北京市生活污水中曲马多和芬太尼的赋存
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摘要
曲马多和芬太尼是临床上常用的止痛药品,具有一定的成瘾性,其滥用问题被社会广泛关注.这两种药物经人体代谢后,会以代谢产物和原药的形式随尿液进入生活污水并汇入污水处理厂,经处理后被排入自然水体,带来潜在的环境风险.在国内外已有研究的基础上,建立了污水中曲马多和芬太尼的前处理及分析测定方法,并首次对北京市23家污水厂进出水中曲马多和芬太尼进行测定.进水中曲马多的浓度范围为(10. 2±8. 7)～(175. 3±59. 7) ng·L-1,而芬太尼在多数水样中未被检出.传统活性污泥工艺对曲马多的去除效果较差,其它工艺均能有效去除曲马多.北京市中心城区曲马多的负荷水平显著高于近郊的负荷水平.基于污水流行病学方法对北京市曲马多的使用进行了估算,海淀区曲马多的年使用量最高,约为202. 5 kg.北京市夏季曲马多的使用量显著高于冬季.本研究为全国范围曲马多和芬太尼使用的污水流行病学调查提供了参考依据.
Tramadol( TRA) and fentanyl( FEN) are used as common painkillers in clinical practice,but they have been increasingly abused in recent years due to their addictive nature. Two substances and their metabolites enter wastewater through urine and are collected and treated by wastewater treatment plants( WWTPs) before being discharged into the aquatic environment. In this study,wastewater analysis was performed to examine the patterns of TRA and FEN use in the urban area of Beijing for the first time. Influent and effluent samples were collected from 23 WWTPs during two sampling campaigns. Concentrations TRA in influents were found to range from( 10. 2 ± 8. 7) to( 175. 3 ± 59. 7) ng·L-1,while FEN was not detected in most of the samples,or occurred at very low concentrations. Relatively low TRA removal was observed at plants with activated sludge processes. Moreover,TRA loads in the central area of Beijing were significantly higher than those in the suburban areas. Annual TRA use was estimated through wastewater-based epidemiology. The greatest TRA use,approximately 202. 5 kg,was found in Haidian district. Seasonal variation in TRA loads was significant,with greater use in the summer than in winter. The method presented in this study can be used as an important reference for monitoring TRA and FEN use via wastewater-based epidemiology and for assessing the risk of the abuse of these compounds in China.
Tramadol( TRA) and fentanyl( FEN) are used as common painkillers in clinical practice,but they have been increasingly abused in recent years due to their addictive nature. Two substances and their metabolites enter wastewater through urine and are collected and treated by wastewater treatment plants( WWTPs) before being discharged into the aquatic environment. In this study,wastewater analysis was performed to examine the patterns of TRA and FEN use in the urban area of Beijing for the first time. Influent and effluent samples were collected from 23 WWTPs during two sampling campaigns. Concentrations TRA in influents were found to range from( 10. 2 ± 8. 7) to( 175. 3 ± 59. 7) ng·L-1,while FEN was not detected in most of the samples,or occurred at very low concentrations. Relatively low TRA removal was observed at plants with activated sludge processes. Moreover,TRA loads in the central area of Beijing were significantly higher than those in the suburban areas. Annual TRA use was estimated through wastewater-based epidemiology. The greatest TRA use,approximately 202. 5 kg,was found in Haidian district. Seasonal variation in TRA loads was significant,with greater use in the summer than in winter. The method presented in this study can be used as an important reference for monitoring TRA and FEN use via wastewater-based epidemiology and for assessing the risk of the abuse of these compounds in China.
引文
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[18] Khan U,van Nuijs A L N,Li J,et al. Application of a sewagebased approach to assess the use of ten illicit drugs in four Chinese megacities[J]. Science of the Total Environment,2014,487:710-721.
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[20] Du P,Zhou Z L,Bai Y Q,et al. Estimating heroin abuse in major Chinese cities through wastewater-based epidemiology[J].Science of the Total Environment,2017,605-606:158-165.
[21] Du P,Zhou Z L,Huang H M,et al. Estimating population exposure to phthalate esters in major Chinese cities through wastewater-based epidemiology[J]. Science of the Total Environment,2018,643:1602-1609.
[22] Rodayan A,Majewsky M,Yargeau V. Impact of approach used to determine removal levels of drugs of abuse during wastewater treatment[J]. Science of the Total Environment,2014,487:731-739.
[23] Tscharke B J,Chen C,Gerber J P,et al. Temporal trends in drug use in Adelaide,South Australia by wastewater analysis[J]. Science of the Total Environment,2016,565:384-391.
[24] Rúa-Gómez P C, Püttmann W. Occurrence and removal of lidocaine, tramadol, venlafaxine, and their metabolites in German wastewater treatment plants[J]. Environmental Science and Pollution Research,2012,19(3):689-699.
[25]高婷婷,杜鹏,徐泽琼,等.污水中常见违禁药物分析方法优化及验证[J].环境科学,2017,38(1):201-211.Gao T T,Du P,Xu Z Q,et al. Optimization and validation of the analytical method to detect common illicit drugs in wastewater[J]. Environmental Science,2017,38(1):201-211.
[26]陈培培,杜鹏,周子雷,等.污水中新精神活性物质的分析方法优化及验证[J].环境科学,2018,39(8):3736-3743.Chen P P,Du P,Zhou Z L,et al. Optimization and validation of the analytical method to detect new psychoactive substances in wastewater[J]. Environmental Science,2018,39(8):3736-3743.
[27] Baker D R,Kasprzyk-Hordern B. Multi-residue determination of the sorption of illicit drugs and pharmaceuticals to wastewater suspended particulate matter using pressurised liquid extraction,solid phase extraction and liquid chromatography coupled with tandem mass spectrometry[J]. Journal of Chromatography A,2011,1218(44):7901-7913.
[28] Mackul'ak T,BiroováL,Gál M,et al. Wastewater analysis:the mean of the monitoring of frequently prescribed pharmaceuticals in Slovakia[J]. Environmental Monitoring and Assessment,2016,188(1):18.
[29]枸橼酸芬太尼注射液说明书. 2010年版.宜昌人福药业有限责任公司[EB/OL]. https://wenku. baidu. com/view/69b12972168884868762d6b6. html,2010-10-07.
[30]盐酸曲马多缓释片说明书. 2007年版.黑龙江龙桂制药有限公司[EB/OL]. https://wenku. baidu. com/view/3047bafe941ea76e58fa04c1. html,2007-03-27.
[31]李博,王志谨,曹军,等.污水处理传统工艺与新工艺出水中有机提取物的雌激素样作用比较[J].卫生研究,2014,43(3):477-482.Li B,Wang Z J,Cao J,et al. Estrogenic activity of organic extracts in the effluents treated by present treatment and the new process[J].Journal of Hygiene Research,2014,43(3):477-482.
[2] Petrovi'c M,Gonzalez S,BarcelóD. Analysis and removal of emerging contaminants in wastewater and drinking water[J].Tr AC Trends in Analytical Chemistry,2003,22(10):685-696.
[3]张志申.曲马多的药理学特点及其依赖性调研[J].中国医药指南,2017,15(28):293.
[4]刘志民.芬太尼及其衍生物的滥用与管制:危害与挑战[J].中国药物依赖性杂志,2017,26(4):274-276.
[5]关于加强曲马多等麻醉药品和精神药品监管的通知.国食药监办[2007]749号[EB/OL]. https://wenku. baidu. com/view/d1525473f46527d3240ce0c0. html,2007-12-07.
[6]国家食品药品监督管理局.关于加强对瑞芬太尼、扎莱普隆等药品管理的通知.国食药监安[2003]90号[EB/OL]. http://samr. cfda. gov. cn/WS01/CL0844/9904. html,2003-06-10.
[7] Grond S,Sablotzki A. Clinical pharmacology of tramadol[J].Clinical Pharmacokinetics,2004,43(13):879-923.
[8]马军丽,逄立艳,钟蕾,等.芬太尼的滥用及监测管理[J].临床药物治疗杂志,2012,10(6):44-47.
[9] International Narcotics Control Board. Report of the international narcotics control board for 2009[R]. New York:INCB,2010.
[10] Grabicova K,Grabic R,Fedorova G,et al. Bioaccumulation of psychoactive pharmaceuticals in fish in an effluent dominated stream[J]. Water Research,2017,124:654-662.
[11]国家食品药品监督管理总局.国家药物滥用监测年度报告(2016年)[EB/OL]. http://www. samr. cfda. gov. cn/WS01/CL1033/175995. html,2017-08-11.
[12] Fentanyl and its anolognes-50 years on[J]. Global Smart Update,UNODC,2017,17:3-8.
[13] Buǐiˇc M,GrabicováK,Kubec J,et al. Environmentally relevant concentrations of tramadol and citalopram alter behaviour of an aquatic invertebrate[J]. Aquatic Toxicology,2018,200:226-232.
[14] Sehonova P,Plhalova L,Blahova J,et al. Toxicity of naproxen sodium and its mixture with tramadol hydrochloride on fish early life stages[J]. Chemosphere,2017,188:414-423.
[15] Zuccato E,Chiabrando C,Castiglioni S,et al. Cocaine in surface waters:a new evidence-based tool to monitor community drug abuse[J]. Environmental Health,2005,4:14.
[16] Zuccato E,Chiabrando C, Castiglioni S, et al. Estimating community drug abuse by wastewater analysis[J]. Environmental Health Perspectives,2008,116(8):1027-1032.
[17] Li J,Hou L L,Du P,et al. Estimation of amphetamine and methamphetamine uses in Beijing through sewage-based analysis[J]. Science of the Total Environment,2014,490:724-732.
[18] Khan U,van Nuijs A L N,Li J,et al. Application of a sewagebased approach to assess the use of ten illicit drugs in four Chinese megacities[J]. Science of the Total Environment,2014,487:710-721.
[19] Du P,Li K Y,Li J,et al. Methamphetamine and ketamine use in major Chinese cities,a nationwide reconnaissance through sewagebased epidemiology[J]. Water Research,2015,84:76-84.
[20] Du P,Zhou Z L,Bai Y Q,et al. Estimating heroin abuse in major Chinese cities through wastewater-based epidemiology[J].Science of the Total Environment,2017,605-606:158-165.
[21] Du P,Zhou Z L,Huang H M,et al. Estimating population exposure to phthalate esters in major Chinese cities through wastewater-based epidemiology[J]. Science of the Total Environment,2018,643:1602-1609.
[22] Rodayan A,Majewsky M,Yargeau V. Impact of approach used to determine removal levels of drugs of abuse during wastewater treatment[J]. Science of the Total Environment,2014,487:731-739.
[23] Tscharke B J,Chen C,Gerber J P,et al. Temporal trends in drug use in Adelaide,South Australia by wastewater analysis[J]. Science of the Total Environment,2016,565:384-391.
[24] Rúa-Gómez P C, Püttmann W. Occurrence and removal of lidocaine, tramadol, venlafaxine, and their metabolites in German wastewater treatment plants[J]. Environmental Science and Pollution Research,2012,19(3):689-699.
[25]高婷婷,杜鹏,徐泽琼,等.污水中常见违禁药物分析方法优化及验证[J].环境科学,2017,38(1):201-211.Gao T T,Du P,Xu Z Q,et al. Optimization and validation of the analytical method to detect common illicit drugs in wastewater[J]. Environmental Science,2017,38(1):201-211.
[26]陈培培,杜鹏,周子雷,等.污水中新精神活性物质的分析方法优化及验证[J].环境科学,2018,39(8):3736-3743.Chen P P,Du P,Zhou Z L,et al. Optimization and validation of the analytical method to detect new psychoactive substances in wastewater[J]. Environmental Science,2018,39(8):3736-3743.
[27] Baker D R,Kasprzyk-Hordern B. Multi-residue determination of the sorption of illicit drugs and pharmaceuticals to wastewater suspended particulate matter using pressurised liquid extraction,solid phase extraction and liquid chromatography coupled with tandem mass spectrometry[J]. Journal of Chromatography A,2011,1218(44):7901-7913.
[28] Mackul'ak T,BiroováL,Gál M,et al. Wastewater analysis:the mean of the monitoring of frequently prescribed pharmaceuticals in Slovakia[J]. Environmental Monitoring and Assessment,2016,188(1):18.
[29]枸橼酸芬太尼注射液说明书. 2010年版.宜昌人福药业有限责任公司[EB/OL]. https://wenku. baidu. com/view/69b12972168884868762d6b6. html,2010-10-07.
[30]盐酸曲马多缓释片说明书. 2007年版.黑龙江龙桂制药有限公司[EB/OL]. https://wenku. baidu. com/view/3047bafe941ea76e58fa04c1. html,2007-03-27.
[31]李博,王志谨,曹军,等.污水处理传统工艺与新工艺出水中有机提取物的雌激素样作用比较[J].卫生研究,2014,43(3):477-482.Li B,Wang Z J,Cao J,et al. Estrogenic activity of organic extracts in the effluents treated by present treatment and the new process[J].Journal of Hygiene Research,2014,43(3):477-482.
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