生物强化系统微生物分子诊断技术的应用及新发展

现代分子生物技术的飞速发展及其在环境研究领域的应用，为生物强化技术的研究和发展提供了新方法和新思路。本文从生物强化系统特异微生物检测及定量化技术、生物强化系统微生物群落结构组成及动态演替规律研究、生物强化作用机制的分子生物学解析、生物强化菌的基因工程构建、生物强化系统微生物的安全释放及控制技术几方面，对生物强化系统微生物分子诊断技术的应用和发展作了较为全面的综述。     

高分子量高纯度阳离子聚丙烯酰胺的合成

以丙烯酰胺与丙烯酰氧乙基三甲基氯化铵为单体,在复合引发剂的作用下,选择水溶液共聚法合成高分子量与高纯度阳离子型聚丙烯酰胺(CPAM)。实验表明,有机偶氮引发剂A用量0.5‰、氧化还原引发剂用量0.45‰、还原剂与氧化剂摩尔比2∶1、反应体系pH为4与反应时间5 h条件下,CPAM分子量为1 042万,且溶解性好。通过对聚合物残单含量影响因素添加剂用量、反应时间的研究,结果表明,添加剂EDTA和增溶剂D对残留AM含量影响小,而苯甲酸钠对聚合物残留AM的含量影响显著;延长反应时间至7 h,残单含量可降低至0.27%,CPAM的纯度高。通过与国内外3种同类型产品进行对比,结果表明,自制产品的分子量明显高于其他产品,且残单含量比国内产品降低了50%～75%。     

阶式生物接触氧化对富营养化太湖水源水中溶解有机物的去除性能研究

构建阶式生物接触氧化反应器处理富营养化太湖水源水,对其净水效能进行研究。结果表明,在优化工况条件下,阶式生物氧化反应器的三阶对太湖水源水中DOC的累积去除率分别为34．4％、40．2％和47．5％,对BDOC的总去除率为68．4％,除生物降解外,填料拦截、生物吸附絮凝等物理、化学作用对去除原水中的DOC仍有重要作用。DOC分子量分级表明,太湖源水中含量最大的是分子量〈500Da的DOC,含量最小的是分子量在5k～500Da间的DOC。阶式生物接触氧化反应器对分子量〈500 Da的DOC的去除率在60％以上,而出水中5k～500 Da区间的DOC含量相比原水增加近1倍。     

Molecular docking: A potential tool to aid ecotoxicity testing in environmental risk assessment of pharmaceuticals

A cocktail of human pharmaceuticals pollute aquatic environments and there is considerable scientific uncertainty about the effects that this may have on aquatic organisms. Human drug target proteins can be highly conserved in non target species suggesting that similar modes of action (MoA) may occur. The aim of this work was to explore whether molecular docking offers a potential tool to predict the effects of pharmaceutical compounds on non target organisms. Three highly prescribed drugs, diclofenac, ibuprofen and levonorgestrel which regularly pollute freshwater environments were used as examples. Their primary drug targets are cyclooxygenase 2 (COX2) and progesterone receptor (PR). Molecular docking experiments were performed using these drugs and their primary drug target homologues for Danio rerio, Salmo salar, Oncorhynchus mykiss, Xenopus tropicalis, Xenopus laevis and Daphnia pulex. The results show that fish and frog COX2 enzymes are likely to bind diclofenac and ibuprofen in the same way as humans but that D. pulex would not. Binding will probably lead to inhibition of COX function and reduced prostaglandin production. Levonorgestrel was found to bind in the same binding pocket of the progesterone receptor in frogs and fish as the human form. This suggests implications for the fecundity of fish and frogs which are exposed to levonorgestrel. Chronic ecotoxicological effects of these drugs reported in the literature support these findings. Molecular docking may provide a valuable tool for ecotoxicity tests by guiding selection of test species and incorporating the MoA of drugs for relevant chronic test end points in environmental risk assessments.     

表面活性剂改性4A分子筛对Cr(VI)的吸附行为

采用浸渍法对4A分子筛进行表面改性,通过引入阳离子表面活性剂,使4A分子筛表面附着季铵型阳离子,并与反离子Br-形成\"阴离子交换膜\",从而促使更多的Cr(VI)阴离子通过离子交换吸附到改性4A分子筛上,通过X-射线衍射(XRD)和傅里叶变换红外光谱(FTIR)对样品的物相结构和组成进行表征分析。研究表明,表面活性剂的类型和疏水碳氢链结构会影响4A分子筛的吸附能力,十八烷基三甲基溴化铵(OTAB)碳氢链长,在分子筛表面形成的双分子层密,对Cr(VI)的吸附量最大。采用准一级、准二级、Elovich和Bangham动力学模型对六价铬的吸附数据进行拟合,其中准一级动力学方程最符合十八烷基三甲基溴化铵改性分子筛的吸附行为。同时,分别从Langmuir和Redlich-Peterson等温吸附模型获得六价铬的最大吸附量为13.98 mg/g,且改性分子筛以均一表面吸附为主。     

有机蒸气-空气分子扩散系数实测数据及分析

利用自行研发的气体扩散系数测试装置,测定了烷烃、环烷烃、芳香烃、含氧化合物（酯类、醇类、酮类等）等21种挥发性有机化合物在空气中的分子扩散系数。测定结果表明：互为同系物的有机化合物在相同温度下,分子扩散系数随着分子链的增长而减小,与其沸点呈负相关;互为同分异构体的有机化合物在相同温度下,有支链的分子扩散系数比没有支链的要大。另外,将实验实测值与FSG方程计算值以及文献值进行了对比分析。通过比较实测值与计算值,认为大部分分子结构全部为单键并且不含环状结构的有机化合物的实测值与计算值吻合度比较高,但分子结构中含苯环、碳环和烷烃支链的有机化合物,实测值与计算值吻合度不是很高。建议FSG方程进一步考虑分子结构差异性的影响。     

Modelling the environmental degradation of water contaminants. Kinetics and mechanism of the riboflavin-sensitised-photooxidation of phenolic compounds

The aerobic visible-light-photosensitised irradiation of methanolic solutions of either of the phenolic-type contaminants model compounds (ArOH) p-phenylphenol (PP), p-nitrophenol (NP) and phenol (Ph), and for two additional phenolic derivatives, namely p-chlorophenol (ClP) and p-methoxyphenol (MeOP), used in some experiments, was carried out. Employing the natural pigment riboflavin (Rf) as a sensitiser, the degradation of both the ArOH and the very sensitiser was observed. A complex mechanism, common for all the ArOH studied, operates. It involves superoxide radical anion (O₂^√−) and singlet molecular oxygen (O₂(¹Δ_g)) reactions. Maintaining Rf in sensitising concentrations levels (≈0.02 mM), the mechanism is highly dependent on the concentration of the ArOH. Kinetic experiments of oxygen and substrate consumption, static fluorescence, laser flash photolysis and time-resolved phosophorescence detection of O₂(¹Δ_g) demonstrate that at ArOH concentrations in the order of 10 mM, no chemical transformation occurs due to the complete quenching of Rf singlet excited state. When ArOH is present in concentrations in the order of mM or lower, O₂^√− is generated from the corresponding Rf radical anion, which is produced by electron transfer reaction from the ArOH to triplet excited Rf. The determined reaction rate constants for this step show a fairly good correlation with the electron-donor capabilities for Ph, PP, NP, ClP and MeOP. In this context, the main oxidative species is O₂^√−, since O₂(¹Δ_g) is quenched in an exclusive physical fashion by the ArOH. The production of O₂^√− regenerates Rf impeding the total degradation of the sensitiser. This kinetic scheme could partially model the fate of ArOH in aquatic media containing natural photosensitisers, under environmental conditions.     

溶解性有机物与活性氯物种反应过程中其分子组成对消毒副产物生成的影响

溶解性有机物(DOM)在紫外/氯(胺)高级处理过程中会与活性氯物种(Cl^•和Cl₂^•−)反应生成消毒副产物(DBPs),进而影响水质的毒性和安全性。本研究详细研究了单一活性氯物种(Cl^•或Cl₂^•−)与不同来源DOM反应生成DBPs的情况,重点探究了DOM分子组成与生成DBPs质量浓度、种类、毒性之间的相关关系。结果表明：Cl^•与DOM反应过程中主要生成的DBPs及毒性贡献者分别为三卤甲烷(THMs)和卤乙醛(HALs)。DOM的分子组成与生成DBPs的质量浓度、种类及毒性之间相关性较低,这可能归因于Cl^•与不同DOM之间相似的反应活性,而在Cl₂^•−与DOM反应过程中HAAs和非管制类DBPs分别为主要生成的DBPs和毒性贡献者。此外,生成DBPs的质量浓度、种类及体系的毒性与DOM分子的不饱和度、芳香度、含氧量、极性呈负相关,与DOM中含N、S、P官能团化合物的相对含量呈正相关。本研究推动了DOM在单一活性氯物种介导下生成DBPs的研究,并为高级氧化工艺参数的优化及高毒性副产物的消减提供依据。     

活性艳橙K-7R分子印迹聚合物微球的制备及结合特性研究

以微米级聚苯乙烯微球为种球,活性艳橙K-7R为模板分子,甲基丙烯酸为功能单体,乙二醇二甲基丙烯酸酯为交联剂,采用单步溶胀聚合法在水相中制得了分子印迹聚合物微球(MIPs),并用平衡吸附实验研究了其吸附性能。通过Scatchard分析,结果表明,MIPs在识别K-7R过程中存在两类结合位点,高亲和力结合位点的平衡离解常数Kd1=14.855μmol/L,最大结合量Qmax1=1.282μmol/g;低亲和力结合位点的平衡离解常数Kd2=70.939μmol/L,最大结合量Qmax2=3.930μmol/g。该MIPs对K-7R有较高的亲和性和选择性。