Environmental Levels and Degradation Behavior of Pharmaceuticals and Personal Care Products (PPCPs) in the Water Environment
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摘要:
药物和个人护理品(PPCPs)是一种存在于各种介质中的新污染物,具有生物富集、致癌致畸性,近年来在水环境中被广泛检出,其种类和浓度也有逐渐增多和加重的趋势,加之与人类生活密切相关,可以通过家庭垃圾、医院废水、垃圾填埋场、污水处理厂等方式直接污染地表水,并进一步污染孔隙水、地下水等,致使生态环境和人体健康存在风险。因此,广泛了解PPCPs在各种环境介质中的浓度水平对于防范生态健康风险具有重要意义。近年来,对PPCPs浓度的调查研究取得了较大进展,自1976年美国堪萨斯城首次报道药物以来,各国陆续报道了不同介质中PPCPs的存在,弥补了各研究区污染物及浓度的空白,有利于开展综合治理工作。PPCPs在水环境中常见的降解方式有水解、光解及生物降解,同时在降解过程还会受到pH、温度、共存离子等影响,而且在各种降解过程中生成的产物也有所不同。污水处理厂因为去除工艺的限制,使得地表水中许多PPCPs虽然经过了废水的生物降解环境,但是光降解仍然可能比暴露在阳光下的生物降解更强。其中,抗生素在水环境中主要发生光降解;布洛芬、碘普罗胺、咖啡因等更易发生生物降解;而自然界中PPCPs发生水解的概率较低,酯类和酰胺类是其中最常见的易水解的官能团,除此之外,四环素类等因为吸附到沉积物中,也会发生水解反应。目前,对于PPCPs浓度水平的研究很多集中在单一水体,而海水、雨水等介质缺乏监测和分析,同时对于降解行为的研究大都没有关注到降解过程和降解产物,使得一些降解产物的高毒性被低估。因此,全面了解各种水环境介质中PPCPs浓度可以较为准确、系统地获知各地区PPCPs的污染情况,对于PPCPs治理与削减工作具有重要的现实意义;而探究PPCPs在水环境中的降解行为,有利于了解其在环境中的残留和代谢情况,厘清中间产物和最终产物的性质,以便针对性地对PPCPs的环境生态效应进行评估分析,降低风险。
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关键词:
- 水环境 /
- 药物和个人护理品(PPCPs) /
- 浓度水平 /
- 降解行为 /
- 影响因素
Abstract:Pharmaceuticals and personal care products (PPCPs) are a class of chemicals used by humans for daily life. PPCPs are closely related to people’s production and life, and are even used every day worldwide. PPCP-like compounds were first detected in treated wastewater in Kansas City, USA in 1976 (concentrations of 0.8-2μg/L[6]), and subsequently detected in various countries. The mass production and use of PPCPs have led to increasing concentrations in the environment. PPCPs can induce microorganisms to produce resistance genes because of their persistence and bioaccumulation, thus changing the structure and community of microorganisms in the ecosystem. At the same time, they are accumulated at the top of the food chain or food web[17-21], destroying the balance of the ecosystem. In addition, PPCPs also have chronic toxicity, teratogenicity and carcinogenicity. For example, sulfonamides will damage tissues and organs and cause drug resistance of pathogenic bacteria[9]. Synthetic musk interferes with the secretion of hormones and can also lead to asthma, allergies, migraines and other diseases[20]. Long-term use will lead to liver and kidney damage and induce cancer[21], causing irreversible damage to human health.
PPCPs are mainly accumulated in the environment through hospitals, landfills, farms, factory wastewater and domestic sewage, and enter the water environment through various pathways. After the production of PPCPs, some are used by humans, some are directly generated in the production of waste, and some are used by animals in livestock farms. The solid or liquid waste generated in the above three ways will enter the sewage treatment plant or landfill. Then through sewage, landfill leachate directly into the surface water, through further infiltration into the sediment, pore water, groundwater, ocean and other environments, in addition to the surface water through evaporation and precipitation can also return to the water environment. The above environmental behaviors will cause harm to the ecological environment, ecosystem, and humans.
PPCPs exist in surface water, groundwater, sediment, and other environmental media, but the pollution degree varies in different countries. In recent years, a large concentration of PPCPs has been detected in various water environmental media, and sulfonamides, antibiotics, ibuprofen, carbamazepine and DEET are widely distributed in the environment, among which sulfamethoxazole has the highest detection frequency and the highest concentration can reach 1080ng/L[8]. China is the world's largest consumer of drugs, with more than 20000t PPCPs used annually, which have been widely detected in surface water, groundwater, soil and sediments, among which antibiotics transmitted through water bodies are used more[7] than others. In addition, PPCPs are also detected in water environmental media in the United States[50], Europe[57], and Africa[9], and the study found that the concentration of PPCPs is positively correlated with the degree of economic development. In China, the highest concentration of sulfamethoxazole is detected in the sediments of the Qingpu District of Shanghai, with a concentration of 688.59ng/L[44], while the highest concentration of sulfamethoxazole in other countries is detected in groundwater of the United States, with a concentration of 1110ng/L[50]. The concentration of PPCPs in pore water and seawater is relatively low, and caffeine is the most widely detected PPCP in seawater. Some compounds have been detected in rainwater because of their volatility. Atrazine has been reported in Mississippi and at the mouth of the Yangtze River[60-61]. The presence of ofloxacin and ciprofloxacin has also been detected in Minnesota, USA[38]. PPCPs in groundwater are mainly produced through the infiltration of domestic sewage, hospital and aquaculture wastewater, and compounds with greater polarity are more likely to penetrate into groundwater[59]. Antibiotics such as lincomycin and erythromycin have been detected in groundwater in North America, Jianghan Plain of China[53,50] and Harbin[52]. Carbamazepine is one of the most commonly detected drugs in sediments, and it has been reported in the Haihe River and Baiyang Lake[55], with the highest concentration of 14.7ng/g, and also in the sediments of the Taihu Lake Basin[54], the concentrations of ciprofloxacin and ofloxacin are relatively high, 15.33ng/g and 18.27ng/g respectively. The ocean is considered by many to be an important sink of pollutants. Studies have found that more than 20 kinds of antibiotics with concentrations as high as μg/L have been detected in seawater[62]. Among them, caffeine has been widely detected in the Aegean and Baltic Sea. Besides caffeine, sulfamethoxazole and clarithromycin also have a high detection frequency[57]. PPCPs were also detected in pore water and rainwater. The pore water samples of Baiyangdian Lake[55] mainly contain erythromycin and caffeine, but their concentrations are much lower than those of surface water in the same area. In Taihu Lake[56], the concentrations of oxytetracycline and ofloxacin are found, but the concentrations of surface water are lower than those of pore water. Therefore, the different physical and chemical conditions of environmental substrates in different study areas are considered to be the cause. There are relatively few reports of PPCPs in rainwater, and the content of PPCPS is less than 10ng/L.
PPCPs will degrade after entering water, and different degradation processes have their own degradation mechanisms. The degradation behavior of PPCPs in water mainly includes hydrolysis, photodegradation and biodegradation. Hydrolysis is an important way to eliminate or reduce the concentration of PPCPs in a water environment. Its essence is nucleophilic substitution reaction, that is, the nucleophilic group (hydroxide ion or water molecule) attacks the electrophilic group in the compound (RX), and replaces the associated strong electron-withdrawing group (X) with a negative electric tendency. For example, the hydrolysis of penicillin G and amoxicillin is the intramolecular nucleophilic attack of the side chain on the β-lactam carbonyl group, and the C-N bond is broken causing degradation. Degradation can be divided into direct photolysis and indirect photolysis processes. PPCPs with light-absorbing groups can be directly degraded by absorbing light energy. PPCPs without light-absorbing groups need to absorb photons through other substances to obtain energy, so that indirect photodegradation occurs. For example, atenolol is a degradation process that directly absorbs light energy, while acyclovir is an indirect photodegradation process by adding a catalyst. Biodegradation means that microorganisms change the chemical structure of PPCPs through a series of biochemical reactions under aerobic or anoxic conditions, and finally achieve the purpose of removal. At present, studies on the biodegradation of PPCPs mainly focus on three aspects: sewage treatment system, natural surface water and laboratory simulation system[79]. For sewage treatment plants, PPCPs are mainly removed through biodegradation of secondary treatment[80].
The degradation of PPCPs is affected by various factors, among which pH and temperature are the main influencing factors. The study on hydrolysis of PPCPs mainly considers the influence of pH on PPCPs. Different pH and target compounds will have different reactions, which have certain effects on the hydrolysis rate and hydrolysis products. In addition, temperature will also affect hydrolysis. In general, the higher the temperature, the faster the hydrolysis of a compound[61], because the hydrolysis process of a compound is a thermal reaction, and the activation energy mainly comes from the collision between molecules. The mechanism of photodegradation of PPCPs in water mainly lies in the molecular absorption of light energy into an excited state, which triggers various reactions[71]. There are many factors affecting the photodegradation of PPCPs in a water environment, mainly including pH of water and co-existing ions. It is generally believed that the higher pH in a water environment, the faster the photodegradation rate. Because many PPCP molecules contain acid-base dissociative groups, they are easily ionized in aqueous solution to produce a variety of dissociative forms, and the reason for affecting the ionization of PPCPs is the change of solution pH[74]. The presence of co-existing ions can either promote or inhibit the photodegradation of pollutants. The pH and temperature of the environment will affect the absorption, growth and metabolism of nutrients by microorganisms, thus changing the growth and living state of microorganisms, and then affecting biodegradation[82]. In addition, different compounds have different sensitivity to pH and temperature in the process of biodegradation. Also, the types of degraded strains have a certain impact on degradation. In general, photodegradation and biodegradation are more common than hydrolysis. In surface water, many PPCPs have avoided the strict biodegradation environment of wastewater treatment, and photochemistry may have a greater effect than the biodegradation under sunlight, in which antibiotics are mainly photodegraded in the water environment; ibuprofen, iopromide and caffeine are more prone to biodegradation; esters and amides are the most common functional groups that are easily hydrolyzed in PPCPs[63], and tetracycline can undergo hydrolysis reactions due to adsorption into sediments. The factors affecting the degradation of PPCPs include pH, temperature, co-existing ions and dissolved organic matter, among which pH and temperature are the main factors affecting the degradation. Exploring the fate of PPCPs in the environment is the key to studying their distribution and environmental level, so it is necessary to analyze the degradation mode of PPCPs in a water environment to help further understand the degradation principle and behavior of PPCPs.
Future research on PPCPs should be more in-depth and detailed. More emphasis will be placed on the water environment such as rain and sea water, which has been studied less before, to make the system more complete. The current research mainly focuses on the migration, transformation and toxic effects of PPCPs, and the toxic effects of degradation products need to be studied further. It is necessary to study the behavior, migration, transformation and toxic effects of PPCPs metabolites in the water environment, so as to provide basis for water environment pollution removal. In addition, the content of PPCPs in the water environment is very low, and the testing technology and instrument requirements are relatively strict. The existing analysis technology and instrument conditions need to be continuously improved to establish a more comprehensive and systematic testing system.
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Keywords:
- water environment /
- pharmaceuticals and personal care products (PPCPs) /
- concentration level /
- degradation behavior /
- influencing factors
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表 1 抗生素、激素、消炎止痛药、降压药类等常见PPCPs的物理化学特征
Table 1 Physical and chemical characteristics of common PPCPs such as antibiotics, hormones, anti-inflammatory painkillers and antihypertensive drugs.
PPCPs
的常见类别中文名称 英文名称 缩写 分子式 医学应用 CAS号 抗生素 磺胺甲噁唑 Sulfamethoxazole SMX C10H11N3O3S 抗菌 723-46-6 诺氟沙星 Norfloxacin NOR C16H18FN3O3 治疗肠炎痢疾 70458 -96-7四环素 Tetracycline TC C22H24N2O8 杀菌 60-54-8 土霉素 Oxytetracycline OTC C22H28N2O11 治疗犬、猫的呼吸道、尿道感染 79-57-2 红霉素 Erythromycin ERY C37H67NO13 治疗呼吸道感染 114-07-8 激素 地塞米松 Dexamethasone DEX C22H29FO5 抗炎、免疫抑制 50-02-2 雌酮 Estrone E1 C18H22O2 维持雌性个体的第二生理特征 53-16-7 乙烯雌酚 Diethylstilbestrol DES C18H20O2 治疗雌激素低下症及激素平衡失调引起的功能性出血 56-53-1 消炎止痛药 萘普生 Naproxen NAP C14H14O3 止痛解热 22204 -53-1双氯芬酸 Diclofenac Acid DIC CHClNO 治疗风湿性关节炎等 15307 -86-5布洛芬 Ibuprofen IBU C13H18O2 镇痛、抗炎 15687 -27-1降压药 科素亚 Losartan - C22H22ClKN6O 降血压 124750 -99-8缬沙坦 Valsartan ARB C24H29N5O3 降血压 137862 -53-4降血脂药 吉非罗齐 Gemfibrozil GEM C15H22O3 调血脂 25812 -30-0苯扎贝特 Bezafibrate BZF CHClNO 调血脂 41859 -67-0β-受体阻断药 阿替洛尔 Atenolol - C14H22N2O3 降压、调整心率 29122 -68-7美托洛尔 Metoprolol MPL C15H25NO3 降压、调整心率 51384 -51-1抗精神病药 卡马西平 Carbamazepine CBZ CHN2O 治疗癫痫、神经性疾病 298-46-4 可铁宁 Cotinine - C10H12N2O 促进神经系统兴奋 486-56-6 驱虫剂 避蚊胺 Diethyltoluamide DEET C12H17NO 防止蚊虫叮咬 134-62-3 合成麝香 佳乐麝香 Galaxolide HHCB C18H26O 用于化妆品、调制香料 1222 -05-5吐纳麝香 Tonalide AHTN C18H26O 用于化妆品、调制香料 1506 -02-1消毒杀菌剂 三氯生 Triclosan TCS C12H7Cl3O2 抗菌除臭 3380 -34-5三氯卡班 Triclocarban TCC C13H9Cl3N2O 杀菌除臭 101-20-2 除草剂 阿特拉津 Atrazine ATZ C8H14ClN5 除草 1912-24-9 表 2 水环境中抗生素类PPCPs在地表水、地下水、沉积物、孔隙水、海水、雨水中的检出情况
Table 2 Detection of antibiotic PPCPs in surface water, groundwater, sediment, pore water, seawater and rainwater.
水环境
介质PPCPs化合物 PPCPs检出含量
(ng/L)水环境 数据来源 地表水 磺胺甲恶唑 ND~57.76 中国上海市青浦区 [44] 28.34 中国上海黄浦江 [45] <MDL~934 斯里兰卡 [46] 0.7~16 意大利米兰 [47] 77.7(最大浓度) 密西西比河国家河和娱乐河 [13] 氧氟沙星 114 中国黄河 [42] 0 中国黄浦江 [45] 诺氟沙星 152 中国黄河 [42] 0 中国黄浦江 [45] 红霉素 34 中国黄河 [42] 0~722.04 中国天津 [48] 罗红霉素 53 中国黄河 [42] 3.63 中国黄浦江 [45] 四环素 113.89 中国黄浦江 [45] 0~9.74 天津 [48] 地下水 醋磺胺甲恶唑 ND~91 中国北运河 [49] 磺胺二甲基嘧啶 ND~969.7 中国北运河 [49] 磺胺甲恶唑 ND~14.2 中国北运河 [49] 1110 美国 [50] 23.40 西班牙 [51] 磺胺嘧啶 11.62 西班牙 [51] 29.9 哈尔滨 [52] 环丙沙星 4~9.68 中国江汉平原 [53] 0.82 哈尔滨 [52] 四环素 2.26~9.51 中国江汉平原 [53] 罗红霉素 1.47~13.8 中国江汉平原 [53] 诺氟沙星 4.74~52.6 中国江汉平原 [53] 土霉素 1.1~7.24 中国江汉平原 [53] 林可霉素 0.32 美国 [50] 沉积物 磺胺甲恶唑 1. 27~688.59 中国上海市青浦区 [44] 0~11.3 中国太湖 [54] 磺胺嘧啶 0~0.41 中国太湖 [54] 土霉素 0~8.73 中国太湖 [54] 环丙沙星 0~15.33 中国太湖 [54] 氧氟沙星 0.9~18.27 中国太湖 [54] 罗红霉素 0.15~3.96 中国太湖 [54] 孔隙水 红霉素 29.9 中国白洋淀 [55] 林可霉素 20.2 中国白洋淀 [55] 土霉素 47.8 中国太湖 [56] 氧氟沙星 33.6 中国太湖 [56] 雨水 环丙沙星 10.3 美国明尼苏达州 [38] 恩诺沙星 2.97 美国明尼苏达州 [38] 海水 磺胺甲恶唑 42 波罗的海 [57] 11 希腊爱琴海 [57] 7.2 意大利威尼斯 [57] 克拉霉素 14 波罗的海 [57] 16 希腊爱琴海 [57] 8.5 意大利威尼斯 [57] 表 3 水环境中PPCPs常见化合物的降解类型、影响和因素及降解产物
Table 3 Types, effects, factors, and degradation products of common PPCPs in the water environment.
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