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首页> 外文学位 >Devenir environnemental des antidepresseurs dans les rejets urbains par chromatographie liquide a haute performance couplee a la spectrometrie de masse en tandem.
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Devenir environnemental des antidepresseurs dans les rejets urbains par chromatographie liquide a haute performance couplee a la spectrometrie de masse en tandem.

机译：高效液相色谱-串联质谱联用分析城市废物中抗抑郁药的环境命运。

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摘要

Mood disorders such as depression, burn-out and anxiety have increased in our modern society. Increasing amounts of antidepressant prescriptions around the world are now suspected to be the main cause of the recent detection of traces of antidepressant residues within urban wastewaters. These so-called “emerging” substances that possess pharmacological activity towards neurotransmitter regulation in the brain have raised serious concerns from the scientific community.;The initial goal of the study was to better understand the fate of various classes of antidepressants present in different environmental matrices (e.g. surface waters, wastewaters, treatment sludge, and biological tissues) by developing novel reliable analytical methods that can detect, quantify and confirm antidepressants using high performance liquid chromatography coupled to tandem-mass spectrometry (LC-QqQMS, LC-QqToFMS).;A preliminary study completed at the Montreal sewage treatment plant (STP) confirmed the presence of six antidepressants and four N-desmethyl metabolites in raw sewage (2 – 330 ng L-1). For this primary treatment (physico-chemical), low removal rates (≤ 15%) were obtained. Concentrations of antidepressant close to 100 ng L-1 were also detected directly in the St. Lawrence River at 0.5 km of the effluent outfall.;A second study conducted at the same STP allowed the selective extraction of antidepressants in three biological tissues (e.g. liver, brain, and filet) dissected from juvenile brook trouts previously exposed to diluted untreated and treated effluents with ozone. Bioaccumulation of antidepressants was readily observed in fish tissues (0.08-10 ng g-1) for the specimens exposed to untreated effluent (20% v/v), with major distribution in liver and brain. During experiments, a significant correlation was established between the concentrations of three antidepressant detected in brain tissues and the activity of a selected biomarker of exposition (e.g. an N/K ATPase pump involved in the serotonin regulation) measured within dissected synaptosomes from trout exposed to effluents.;Investigation of estimated treatment removal efficiencies from various Canadian STPs operating different disinfection modes showed that secondary treatments (biological) were more efficient than primary (physico-chemical) to remove antidepressants (mean removal rates : 30%). The highest amounts detected in treated sludge (biosolids) were obtained respectively with citalopram (1033 ng g-1), venlafaxine (833 ng g-1), and amitriptyline (78 ng g-1). Experimental calculated sorption coefficients (Kd) of each antidepressant predicted fairly good sorption capacities for sertraline, desmethylsertraline, paroxetine, and fluoxetine to solid matters (log Kd > 4). Finally, an excellent mean removal rate of 88% was obtained after ozonation (5 mg L-1) of a primary effluent. However, the characterization of new N-oxide side-products (venlafaxine, desmethylvenlafaxine) in ozonized effluent by high-resolution mass spectrometry (LC-QqToFMS) highlighted the possibility of formation of multiple polar compounds with unknown toxicity.;Keywords: Antidepressants, metabolites, side-products, pharmaceuticals, wastewater, treated sludge, sewage treatment plants, ozone, liquid chromatography, tandem-mass spectrometry.
机译：在现代社会中，诸如抑郁，倦怠和焦虑之类的情绪障碍有所增加。现在怀疑全世界范围内抗抑郁药处方的增加是最近发现城市废水中痕量抗抑郁药残留的主要原因。这些对大脑中神经递质调节具有药理活性的所谓“新兴”物质引起了科学界的严重关注。该研究的最初目标是更好地了解存在于不同环境基质中的各种抗抑郁药的命运。 （例如地表水，废水，处理污泥和生物组织），通过开发新型可靠的分析方法，可以使用高效液相色谱-串联质谱（LC-QqQMS，LC-QqToFMS）检测，定量和确认抗抑郁药。蒙特利尔污水处理厂（STP）完成的一项初步研究证实，原污水（2 – 330 ng L-1）中存在6种抗抑郁药和4种N-去甲基代谢产物。对于这种初级处理（物理化学处理），去除率较低（≤15％）。在出水口0.5公里处的圣劳伦斯河中也直接检测到了约100 ng L-1的抗抑郁药浓度。在同一STP上进行的第二项研究允许在三种生物组织（例如肝脏）中选择性提取抗抑郁药，大脑和鱼片）从先前暴露于未经处理和经臭氧稀释的稀释水中的幼小河鳟中分离出来。暴露于未经处理的废水（20％v / v）的标本在鱼组织（0.08-10 ng g-1）中很容易观察到抗抑郁药的生物蓄积，主要分布在肝脏和大脑中。在实验过程中，在脑组织中检测到的三种抗抑郁药的浓度与暴露于鳟鱼的分离的突触小体中测得的所选生物标志物的活性（例如，参与血清素调节的N / K ATPase泵）之间存在显着相关性。 。;从采用不同消毒模式的各种加拿大STP估计的治疗去除效率的调查表明，二级治疗（生物）比初级治疗（物理化学）去除抗抑郁药的效率更高（平均去除率：30％）。用西酞普兰（1033 ng g-1），文拉法辛（833 ng g-1）和阿米替林（78 ng g-1）分别获得处理过的污泥（生物固体）中检测到的最高量。实验计算的每种抗抑郁药的吸附系数（Kd）预测了舍曲林，去甲基舍曲林，帕罗西汀和氟西汀对固体物质的吸附能力相当好（log Kd> 4）。最终，一次废水进行臭氧化处理（5 mg L-1）后，获得了88％的优异平均去除率。然而，通过高分辨率质谱（LC-QqToFMS）对臭氧化废水中新的N氧化物副产物（文拉法辛，去甲基文拉法辛）的表征突出了形成具有未知毒性的多种极性化合物的可能性;关键词：抗抑郁药，代谢物，副产品，药品，废水，处理后的污泥，污水处理厂，臭氧，液相色谱法，串联质谱法。

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  • 作者

    Lajeunesse, Andre.;

  • 作者单位

    Universite de Montreal (Canada).;

  • 授予单位 Universite de Montreal (Canada).;
  • 学科 Chemistry Analytical.;Engineering Environmental.
  • 学位 Ph.D.
  • 年度 2012
  • 页码 210 p.
  • 总页数 210
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 肿瘤学;
  • 关键词

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