结构特点可分为硅氧烷型表面、水合氧化物型表面和有机物表面.环境污染物在土壤胶体微界面的迁移转化是污染物在土壤固-液界面反应的动态平衡过程,包括吸附/解吸、沉淀/溶解、络合/螯合、氧化/还原等反应.植物根际是植物与土壤组分和微生物相互作用的活跃区域,根际微界面决定着污染物向植物根系的运输、植物吸收及转运,为污染物经土壤向食物链传递的主要通道.根际微生物在重金属离子的吸附和氧化、还原、转化,以及有机污染物的降解和转化中起重要作用.这些异质微界面相互关联、相互作用,在土壤环境中构成微界面的连续体,决定着污染物在土壤环境中的赋存形态、生物有效性和向其它环境介质(如水体和植物)的迁移,因而在土壤污染控制和污染土壤修复中具有特别重要的意义.土壤环境微界面过程的研究已成为环境科学的研究前沿,值得引起土壤环境科学工作者的重视,并进行系统而深入的研究.     

有机污染物界面行为调控技术及其应用

污染物的多介质/多界面行为影响其赋存状态、迁移转化及生物生态效应.阐明污染物界面行为及其调控技术原理,是准确认识污染物源汇机制、预测其生物有效性、发展污染控制新材料与新技术的重要基础.本文介绍了典型有机污染物的多介质界面行为及其微观机制,表面活性剂调控有机污染物固-液界面分配行为及生物有效性的基本原理,重点阐述了污染物界面行为调控技术在难降解有机废水吸附处理、土壤有机污染缓解与修复中的应用.     

铝氧化物-水界面化学及其在水处理中的应用

天然水体中,铝氧化物矿物表面上的吸附等各种反应在很大程度上影响着金属阳离子、无机阴离子和一些天然有机物的迁移转化和归趋.在水处理等工业领域中,铝氧化物由于其水合表面的吸附能力而被用做离子交换剂和催化剂载体.因此,对铝氧化物表面化学过程的研究具有重要意义.铝氧化物-水界面上的反应十分复杂,对各种无机、有机污染物的吸附结合能力取决于氧化物固相表面性质、溶液条件和吸附质的性质.从对铝氧化物表面荷电特性和吸附活性的认识出发,就各种铝氧化物的结构特征和表面反应活性及其在水处理技术中的应用进行了简要综述.     

环境微界面过程的原位和在线研究方法

环境微界面过程是污染物在各环境要素中迁移转化的基本过程,也是研究污染控制方法的基础.发展原位和在线研究方法,对于揭示污染物在环境微界面的迁移转化规律和进行污染控制过程的研究具有重要意义.本文基于环境微界面过程的基本特征,在针对多相环境催化的原位研究方法基础上,分析了用于环境微界面过程的原位和在线研究方法所面临的挑战和相应对策,主要介绍了红外光谱、拉曼光谱和质谱等技术在气固环境微界面过程原位研究中的应用,提出了发展环境微界面过程原位和在线研究方法体系的构想.     

土壤-植物系统中的微界面过程及其生态环境效应

土壤 植物系统是地球生态系统中与人类生存与健康关系最为密切的亚系统 .该系统中的水分、养分 污染物的运移必须历经土壤固 液界面、根土界面 (根际微环境 )、细胞跨膜运输和植物体内不同组织和细胞内不同组分间的再分配等微界面过程 .这些微界面过程涉及到系统中许多生物、生物化学和物理化学反应机理 ,与植物对土壤中养分高效利用、污染物迁移转化及其归宿具有密切的关系 .理解这些微界面过程对提高农作物生长、改善土壤环境质量和提高农产品安全品质具有直接的理论和实践指导意义     

铊在矿物胶体和天然有机质界面上迁移转化行为的研究进展

铊(Tl)是典型的毒害重金属元素之一,对生物体的毒性高于Hg、Cd和Pb等元素。铊在天然水环境相关介质中的背景含量较低,但可通过各种工业活动大量进入水体环境,借由水体迅速迁移扩散,对生态系统造成巨大的环境隐患。本文总结了铊在水体中的分布特征,并重点阐述了铊在矿物胶体和天然有机质(腐殖酸)等界面上迁移转化行为的研究进展。研究表明,铁(氢)氧化物、锰(氢)氧化物均能在一定程度上吸附水体中的Tl(I),铊在一些锰(氢)氧化物表面的吸附行为可能会涉及Tl(I)在矿物表面的氧化还原机制。矿物表面对铊离子的吸附作用不仅与矿物的组成成分有关,还可能与矿物组成成分的晶型结构密切相关。天然有机质对铊迁移转化影响作用的研究目前主要偏重天然腐殖酸对铊的络合作用。因此,要加强的研究铊分别在不同种类、不同晶型的矿物和不同类型的天然有机质界面上的迁移转化行为,并借助高精度的价态和结构分析手段从分子水平上探讨其迁移转化机理。了解铊在水体中的迁移转化有助于深入认识铊的环境地球化学行为,并为研究铊的污染治理提供理论基础。     

汞(Ⅱ)-有机物-悬浮物体系的吸附行为和电泳特征的探讨

本文研究了Hg(Ⅱ)-HS—CH_2—COOH—OH—α-Al_2O_3悬浮体系的吸附行为和电泳特征.通过Gouy-Chapman和Healy模化处理,揭示了α-Al_2O_3微粒固-液界面双电层电荷密度和厚度的分布状况.以Healy模型拟合实验吸附曲线的结果,从热力学的角度,提出了吸附反应存在库仑吸附和化学吸附两种途径.计算结果与实验曲线拟合较好.运用ESCA技术,观察到固-液界面的成键效应.     

利用壳聚糖溶液探讨黄土中铬(VI)的提取效果研究

铬是环境中一种重要的重金属污染物,大量含铬的废水、废渣随意排放导致土壤、水体和生物遭到不同程度的污染.中国黄土分布面积广泛,本研究以典型的西部黄土为对象,通过室内土柱淋滤试验,以灌水量和示踪铬浓度为控制因子,研究铬在黄土层中的分布、迁移转化规律及黄土对铬的吸附特性.由于壳聚糖的结构中含有大量的-NH2和-OH,因此壳聚糖,它对重金属离子有优良的吸附作用.探讨了吸附时间、壳聚糖浓度、pH、液固比、温度对壳聚糖吸附黄土中Cr(VI)的提取效果.     

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.     

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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Isolation and preliminary characterization of a 3-chlorobenzoate degrading bacteria

A study was conducted to compare the diversity of 2-, 3-, and 4-chlorobenzoate degraders in two pristine soils and one contaminated sewage sludge. These samples contained strikingly different populations of mono-chlorobenzoate degraders. Although fewer cultures were isolated in the uncontaminated soils than contaminated one, the ability of microbial populations to mineralize chlorobenzoate was widespread. The 3- and 4-chlorobenzoate degraders were more diverse than the 2-chlorobenzoate degraders. One of the strains isolated from the sewage sludge was obtained. Based on its phenotype, chemotaxonomic properties and 16S rRNA gene, the organism S-7 was classified as Rhodococcus erythropolis. The strain can grow at temperature from 4 to 37℃. It can utilize several （halo）aromatic compounds. Moreover, strain S-7 can grow and use 3-chlorobenzoate as sole carbon source in a temperatures range of 10-30℃ with stoichiometric release of chloride ions. The psychrotolerant ability was significant for bioremediation in low temperature regions. Catechol and chlorocatechol 1,2-dioxygenase activities were present in cell free extracts of the strain, but no （chloro）catechol 2,3- dioxygenase activities was detected. Spectral conversion assays with extracts from R. erythropolis S-7 showed accumulation of a compound with a similar UV spectrum as chloro-cis,cis-muconate from 3-chlorobenzoate. On the basis of these results, we proposed that S-7 degraded 3-chlorobenzoate through the modified ortho-cleave pathway.     

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.     

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.     

Alterations of organ histopathology and metallolhionein mRNA expression in silver barb, Puntius gonionotus during subchronic cadmium exposure

Common silver barb,Puntius gonionotus,exposed to the nominal concentration of 0.06 mg/L Cd for 60 d,were assessed for histopathological alterations(gills,liver and kidney),metal accumulation,and metallothionein(MT)mRNA expression.Fish exhibited pathological symptoms such as hypertrophy and hyperplasia of primary and secondary gill lamellae,vacuolization in hepatocytes,and prominent tubular and glomerular damage in the kidney.In addition,kidney accumulated the highest content of cadmium,more than gills and liver.Expression of MT mRNA was increased in both liver and kidney of treated fish.Hepatic MT levels remained high after fish were removed to Cd-free water.In contrast,MT expression in kidney was peaked after 28 d of treatment and drastically dropped when fish were removed to Cd-free water.The high concentrations of Cd in hepatic tissues indicated an accumulation site or permanent damage on this tissue.