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药物及个人护理品的污染现状、分析技术及生态毒性研究进展

王丹丹 张婧 杨桂朋 李锋民

王丹丹, 张婧, 杨桂朋, 李锋民. 药物及个人护理品的污染现状、分析技术及生态毒性研究进展[J]. 环境科学研究, 2018, 31(12): 2013-2020. doi: 10.13198/j.issn.1001-6929.2018.10.04
引用本文: 王丹丹, 张婧, 杨桂朋, 李锋民. 药物及个人护理品的污染现状、分析技术及生态毒性研究进展[J]. 环境科学研究, 2018, 31(12): 2013-2020. doi: 10.13198/j.issn.1001-6929.2018.10.04
WANG Dandan, ZHANG Jing, YANG Guipeng, LI Fengmin. Pollution Status, Analytical Techniques and Ecotoxicity of Pharmaceuticals and Personal Care Products[J]. Research of Environmental Sciences, 2018, 31(12): 2013-2020. doi: 10.13198/j.issn.1001-6929.2018.10.04
Citation: WANG Dandan, ZHANG Jing, YANG Guipeng, LI Fengmin. Pollution Status, Analytical Techniques and Ecotoxicity of Pharmaceuticals and Personal Care Products[J]. Research of Environmental Sciences, 2018, 31(12): 2013-2020. doi: 10.13198/j.issn.1001-6929.2018.10.04

药物及个人护理品的污染现状、分析技术及生态毒性研究进展

doi: 10.13198/j.issn.1001-6929.2018.10.04
基金项目: 

国家重点研发计划项目 2016YFA0601304

海洋国家实验室“鳌山人才”卓越科学家计划项目 2015 ASTP-OS12

详细信息
    作者简介:

    王丹丹(1992-), 女(蒙古族), 辽宁建平人, wdd120192@163.com

    通讯作者:

    张婧(1982-), 女, 山东青岛人, 副教授, 博士, 主要从事海洋化学、海洋环境研究, zhangjouc@ouc.edu.cn

  • 中图分类号: X522

Pollution Status, Analytical Techniques and Ecotoxicity of Pharmaceuticals and Personal Care Products

Funds: 

National Key Research and Development Program of China 2016YFA0601304

Aoshan Talents Program of Qingdao National Laboratory for Marine Science and Technology, China 2015 ASTP-OS12

  • 摘要: 随着医药及洗化行业的快速发展,PPCPs(pharmaceuticals and personal care products,药物及个人护理品)的生产和使用量增长迅速,已经成为自然环境中具有潜在生态风险的一类新型污染物.由于PPCPs在环境中浓度低、检测难度大、生态风险具有潜伏性,高灵敏度的定量检测方法已成为研究的热点.比较了文献中常用的不同预处理方法〔液液萃取(liquid liquid extraction,LLE)、固相萃取(solid phase extraction,SPE)、固相微萃取(solid phase micro extraction,SPME)、超声波溶剂萃取(ultrasonic solvent extraction,USE)、加压液相萃取(pressurized liquid extraction,PLE)、微波辅助溶剂萃取(microwave assisted solvent extraction,MASE)〕和检测方法〔GC/MS(气相色谱-质谱)、GC/MS/MS(气相色谱-双质谱)、HPLC/MS(高效液相色谱-质谱)、HPLC/MS/MS(高效液相色谱-双质谱)〕对地表水、沉积物、饮用水等不同介质中PPCPs检出限和检出浓度的异同,发现水样预处理常采用固相萃取法,其具有高回收和富集倍数、消耗有机溶剂少、省时等优点;固相样品预处理常采用超声溶剂萃取,其具有操作简单、适用性广等优点;HPLC/MS/MS检测方法具有广泛适用性,可检测大多数PPCPs,并且操作简单、灵敏度高.PPCPs会在水生生物体富集,并会表现出抑制酶活性、蛋白质及核酸合成、干扰藻类生长、影响动物活动等毒性效应.建议未来应加强环境中超低浓度PPCPs定量、定性分析技术的研发与应用,同时加强其环境风险研究,为揭示PPCPs的环境归趋行为提供技术支持.

     

  • 图  1  PPCPs的主要来源及进入水环境中的途径

    Figure  1.  The main source of PPCPs and access to water environment

    表  1  不同介质中检出的PPCPs含量

    Table  1.   The concentration of PPCPs in different media

    介质 类别 PPCPs化合物 PPCPs含量 水体 数据来源
    地表水/
    (ng/L)
    非类固醇消炎药
    (NSAIDs)
    水杨酸(Salicylic acid) 478~13 750 中国东江 文献[16]
    66~14 736 中国珠江 文献[12]
    ND~35.5 中国黄河 文献[17]
    双氯芬酸(Diclofenal) 0.2~150 中国珠江 文献[12]
    ND~25 中国黄浦江 文献[18]
    0.87~98 韩国Han河 文献[5]
    布洛芬(Diclofenal) 26.6~67.6 中国东江 文献[16]
    17.5~685 中国珠江 文献[12]
    8.5~416 中国黄河 文献[17]
    萘普生(Naproxen) 28~43.6 中国东江 文献[16]
    ND~380 瑞士Greifensee 文献[19]
    ND~128 中国珠江 文献[12]
    甲灭酸(Mefenamic acid) 12~25 中国珠江 文献[12]
    13.50~21.50 中国东江 文献[16]
    降血脂(Antilipemicagent) 吉非罗齐(Gemfibrozil) ND~20 中国黄浦江 文献[18]
    苯扎贝特(Bezafibrate) <10~66 英国South Wales 文献[20]
    ND~25.5 西班牙Ebro河 文献[11]
    抗生素(Antibiotics) 磺胺甲基异
    (Sulfamethoxazole)
    0.45~12 中国钦州湾 文献[2]
    ND~0.091 中国大辽河 文献[21]
    2~165 中国珠江 文献[22]
    甲氧苄氨嘧啶
    (Trimethoprim)
    ND~66 中国黄浦江 文献[18]
    2.3~63.3 美国Tennessee河 文献[7]
    <1.5~126 英国South Wales 文献[20]
    ND~410 西班牙Doñana Park 文献[23]
    四环素(Tetracyclines) ND~15 中国大辽河 文献[21]
    诺氟沙星(Norfloxacin) ND~1 380 中国大辽河 文献[21]
    117~251 中国珠江 文献[22]
    124~26.1 中国珠江 文献[24]
    兴奋剂(Incitant) 咖啡因(Caffein) 11~400 美国Indiana 文献[25]
    个人护理品
    (Personal care products)
    三氯生(Triclasan) LOD~478 中国珠江 文献[26]
    苯甲酮(Benzophenone) 3~371 英国South Wales河 文献[20]
    佳乐麝香(Galaxolide) 100~300 中国素梅什河 文献[27]
    沉积物/
    (μg/kg)
    非类固醇消炎药(NSAIDs) 布洛芬(Ibuprofen) 14.3 巴西托斯湾 文献[9]
    抗生素(Antibiotics) 阿奇霉素(Azithromycin) 4.4~1 204.9 中国徒骇河 文献[28]
    磺胺甲嘧啶(Sulfamethazine) ND~248 中国珠江 文献[29]
    诺氟沙星(Norfloxacin) ND~1 120 中国珠江 文献[29]
    兴奋剂(Incitant) 咖啡因(Caffein) 23.4 巴西托斯湾 文献[9]
    激素(hormone) 双酚A(Bisphenol-A) 0.68~4.82 中国巢湖 文献[30]
    2.1~429.5 中国珠江 文献[31]
    个人护理品
    (Personal care products)
    佳乐麝香(Galaxolide) 52.5 巴西托斯湾 文献[9]
    多环麝香(Polycyclic Musks) 5.76~167 中国珠江 文献[32]
    三氯生(Triclosan) 0.27~130.7 西班牙Almerıa 文献[33]
    LOD~1 329 中国珠江 文献[31]
    4-壬基酚(4-Nonyl Phenol) 107~16 198 中国珠江 文献[34]
    饮用水/
    (ng/L)
    非类固醇消炎药(NSAIDs) 萘普生(Naproxen) 63~68 路易斯安那州 文献[10]
    抗生素(Antibiotics) 扑热息痛(Paracetamol) LOD~211 法国Herault River 文献[35]
    甲氧苄啶(Trimethoprim) 2.84 中国华南地区 文献[34]
    诺氟沙星(Norfloxacin) ND~4.4 中国江苏地区 文献[36]
    兴奋剂(Incitant) 咖啡因(Caffein) 22.9 法国Herault River 文献[35]
    个人护理品
    (Personal care products)
    驱蚊露(Drive midge dew) 0.14 文献[37]
    注: ND为低于检出限浓度;LOD为检出限.
    下载: 导出CSV

    表  2  常用环境中PPCPs的检测方法

    Table  2.   Common detection methods of PPCPs in the environment

    分析物质 富集方法 色谱及质谱条件 数据来源
    水杨酸、氯贝酸、双氯芬酸、甲芬那酸、吉非罗齐、萘普生 SPE, Oasis HLB柱 PFBBr衍生,DB35-MS柱,负化学电离(NCI) 文献[16]
    水杨酸、布洛芬、双氯芬酸、吉非罗平、萘普生、酪洛芬 SPE, Oasis HLB柱 PFBBr衍生,负化学电离 文献[17]
    扑癫酮、卡马西平 SPE, Oasis HLB柱 N-甲基-N-(三甲基硅基)三氟苄基溴衍生,负化学电离 文献[39]
    灭虫剂、醋氨酚、双氯芬酸钠、5-氟嘧啶等 SPE Phenomenex Strata柱 四极质谱,DB-5MS柱,离子源为电子轰击 文献[45]
    二甲双胍、磺胺甲唑等 SPE, Oasis HLB柱 Metasil Basic C18柱,离子源为ESI+ 文献[46]
    对乙酰氨基酚、布洛芬、三氯生、咖啡因等 SPE, Oasis HLB柱 RPC18 ZORBAX Eclipse XDB柱,TOF质谱检测器,离子源为ESI+ 文献[47]
    咖啡因、甲氧苄啶、卡马西平等 SPE, Oasis HLB柱 HPLC-ESI-MS/MS,离子源为ESI+和ESI-,反应模式为MRM 文献[18]
    氯贝酸、酮洛芬、萘普生、布洛芬、双氯芬酸 水样为SPE,颗粒物为USE XDB-C18反相柱,离子源为ESI 文献[48]
    青霉素G、青霉素V、咖啡因、避蚊胺、三氯卡班等 水样为SPE Oasis HLB柱,沉积物为PLE Water AcquityTM UPLC BEHC18色谱柱,离子源为ESI+和ESI-,检测模式为MRM 文献[49]
    卡马西平、苯扎贝特、吉非罗齐、吲哚美辛 SPE, Oasis HLB小柱 HPLC-ESI-MS/MS,正离子源为XDB-C18,负离子源为Capcell PAKC18 文献[50]
    诺佛沙星等23种 SPE, Oasis HLB柱 Poroshell 120 EC-C18,离子源为ESI+和ESI-,检测模式为MRM 文献[51]
    注:PFBBr为五氟苄基溴;SPE为固相萃取;USE为超生波溶剂萃取;PLE为加压液相萃取;MRM为多反应检测.
    下载: 导出CSV

    表  3  不同种类PPCPs对水生生物的毒性效应

    Table  3.   Toxic effects of different PPCPs on aquatic organisms

    毒性效应类别 PPCPs类型 PPCPs化合物 受试生物 表现形式 数据来源
    抑制蛋白质合成 非类固醇消炎药 扑热息痛 小麦 21 d:破坏可溶性蛋白合成 文献[56]
    抗生素 诺氟沙星,四环素 费氏孤菌 24 h:四环素、诺氟沙星抑制蛋白质合成 文献[57]
    螺旋霉素 铜绿微囊藻 7 d:螺旋霉素抑制蛋白质合成 文献[58]
    抑制核酸合成 抗生素 诺佛沙星 费氏孤菌 24 h:诺氟沙星抑制DNA/RNA合成 文献[57]
    降血压药 阿替洛尔 鲫鱼 14 d:对鲫鱼的新城代谢和基因组改变有影响 文献[55]
    抑制酶活性 非类固醇消炎药 扑热息痛 小麦 14 d:小麦CAT酶活性降低 文献[55]
    抗生素 恩诺沙星 球等鞭金藻 96 h:随着ρ(恩诺沙星)增加,CAT活性递减;ρ(恩诺沙星)在0~10 mg/L时,CAT活性下降明显 文献[59]
    干扰藻类生长 非类固醇消炎药 布洛芬 蓝细菌紫背浮萍 布洛芬对蓝细菌的生长发育起到促进作用;对浮萍的抑制作用呈剂量-效应关系 文献[60]
    影响动物活动 非类固醇消炎药 双氯芬酸 青鳉鱼 9 d:影响青鳉鱼摄食行为 文献[61]
    个人护理品 麝香酮 斑马鱼(雌) 8周:雌鱼体质量和长度减少;肝脏和性腺;繁殖力减弱;死亡率增加;NOEC=10 μg/L;LOEC=33 μg/L 文献[62]
    影响ρ(Chla) 其他 卡马西平 小球藻 96 h:抑制小球藻ρ(Chla) 文献[63]
    注:NOEC (no observed effect concentration)为无毒性效应浓度;LOEC (lowest observed effect concentration)为毒性效应最低浓度.
    下载: 导出CSV
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  • 收稿日期:  2018-04-24
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