药物和个人护理用品(PPCPs)在环境介质中的广泛分布可能会对生态系统以及人体健康造成危害。精神药物作为PPCPs中的重要一类，近年来引起了大家的广泛关注。这类药物在污水厂出水、地表水、地下水、饮用水、土壤甚至动植物体内都有检出。能够掌握精神药物在环境中的分布、迁移转化规律、生态风险、主要污染源以及处理方法，对控制该类药物的污染水平和降低其对生态环境及人体健康造成的毒害至关重要。本文通过对上海城市水体系统(污水厂污水、黄浦江地表水、居民饮用水)和精神病医院剧边环境介质(医院出水、地表水、地下水、土壤、植被)进行实测和分析，筛选典型精神药物，研究了该类药物在典型城市水体系统的迁移转化规律以及精神病医院作为点污染源对周边环境的影响；同时探讨了不同碳材料对典型精神药物的吸附去除效果及吸附机理。具体研究内容如下： I 建立环境中精神药物痕量分析方法 基于高效液相色谱与质谱联用仪(HPLC-MS/MS)高灵敏度、高分辨率以及优越的选择性，通过对色谱条件和质谱参数的优化，建立了环境中15种精神药物痕量分析方法。在样品前处理方面，对于固体环境样品(土壤、植被)本研究采用了超声萃取联合固相萃取(SPE)前处理方法，针对液体样品(污水、地表水、地下水、饮用水)选择并优化了固相萃取方法，使得样品回收率、方法检测限(<5ng/L)以及方法的精确度和准确性都能满足实际研究的需求。 II 精神药物在典型城市水体系统中的分布以及迁移转化规律 对上海市淀山湖水源地、黄浦江上中下游地表水、沿江污水处理厂进出水以及居民饮用水进行检测分析，结果表明在污水处理厂进水中精神药物的浓度范围为ND-68.2 ng/L，主要的精神药物为卡马西平、多虑平、地西泮和劳拉西泮。在污水厂出水中检测的目标药物主要是卡马西平和奥沙西泮，浓度范围为ND-47.3 ng/L。污水处理厂对大部分的精神药物的去除效果较差，平均去除率低于50％。此外，地西泮、卡马西平、奥沙西泮以及劳拉西泮在淀山湖水库和黄浦江地表水也有检出，最高浓度达到75.5 ng/L。在居民饮用水中卡马西平(0.8-2.5 ng/L)、地西泮(0.5-3.2 ng/L)、阿普唑仑(2.3 ng/L)部分检出，浓度在健康风险阈值以下。通过相关性分析得出地表水中精神药物组成与附近污水厂出水的药物组成具有显著的相关性(r>0.5)，表明污水处理厂可能是精神药物的典型污染源。水源地药物与居民饮用水中的药物没有显著的相关性。本研究表明精神药物可能通过污水处理厂、地表水系统进入居民饮用水。需要对该类药物进行持续的关注。 III 精神病医院污水中的精神药物的分布、迁移转化及风险评估。 精神病医院作为精神药物的集中使用场所，可能成为环境中精神药物的典型污染源。通过对上海三个具有代表性的精神病医院出水以及周边地下水、地表水、土壤、植被采样分析，系统地研究了精神病医院周边环境中精神药物的分布，分析了目标药物在医院附近地表水和地下水中的迁移，探讨了目标药物在土壤和植被中的富集情况，最后对目标药物进行了环境风险评估。 检测结果表明目标药物阿米替林(83.57 ng/L)、劳拉西泮(22.26 ng/)在医院污水出水中检出的浓度较高。15种药物中有10种在所有12个地表水样中检出，其中劳拉西泮、卡马西平以及地西泮浓度较高。5种药物在3个地下水样品中检出，其中劳拉西泮的最高浓度高达46.83 ng/L。仅有6种药物在土壤样本中检出，浓度较低(
Pharmaceuticals and personal care products (PPCPs) have gained growing attention since these compounds have been found to negatively affect ecosystems and environment. Psychiatric compounds as the most widely used drugs in the world have drawn great attention. These compounds have been detected in waste water, surface water, groundwater, drinking water, soil, and even animal and plant tissues. Clarifying the occurrence, fate, environmental risk and main pollution sources of psychiatric pharmaceuticals in the environment and studying the treatment of pollutants are crucial to control the pollution of psychiatric pharmaceuticals and reduce the damage to ecological environment and human health. This work studied the occurrence and fate of typical psychiatric drugs in the urban water system and psychiatric hospital by analyzing these compounds in Shanghai urban water system (waster water treatment plants, Huangpu River surface water and the residents' drinking water) and environment medium (hospital effluent, surface water, groundwater, soil, and plant tissues) around psychiatric hospitals. In addition, adsorption removal and adsorption mechanism of psychiatric drugs on the different carbon materials was also studied. The research contents are as follows: I Establishment of trace analytical method for psychotropic drugs in the environment We established a trace analytical method for 15 psychotropic drugs in the environment by optimizing chromatographic conditions and mass spectrometric parameters based on the versatility, specificity, and selectivity recently of LC-MS/MS. We also optimized the sampling preparation technique (SPE for water sample and ultrasonic extraction + SPE for solid sample). The recovery, linearity, precision, matrix effects and sensitivity of analytical method could meet the requirements of actual research. II The occurrence and fate of psychiatric pharmaceuticals in the typical urban water system The occurrence and fate of 15 selected psychiatric pharmaceuticals, including eight benzodiazepines, four antidepressants, one antiepileptic and two metabolites of benzodiazepines were investigated in wastewater treatment plant (WWTP) influents and effluents, surface water, and final drinking water in Shanghai. Psychiatric pharmaceuticals were in WWTPs influents ranging from low ng L⁻¹ to 68.2 ng L⁻¹, dominated by carbamazepine, doxepin, diazepam and lorazepam. Target analytes were still detected in effluents from low ng L⁻¹ range to 47.3 ng L⁻¹, with carbamazepine, diazepam, and oxazepam as most prevalent. WWTPs were low effective (< 50%) in removing most of them, excluding amitriptyline (mean 60%), doxepin (mean 70%), temazepam (mean 78%) and lorazepam (mean 93%). In addition, carbamazepine, diazepam, oxazepam and lorazepam were detected in low ng L⁻¹ to 75.5 ng L⁻¹ in the surface water of Huang Pu Rive. The pattern of contaminants in surface water is similar to the effluent wastewater, which suggested the main source of organic trace pollutants might be WWTPs. Furthermore, carbamazepine (0.8-2.5 ng L⁻¹), diazepam (0.5-3.2 ng L⁻¹) and alprazolam (2.3 ng L⁻¹) were also detected in drinking water and the concentrations were below the health based precautionary value. The investigation was within the range of those results reported in other countries. Our results indicate ubiquity of the investigated compounds in the aquatic system. As a consequence, these pollutants may potentially reach drinking water resources via WWTP effluents and/or surface waters and require constant attention. III The fate and risk assessment of psychiatric pharmaceuticals from psychiatric hospital effluent This work analyzed the occurrence and fate of 15 selected psychiatric pharmaceuticals in wastewater from 3 psychiatric hospitals in Shanghai, investigated the impact of wastewater on surface water and groundwater around hospital and researched the enrichment of these substances in soil and plant irrigated by receiving water. Finally, a screening level risk assessment was also presented. The target pharmaceuticals amitriptyline (83.57 ng L⁻¹ ) and lorazepam (22.26 ng L⁻¹) showed the highest concentration and were frequently detected in hospital effluent. Ten of fifteen analyzed compounds were detected in all 12 surface water samples. Lorazepam, carbamazepine and diazepam showed higher values. Five of fifteen analyzed compounds were detected in all 3 groundwater samples. The highest concentration for lorazepam reached up to 46.83 ng L⁻¹ and our investigation was higher than those results reported in some countries. Only six target compounds were detected in all three soil sampling points with very low concentration (mean value < LOQ).Alkaline pharmaceuticals were more easily adsorbed by soil. Carbamazepine (1.29ng g⁻¹), oxazepam (1.22ng g⁻¹) and lorazepam (2.95ng g⁻¹) showed the highest concentration and were frequently detected in plant tissues. The correlation analyses performed between hospital effluent and surface water, surface water and groundwater showed that the main source of psychiatric pharmaceuticals pollutants might be hospital effluents (from effluent to surface water; from surface water to ground water). Weak correlations between polluted surface water and soil suggested that psychiatric pharmaceuticals might be easier to degrade or transform in soil. A significant correlation between soil and plant indicated the target compounds in plant tissues were originated from soil pollution. Although the risk assessment indicated that no adverse effect was expected, the continued emissions might cause potential impact on ecosystems. IV Study on adsorption and removal of typical psychiatric pharmaceuticals The interaction between psychiatric pharmaceuticals and two carbon based materials (graphene oxide and biochar) were studied by experiment and density functional theory calculating. The interaction between graphene oxide and psychiatric pharmaceuticals was very strong. The adsorption mechanism of psychiatric pharmaceuticals adsorbed on graphene oxide is heavily dependent on π-π and -F/-C1-π interaction. In addition, biochar has strong adsorption efficiency on psychiatric pharmaceuticals. The adsorption of psychiatric pharmaceuticals on biochar was mainly dependent on π-π interaction. The porous structure and the interaction between functional groups (-OH, -COOH) on graphene oxide and biochar might make contributions to adsorption. The adsorption energy by density functional theory calculating is consistent with the experimental results. In brief graphene oxide and biochar both have strong adsorption efficiency on psychiatric pharmaceuticals. However graphene oxide has faster adsorption rate due to it’s water solubility and biochar has greater adsorption quantity due to it’s porous structure. Keywords: Psychiatric pharmaceuticals, Drinking water, Groundwater, WWTPs, Hospital effluent, Risk assessment, biological enrichment, Adsorption, Graphene oxide