水环境中精神活性物质的分析方法及其应用研究

发布时间：2017-12-27 10:23

本文关键词：水环境中精神活性物质的分析方法及其应用研究　出处：《中国环境科学研究院》2017年硕士论文　论文类型：学位论文

【摘要】：精神活性物质是一类作用于人类中枢神经系统并能够使人形成瘾癖的麻醉药品和精神药品,会对使用者的身体和精神造成极大的伤害。毒品就是一种典型的精神活性物质。近年来,随着全球毒品制造、贩卖和滥用形势的加剧,精神活性物质源源不断地被排入到环境中。由于污水处理厂现有工艺对精神活性物质的去除率低,其随出水进入到自然水环境中,呈现"伪持续性"存在的现象,对生态环境和人体健康可能造成的危害应该引起足够重视。目前国内鲜见关于自然水体精神活性物质的污染水平、环境行为以及生态风险的报道。本研究以我国6种典型精神活性物质[METH(甲基苯丙胺)、AMP(苯丙胺)、KET(氯胺酮)、EPH(麻黄碱)、MC(甲卡西酮)和HY(羟亚胺)]为目标污染物,建立了基于固相萃取技术的主动采样方法,开发了基于薄膜扩散梯度技术(Diffusive gradients in thin-films,DGT)的原位被动采样方法。针对北京市城市河流,调查了其水环境中精神活性物质的污染现状和时空分布特征,并评估了其可能的生态环境风险。主要研究成果如下:(1)建立了固相萃取SPE方法同时测定水环境中的6种精神活性物质(METH、AMP、KET、EPH、MC和HY)。在不酸化样品的前提下,OasisMCX萃取柱对目标物质的萃取富集效果最好,洗脱剂选择含5%(V/V)氨水的甲醇溶液,精神活性物质的回收率可以达到61.0%-91.1%。方法检出限在0.30至0.80 ng/L之间,定量限范围为1.00-2.68 ng/L。(2)开发了薄膜扩散梯度DGT方法同时测定水环境中的5种精神活性物质(METH、AMP、KET、EPH和MC)。选择对目标物质吸附率较高且吸附速率明显较快的XAD凝胶作为DGT装置的吸附膜,选择聚醚砜膜(PES)作为DGT装置的滤膜;通过计算4种有机溶剂(甲醇、乙腈、含5%氨水的甲醇、含5%氨水的乙腈)对目标物质的洗脱效率,确定甲醇为METH、AMP和KET的最佳洗脱试剂,含5%氨水的乙腈为EPH和MC的最佳洗脱试剂;条件实验证明DGT装置在较宽的水环境pH和离子强度条件范围内具有适用性。吸附容量测试实验确定了 XAD吸附膜对目标物质METH、AMP、KET、EPH和MC的最大吸附量分别为57、45、92、83和93 μg/片。在25℃,目标物质的扩散系数(D值)在6.62×10-6-7.60×10-6cm2/s之间。在北京市城市水环境中精神活性物质浓度水平的应用调查中,通过对比DGT方法与SPE方法,验证了 DGT装置在测定实际水环境中精神活性物质浓度水平的可行性和准确性。(3)与国内外其他研究相比,北京市城市地表水中精神活性物质的污染浓度总体处于较低水平。从组成上来看,EPH和METH是在北京市城市地表水中分布较广泛且浓度较高的精神活性物质,其检出频率分别为94%-100%和65%-100%,浓度范围分别在n.d.-185.7ng/L和n.d.-99.5ng/L之间;从空间分布上来看,在城市人口密集、经济和娱乐业较发达地区(坝河、北小河、通惠河),METH和KET的环境浓度明显较高;从季节分布上来看,枯水期(冬季和春季)北京市城市水体中精神活性物质的浓度水平明显高于丰水期(夏季和秋季),其中冬季样品中精神活性物质的浓度总值最高(32.0-245.1 ng/L),夏季最低(0-140.2 ng/L)。(4)利用风险熵评价北京市地表水中典型精神活性物质的环境风险,计算得出目标药物的RQ值均小于0.1,表明其可能的环境风险较低。但是由于精神活性物质具有一定的极性和生物活性,其对水生生态系统可能产生威胁不容小觑。
[Abstract]:Psychoactive substances are a class of narcotic drugs and psychotropic substances that act on the central nervous system of the human body and can make people addicted. They will cause great harm to users' body and spirit. Drug is a typical psychoactive substance. In recent years, with the intensification of the global situation of drug manufacture, trafficking and abuse, psychoactive substances have been continuously discharged into the environment. Due to the low removal rate of psychoactive substances in wastewater treatment plants, it will enter the natural water environment with the effluent, showing a phenomenon of "pseudo persistence". The harm to the ecological environment and human health should be paid enough attention. At present, there are few reports on the pollution level, environmental behavior and ecological risk of the mental active substances in the natural water body. In this study, 6 typical psychoactive substances in China [METH (methamphetamine), AMP (amphetamine), KET (ketamine), EPH (Ma Huangjian), MC (methcathinone) and HY (hydroxyl imine)] as the target pollutant, the active sampling method of solid phase extraction technology based on the development of film diffusion based on the gradient technique (Diffusive gradients in thin-films, DGT) in-situ passive sampling method. In view of the urban river in Beijing, the pollution status and spatial and temporal distribution characteristics of mental active substances in water environment were investigated, and its possible ecological environmental risk was evaluated. The main research results are as follows: (1) a solid phase extraction SPE method has been established for the simultaneous determination of 6 kinds of psychoactive substances in water environment (METH, AMP, KET, EPH, MC and HY). On the premise of not acidifying samples, the OasisMCX extraction column has the best effect on the extraction and enrichment of target substances. The elution agent selects methanol solution containing 5% (V/V) ammonia water, and the recovery rate of psychoactive substances can reach 61.0%-91.1%. The detection limit was between 0.30 and 0.80 ng/L, and the limit of quantitative limit was 1.00-2.68 ng/L. (2) the thin film diffusion gradient DGT method was developed for the simultaneous determination of 5 kinds of psychoactive substances (METH, AMP, KET, EPH and MC) in the water environment. The selection of the target material higher adsorption rate and adsorption rate significantly faster XAD gel as adsorption film DGT device, selection of polyether sulfone (PES) as a membrane DGT device; through the calculation of 4 kinds of organic solvents (acetonitrile, methanol, acetonitrile containing 5% ammonia methanol containing 5% ammonia, the elution efficiency of target substance) sure, METH, AMP and KET methanol as the elution reagent, acetonitrile containing 5% ammonia for EPH and MC the best elution reagent; conditions of experiments prove that the DGT device has applicability in water environment pH and ionic strength of a wide range of conditions. The adsorption capacity test confirmed that the maximum adsorption capacity of XAD adsorption membrane for target substances METH, AMP, KET, EPH and MC were 57, 45, 92, 83 and 93 micron g/ respectively. At 25 C, the diffusion coefficient of the target material (D value) is between 6.62 * 10-6-7.60 * 10-6cm2/s. In the investigation of the concentration of mental active substances in the urban water environment of Beijing, the feasibility and accuracy of DGT device in determining the level of mental active substances in the actual water environment were verified by comparing the DGT method with the SPE method. (3) compared with other studies at home and abroad, the pollution concentration of the spiritual active substances in the surface water of Beijing city is at a lower level. From the point of view, EPH and METH are in the city of Beijing city surface water is widely distributed and the higher concentration of psychoactive substances, the detection frequency were 94%-100% and 65%-100% respectively, the concentration range between n.d.-185.7ng/L and n.d.-99.5ng/L; judging from the spatial distribution, in a densely populated city, developed economy and entertainment area (Ba River, North River, Tonghuihe, METH and KET) environmental concentration was higher; from seasonal distribution, dry season (winter and spring) concentration level of Beijing city spirit in water activity was significantly higher than that in wet season (summer and Autumn), the total concentration of psychoactive substance in the sample is highest in winter (32.0-245.1 ng/L), the lowest in summer (0-140.2 ng/L). (4) using risk entropy to evaluate the environmental risk of typical psychoactive substances in surface water of Beijing. The calculated RQ values of target drugs are all less than 0.1, indicating that their environmental risks are low. However, because of the polarity and biological activity of the psychoactive substances, it may not be underestimated for the possible threat to the aquatic ecosystem.
【学位授予单位】：中国环境科学研究院
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X52

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