【作者】 李燕；

【导师】 丁杰；

【作者基本信息】 哈尔滨工业大学 ， 环境科学与工程， 2021， 博士

【摘要】 药物已被广泛应用于人类健康、畜牧养殖和食品加工等方面,成为与人类生活密切相关的化合物种类之一。近年来,在地表水和地下水等环境水相中检测到的药物污染物种类及浓度水平越来越高。这些物质不仅对水体环境和水生生物产生不利影响,甚至影响整个生态系统和人类健康,因此对药物产生的潜在毒性和环境影响研究成为近年来国内外研究热点。本研究围绕中国七大河流中优先控制药物筛选、基于USEtox的环境水体中药物潜在毒性研究和污水深度处理工艺去除优先控制药物的毒性及环境影响评价等方面开展了相关研究,为研究人员和监管机构提供关于药物对人类和生态健康风险的指导,同时克服传统环境影响评估方法的片面性和局部性,为污水处理厂提标改造工程的规划和决策提供环境影响的科学依据。基于中国药物使用、污染及深度处理现状,采用综合评分法,选取实际环境浓度、环境暴露风险和生态影响作为指标,建立了中国七大河流中优先控制药物筛选体系,并通过筛选体系确立了包括10种抗生素（红霉素、脱水红霉素、阿奇霉素、克拉霉素、甲氧苄啶、磺胺甲恶唑、乙酰磺胺甲恶唑、环丙沙星、诺氟沙星、头孢唑啉）、3种消炎药物（布洛芬、双氯酚酸、吲哚美辛）和1种降血脂药（苯扎贝特）在内的中国七大河流中优先控制药物清单。通过研究发现,抗生素是中国七大河流中风险最高的药物种类,磺胺类则是中国七大河流中风险最高的抗生素类别。此外,长江、珠江和海河流域的药物污染程度高于其他流域,珠江流域对水生生物的潜在风险最高,松花江和海河流域的潜在风险最低。本研究对中国七大河流中药物的分布特征和健康风险进行了系统研究,为我国流域中药物污染的管理和调控提供了新型决策支持体系。基于药物理化特性、降解速率、生物蓄积性、生态毒性和人体毒性等输入参数,利用USEtox模型进行39种药物的生态毒性和人体毒性特征化因子分析,并分析了我国七大河流中药物的潜在毒性影响。在我国七大河流中磺胺类和大环内酯类抗生素是生态毒性影响最高的药物种类,其生态影响分别在ND-1.29×10^-6CTU_e和3.96×10^-8-9.37×10^-7 CTU_e之间。喹诺酮类抗生素和消炎药是人体毒性影响最高的药物种类,其人体影响分别在2.67×10^-17-4.09×10^-15 CTU_h和ND-5.98×10^-12 CTU_h之间。对造成流域中药物污染现状的排放源进行分析,基于综合评分法,选取预测环境浓度、药物去除率、生态影响和健康影响四个指标,确立了适用于中国污水处理厂的优先控制药物清单。采用USEtox方法和CML2001方法分别对颗粒活性炭、纳滤和臭氧氧化三种污水深度处理工艺去除包含优先控制药物在内的39种药物的毒性影响和环境影响进行评价,确定纳滤工艺去除药物生态及人体毒性影响效果最佳且产生的环境负荷最小。纳滤工艺对进水中药物生态和人体毒性分别降低了92%和95%,且运行过程中产生毒性影响最小,电力和化学物的生产使用是造成毒性影响和环境影响的关键因素。电力对非生物性资源耗损、全球气候变暖、臭氧层损耗和光化学烟雾等环境影响类别的贡献度最大,分别为88.25%、87.16%、73.38%和76.36%;化合物对酸化效应和富营养化等环境影响类别的贡献度最大,分别为60.20%和59.55%。更多还原

【Abstract】 Pharmaceuticals have been widely used in human health,animal husbandry,food processing and other aspects,and become one of the compounds closely related to human life.In recent years,the types and concentrations of pharmaceutical contaminants detected in environmental water phases such as surface water and groundwater have been increasing.These substances not only have adverse effects on the aquatic environment and aquatic organisms,but also affect the entire ecosystem and human health.Therefore,the potential toxicity and environmental effects of pharmaceuticals have become a research hotspot in recent years.This study have been carried out on the screening of priority control pharmaceutical s in major rivers of China,the potential toxicity of pharmaceuticals in environmental water based on USEtox,and the toxicity and environmental impact assessment on the removal of priority control pharmaceuticals with advanced treatment process.This study provided guidance to researchers and regulators on the risks of pharmaceuticals to human and ecological health and provided a scientific basis for planning and decision-making on environmental impacts of sewage treatment plant upgrading projects while overcoming the one-sided and partial nature of traditional environmental impact assessment methods.Based on the current situation of use,pollution and advanced treatment of pharmaceuticals in China,the comprehensive scoring method was adopted to select the actual environmental concentration,environmental exposure risk and ecological effects as indexes to establish the ranking system of priority pharmaceuticals of major rivers in China.According to this ranking system,a priority pharmaceuticals list of major rivers in China was obtained which contained 10 kinds of antibiotics（erythromycin,anhydroerythromycin,azithromycin,clarithromycin,trimethoprim,sulfamethoxazole,acetyl sulfamethoxazole,ciprofloxacin,norfloxacin and cefazolin）,3 kinds of antiphlogistics（ibuprofen,diclofenac and indomethacin）and 1 kind of antilipemic agent（bezafibrate）.It was found that antibiotics were the most risky pharmaceutical while sulfonamides were the most risky antibiotics in the major rivers of China.In addition,the Yangtze river,Pearl river and Hai river had higher levels of pharmaceutical contamination than other rivers,and the Pearl river had the highest potential risk to aquatic organisms,while Songhua river and Hai river had the lowest potential risk.This study systematically studied the distribution characteristics and health risks of pharmaceuticals in major rivers of China and provided a new decision support system for the management and control of pharmaceutical contamination in rivers of China.Based on the input parameters of physicochemical properties,degradation rate,bioaccumulation,ecotoxicity and human toxicity,the Usetox model was used to analyze the ecotoxicity and human toxicity characteristic factors of 39 drugs,and the potential toxicity effects of pharmaceuticals in major rivers of China were analyzed.Sulfonamides and macrolides are the pharmaceuticals with the highest ecotoxic effects in major rivers of China,and their ecological effects are between ND-1.29×10^-6CTU_eand 3.96×10^-8-9.37×10^-7 CTU_e,respectively.Quinolone antibiotics and anti-inflammatory pharmaceuticals had the highest toxic effects on human body,and their human effects were 2.67×10^-17-4.09×10^-15 CTU_hand ND-5.98×10^-12 CTU_h,respectively.The emission sources that caused the pharmaceutical pollution in the rivers were analyzed.Based on the comprehensive scoring method,predict the environmental concentration,removal rate,ecological impact and health impact were selected as indexes to establish the ranking system of priority pharmaceuticals of WWTPs in China.Evaluation of toxicity effect and environmental impact of three wastewater advanced treatment processes which contained granular activated carbon,nanofiltration and ozone oxidation for the removal of 39 pharmaceuticals which contained priority control pharmaceuticals has been carried with USEtox method and CML2001 method.The result showed that nanofiltration process has the best effect to remove the ecology and human toxicity of the pharmaceuticals and the least environmental load.The nanofiltration process reduced the ecology and human toxicity of pharmaceuticals by 92%and 95%,respectively.In addition,the toxic effect in the operation process was also the least.The production and use of electricity and chemicals are the key factors that cause the toxic effect and environmental impact.The of electric power contributed the most to non-biological resource depletion,global warming,ozone layer depletion and photochemical smog,which were 88.25%,87.16%,73.38%and 76.36%,respectively.The compounds contributed the most to acidification effect and eutrophication,which were 60.20%and 59.55%,respectively.更多还原