菲和铬(Ⅵ)单一及复合暴露对土壤微生物多样性的影响

有机物和重金属已成为我国土壤环境中常见的2类污染物质,二者间复合污染引起的土壤生态环境风险不容忽视。本研究以多环芳烃模式物菲和典型重金属铬(VI)作为受试物质,采用PCR-DGGE分子指纹图谱技术,探讨这2种污染物单一及复合暴露对土壤微生物群落多样性的影响,并选用主成分分析、聚类分析和戴斯系数3种算法对微生物群落相似性进行了比较。结果表明,在暴露实验第1天,菲单一暴露低浓度组中微生物群落相似性产生了极为明显的变化,而到第7天时,菲和铬(VI)单一暴露高浓度组均对微生物群落结构相似性产生最大程度的影响;采用香农指数法评价微生物群落的多样性,发现在暴露实验第7天,菲和铬(VI)单一暴露高浓度组对微生物群落多样性的影响比复合暴露高浓度组更强,二者复合暴露的相互作用方式表现为拮抗效应。本研究证明低浓度菲短期暴露的效应高于高浓度暴露结果,因而多环芳烃菲自身及其在复合暴露中所扮演的角色尤其值得关注。     

芳香烃菲与基因碱基的非共价结合及驱动机制

疏水芳香烃类化合物能够导致基因遗传性的变化,理解这些化合物对基因污染的前提是必须首先阐明污染物-基因碱基间相互作用及驱动机制.使用等温吸附-光纤固相萃取和定量-构效关系的方法,研究了模型化合物菲与4种基因碱基间的弱相互作用,并揭示了分子驱动机制.结果表明,p H=7.0条件下,腺嘌呤与菲间引力较弱;而鸟嘌呤、胞嘧啶和胸腺嘧啶对菲为分配吸附,引力较强.红外光谱和弱力等值面的分析表明,鸟嘌呤与腺嘌呤分子能够通过2组CN环(CN6环和5环)与菲的2个相互毗邻的苯核同时发生π-π引力作用;而胞嘧啶和胸腺嘧啶仅与菲弧角位置的碳原子通过电子"赠体-受体"发生静电引力作用.当环境体系变成酸性时,腺嘌呤对菲的吸附增强(分配,1/n=1),但胸腺嘧啶对菲的吸附变弱;碱性条件下,由于胞嘧啶和胸腺嘧啶存在羰基取代基,作为电子赠体的含氧嘧啶脱质子化,表面负电性增强,分子平面极化减弱,π电子更易于与菲弧角位的碳原子发生电子"赠体-受体"作用.能量计算的结果表明,对基因碱基作用位点的预测结果可信,属于自发的非共价成因的物理结合.该研究将为深入揭示芳香烃的基因污染提供理论基础,对于防治芳香烃污染、保障生态安全有重要意义.     

3种低分子量有机酸对紫色土吸附菲的影响

采用静态吸附实验,研究了3种低分子量有机酸(柠檬酸、苹果酸和草酸)对紫色土吸附菲的影响.结果表明紫色土吸附菲的动力学过程符合二级动力学模型,3种低分子量有机酸(LMWOAs)均能显著降低紫色土吸附菲的速率常数;线性吸附模型很好地描述了紫色土对菲的吸附热力学过程是以分配作用为主.当加入的3种LMWOAs浓度低于5 mmol·L~(-1)时,促进紫色土吸附菲;当LMWOAs浓度≥10 mmol·L~(-1)时,抑制紫色土吸附菲,抑制作用随LMWOAs浓度的增加而加强.当LMWOAs浓度为20 mmol·L~(-1)时,其抑制作用能力表现为柠檬酸草酸苹果酸,这与3种LMWOAs的分子结构和酸性强弱有关.与对照相比,随着LMWOAs浓度的增加,紫色土溶出的溶解性有机质(DOM)含量呈现先降低后升高的趋势,紫色土对菲的吸附量与土壤溶出的DOM含量呈负相关.     

酸化时间对磁性碳纳米管制备及吸附菲的影响

采用共沉淀法对混酸氧化的多壁碳纳米管（MWCNTs）进行磁化,形成了Fe₃O₄/MWCNTs磁性复合材料（MMWCNTs）.研究了酸化时间对MMWCNTs制备及其吸附水中菲性能的影响.结果表明：弱酸条件下吸附效果较好,MMWCNTs对水中菲的吸附在30min内快速上升,到60min时基本达到平衡,吸附过程符合准二级动力学模型.MMWCNTs对水中菲的饱和吸附量随酸化时间增加呈现先升高后降低的趋势.酸化7h后制备的MMWCNTs的饱和吸附量最大,达到17.56μg/mg.     

甘氨酸-β-环糊精对菲的增溶、解吸行为研究

为改善β-环糊精的水溶性,将β-环糊精和甘氨酸在碱性条件下用环氧氯丙烷连接起来,得到水溶性极好的甘氨酸-β-环糊精,研究了甘氨酸-β-环糊精对菲的增溶、解吸行为,考察了pH、甘氨酸-β-环糊精初始浓度、温度、不同环糊精类型对菲解吸的影响。结果表明,甘氨酸-β-环糊精对菲的增溶效果显著,其初始质量浓度为30 g/L时,对菲的增溶倍数可以达到近30倍;甘氨酸-β-环糊精对菲的解吸随pH的升高而降低;升高甘氨酸-β-环糊精初始浓度和温度有利于菲的解吸;甘氨酸-β-环糊精对菲的解吸好于α-环糊精和β-环糊精,甘氨酸-β-环糊精对菲污染土壤的解吸符合准二级动力学方程。该静态解吸研究可以为菲污染土壤的修复提供基础信息。     

Plant enhanced degradation of phenanthrene in the contaminated soil

The degradative characteristics ofphenanthrene, microbial biomass carbon, plate counts ofheterotrophic bacteria and most probable number （MPN） of phenanthrene degraders in non-rhizosphere or rhizosphere soils with uninoculating or inoculating phenanthrene degraders were measured. At the initial concentration of 20 mg phenanthrene/kg soil, the half-lives of phenanthrene in uninoculated non-rhizosphere soil, uninoculated rhizosphere soil, inoculated non-rhizosphere soil, and inoculated rhizosphere soil were measured to be 81.5, 47.8, 15.1 and 6.4 d, respectively, and corresponding kinetic data fitted first-order kinetics. The highest degradation rate of phenanthrene was observed in inoculated rhizosphere soil. The degradative characteristics of phenanthrene were closely related to the effects of vegetation on soil microbial process. Vegetation could enhance the magnitude of rhizosphere microbial communities, microbial biomass content, and heterotrophic bacterial community, but barely influence those community components responsible for phenanthrene degradation. Results suggested that combination of vegetation and inoculation with degrading microorganisms of target organic contaminants was a better pathway to enhance degradation of the organic contaminants in soil.     

Characterization and phylogenetic analysis of a phenanthrene-degrading strain isolated from oil-contaminated soil

Bacterium strain EVA17 was isolated from an oil-contaminated soil, and identified as Sphingomonas sp.based on analysis of 16S rDNA sequence, cellular fatty acid composition and physiological-chemical tests. The salicylate hydroxylase and catechol 2, 3-dioxygenase (C23O) were detected in cell-free lysates, suggesting a pathway for phenanthrene catabolism via salicylate and catechol. Alignment showed that both of the C23O and GST genes of the strain EVA17 had high similarity with homologues of strains from genus Sphingomonas. The phylogenetic analysis based on 16S rDNA and C23O gene sequence indicated that EVA17 should be classified into genus Sphingomonas, although the two phylogenetic trees were slightly different from each other. The results of co-amplification and sequence determination indicated that GST gene should be located upstream of the C230 gene.     

Effects of humic acid coatings on phenanthrene sorption to black carbon

Black carbon (BC) can strongly adsorb hydrophobic organic compounds (HOCs).The HOC sorption to coated BC could be attenuated in soil and sediment compared with that of the parent BC.To study the potential causes of the sorption attenuation,humic acid (HA) and BC were isolated.Phenanthrene (PHE) was selected as the representative of HOCs.BC was coated with the precipitated HA.The PHE sorption to the HA-coated BC was determined.The HA coatings on BC could result in the significant sorption attenuation of PHE to BC.The attenuation varied in different HA origin and was positively correlated to the aromaticity of HA.The attenuation could be explained by the direct competition between HA and PHE for the available sorption sites on BC and the reduction of the available sorption sites as a result of the pore blockage of BC caused by the HA coatings.Therefore,the HA coatings on BC was one potential cause of the attenuation of HOC sorption to BC in soil and sediment.     

有机粘土矿物对水中菲蒽混合物的吸附

选用长碳链季铵盐阳离子型表面活性剂十六烷三甲基溴化铵(HDTMA-Br)作为改性剂对天然粘土矿物进行改性。利用改性后的粘土矿物对混合污染物进行吸附/解吸实验,结果显示:HDTMA改性粘土矿物对混合溶液中菲、蒽及混合物的吸附等温线均呈线性,是分配作用结果;随着改性土用量的增加,其吸附量逐渐减小,对污染物的去除率逐渐增大,最后趋于平衡;有机粘土矿物吸附混合污染物后解吸率均在5%以下;将改性土对混合污染物的吸附与对单体污染物的吸附进行对照,改性土总的吸附量大大增加,基本是对单体污染物的吸附量之和。     

小麦细胞色素P450作为土壤污染生物标记物的研究

以小麦(Triticum acstivnm)为供试植物,建立了小麦细胞色素P450含量的测定方法.在此基础上,以草甸棕壤为供试土壤,菲为外源污染物,进行了菲污染暴露与P450含量的污染诱导量-效关系研究.比较了P450含量与超氧化物歧化酶(SOD)活性对污染诱导的敏感性.结果表明,当土壤菲浓度在1-8mg· kg-1范围内,P450总量分别为对照组的1.78,2.51,2.48和2.17倍,表现为诱导刺激效应,且P450含量与菲含量之间存在明显的剂量-效应关系(P=0.00).而同样浓度范围内,SOD活性变化与对照相比均无显著差异(P=0.168).