北京市人群尿液中羟基多环芳烃的影响因素
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摘要
于2016年11、12月以北京市3个典型区域的431名普通居民为研究对象,平均年龄(62.80±10.42)岁.以液相色谱联合质谱检测人群尿液中2-OHNap、1-OHNap、2-OHFul、1+9-OHPhe、2-OHPhe、3-OHPhe、4-OHPhe及1-OHPyr浓度水平,并对研究人群进行问卷调查.结果表明,全部人群尿液中2-OHNap、1-OHNap、2-OHFul、∑OHPhe、1-OHPyr浓度中位数水平分别为2.99,3.46,4.24,1.49,0.35μg/g Cr.Logistics回归分析显示,吸烟者尿液中2-OHNap、1-OHNap、2-OHFul、1-OHPyr发生高浓度的可能性分别是不吸烟者的9.83,6.32,4.51,1.89倍;年龄组每增加一个等级,导致2-OHNap、1-OHNap、∑OHPhe、1-OHPyr发生高浓度的可能性分别增加了0.48,0.44,0.31,0.46倍;教育程度每增加一个等级,导致2-OHFul发生高浓度的可能性降低了0.44倍.相关性分析显示,人体尿液中2-OHNap的浓度与环境空气中的萘的浓度呈正相关关系.人体尿液中2-OHNap主要来源于城市空气中的萘.影响北京市典型区域人群尿样中羟基多环芳烃浓度升高的主要因素为吸烟、年龄增高以及受教育程度较低.
The aim of this study is to investigate the levels of polycyclicaromatic hydrocarbons(PAHs) metabolites in the urine collected from a representative resident sample in Beijing and the relevant influencing factors. The resident sample consisted of 431 ordinary residents(average age(62.80±10.42)) recruited in three typical regions of Beijing in November and December 2016. The concentrations of 2-OHNap, 1-OHNap, 2-OHFul 1+9-OHPhe, 2-OHPhe, 3-OHPhe, 4-OHPhe and 1-OHPyr in the urine samples were studied by high performance liquid chromatography with mass spectrometry(LC-MS). Information of the subjects was gathered by a unified questionnaire. The median concentration of 2-OHNap, 1-OHNap, 2-OHFul, ∑OHPhe and 1-OHPyr in the urine samples was 2.99, 3.46, 4.24, 1.49, 0.35μg/g Cr, respectively. Logistics regression analysis showed that the probability of high concentration of 2-OHNap, 1-OHNap, 2-OHFul and 1-OHPyr for smokers was 9.83, 6.32, 4.51 and 1.89 times higher than that of non-smokers, respectively. The probability of high concentration of 2-OHNap, 1-OHNap, ∑OHPhe and 1-OHPyr was shown to increase by 0.48, 0.44, 0.31 and 0.46 times with each increased age level, respectively. The probability of high concentration of 2-OHFul was decreased by 0.44 times with each increased level in education attainment. The study indicated that 2-OHNap,2-OHFul andS∑OHPhe in human urine were mainly derived from naphthalene, fluorene and phenanthrene in urban air. And the major factors influencing the increase of the concentrations of PAHs' metabolites in human urine were smoking, age and relatively low educational level.
The aim of this study is to investigate the levels of polycyclicaromatic hydrocarbons(PAHs) metabolites in the urine collected from a representative resident sample in Beijing and the relevant influencing factors. The resident sample consisted of 431 ordinary residents(average age(62.80±10.42)) recruited in three typical regions of Beijing in November and December 2016. The concentrations of 2-OHNap, 1-OHNap, 2-OHFul 1+9-OHPhe, 2-OHPhe, 3-OHPhe, 4-OHPhe and 1-OHPyr in the urine samples were studied by high performance liquid chromatography with mass spectrometry(LC-MS). Information of the subjects was gathered by a unified questionnaire. The median concentration of 2-OHNap, 1-OHNap, 2-OHFul, ∑OHPhe and 1-OHPyr in the urine samples was 2.99, 3.46, 4.24, 1.49, 0.35μg/g Cr, respectively. Logistics regression analysis showed that the probability of high concentration of 2-OHNap, 1-OHNap, 2-OHFul and 1-OHPyr for smokers was 9.83, 6.32, 4.51 and 1.89 times higher than that of non-smokers, respectively. The probability of high concentration of 2-OHNap, 1-OHNap, ∑OHPhe and 1-OHPyr was shown to increase by 0.48, 0.44, 0.31 and 0.46 times with each increased age level, respectively. The probability of high concentration of 2-OHFul was decreased by 0.44 times with each increased level in education attainment. The study indicated that 2-OHNap,2-OHFul andS∑OHPhe in human urine were mainly derived from naphthalene, fluorene and phenanthrene in urban air. And the major factors influencing the increase of the concentrations of PAHs' metabolites in human urine were smoking, age and relatively low educational level.
引文
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[11]Li Z,Sandau C D,Romanoff L C,et al.Concentration and profile of22 urinary polycyclic aromatic hydrocarbon metabolites in the USpopulation[J].Environmental Research,2008,107(3):320-331.
[12]夏凌.石化区环境空气中多环芳烃的健康风险评估及其对周边居民内暴露的影响[D].广州:暨南大学,2014.Xia L,Health risk assessment of atmospheric PAHs and its impact on internal exposure in the residents around a petrochemical area[D].Guangzhou:Jinan University,2014.
[13]庞月红,马芸,崔燕,等.多环芳烃暴露生物标志物羟基多环芳烃检测方法的研究进展[J].环境与健康杂志,2012,29(6):567-569.Pang Y H,Ma Y,Cui Y,et al.Progress on detection methods for hydroxyl polycyclic aromatic hydrocarbons as a biomarker of exposure to polycyclic aromatic hydrocarbons[J].Journal of Environment and Health,2012,29(6):567-569.
[14]金梦,王梓,黎玉清,等.石化企业周边儿童多环芳烃内暴露负荷的时间变异性[J].中国环境科学,2018,38(5):345-352.Jin M,Wang Z,Li Y Q,et al.The research on the temporal variability of the internal exposure levels of polycyclic aromatic hydrocarbons in children around the petrochemical enterprise[J].China Environmental Science,2018,38(5):345-352.
[15]李新荣,赵同科,于艳新,等.北京地区人群对多环芳烃的暴露及健康风险评价[J].农业环境科学学报,2009,28(8):1758-1765.Li X R,Zhao T K,Yu Y X,et al.Population exposure to PAHS and the health risk assessment in Beijing area[J].Journal of AgroEnvironment Science,2009,28(8):1758-1765.
[16]张娟,吴建芝,刘燕.北京市绿地土壤多环芳烃分布及健康风险评价[J].中国环境科学,2017,37(3):1146-1153.Zhang J,Wu J Z,Liu Y.Polycyclic aromatic hydrocarbons in urban green space of Beijing:distribution and potential risk[J].China Environmental Science,2017,37(3):1146-1153.
[17]路玲,张爱武,康孝岩.北京市大气污染物时空变化特征[J].地球科学前沿,2018,8(3):673-682.Lu L,Zhang A W,Kang X Y.Spatial and temporal variation characteristics of air pollutants in Beijing[J].Frontiers of Earth Science,2018,8(3):673-682.
[18]孟倩倩,李炜宾,周小林,等.非污染区普通人群尿中多环芳烃羟基代谢产物初步调查[J].环境与健康杂志,2016,33(4):360-363.Meng Q Q,Li W B,Zhou X L,et al.Preliminary investigation of polycyclic aromatic hydrocarbons(PAHs)hydroxyl metabolites in urine of general population in non-polluted areas[J].Journal of Environment and Health,2016,33(4):360-363.
[19]谭振,陆少游,吴宏海,等.非职业暴露居民多环芳烃内暴露水平调查[J].环境与健康杂志,2013,30(9):830-831.Tan Z,Lu S Y,Wu H H,et al.Survey of PAHs exposure levels in non-occupational exposed residents[J].Journal of Environment and Health,2013,30(9):830-831.
[20]U.S.CDC.Fourth National Report on Human Exposure to Environmental Chemicals[R].Atlanta,GA:CDC,2013.
[21]岳强,范瑞芳,于志强,等.焦化工人尿中多种多环芳烃单羟基代谢物的调查[J].环境与健康杂志,2010,27(8):86-689.Yue Q,Fan R F,Yu Z Q,et al.Levels of urinary mono-hydroxylated metabolites of PAHs in coke-oven workers[J].Journal of Environment and Health,2010,27(8):686-689.
[22]陆少游,龚诗涵,袁晶,等.我国某塑料垃圾拆解地周边居民多环芳烃内暴露水平调查[J].环境化学,2012,31(5):593-598.Lu S Y,Gong S H,Yuan J,et al.The exposure level of polycyclic aromatic hydrocarbons(PAHs)in the neighborhood of a plastic waste disposal site in China[J].Environmental Chemistry,2012,31(5):593-598.
[23]范瑞芳.广州等城市中学生与电子垃圾拆解地-贵屿镇人群尿中多环芳烃羟基代谢物的初步研究[D].北京:中国科学院研究生院,2007.Fan R F.Preliminary study of urinary PAHs metabolites for students in Pearl River Delta and occupational population in Guiyu-an electronic waste recycling site[D].Beijing:Chinese academy of sciences.2007.
[24]王英锋,张姗姗,李杏茹,等.北京大气颗粒物中多环芳烃浓度季节变化及来源分析[J].环境化学,2010,29(3):369-375.Wang Y F,Zhang S S,Li X R,et al.Seasonal variation and source analysis of PAHs concentration in atmospheric particulate matter in Beijing[J].Environmental Chemistry,2010,29(3):369-375.
[25]Ding Y S,Trommel J S,Yan X J,et al.Determination of 14 polycyclic aromatic hydrocarbons in mainstream smoke from domestic cigarettes[J].Environmental Science&Technology,2015,39(2):471-478.
[26]黄曙海.香烟主流烟雾有毒化学物质含量检测结果[J].应用预防医学,2008,14(6):378-381.Huang S H.Test results of toxic chemicals in mainstream cigarette smoke[J].Journal of Applied Preventive Medicine,2008,14(6):378-381.
[27]张慧涛,张红杰,范燕峰,等.焦化厂工人尿中多环芳烃代谢物浓度的影响因素[J].环境与职业医学,2016,33(4):345-349.Zhang H T,Zhang H J,Fan Y F,et al.Impact factors of urinary polycyclic aromatic hydrocarbon metabolite concentrations in coke oven workers[J].Journal of Environmental&Occupational Medicine,2016,33(4):345-349.
[28]Sherson D,Sigsgaard T,Overgaard E,et al.Interaction of smoking,uptake of polycyclic aromatic hydrocarbons,and cytochrome P450IA2activity among foundry workers[J].British Journal of Industrial Medicine,1992,49(3):197.
[29]Martin F,Hoepfner I,Scherer G,et al.Urinary excretion of hydroxyphenanthrenes after intake of polycyclic aromatic hydrocarbons[J].Environment International,1989,15(1):41-47.
[30]鲍俊哲.城市成年居民尿多环芳烃羟基代谢物水平及其影响因素研究[D].武汉:华中科技大学,2013.Bao J Z.Levels of urinary polycyclic aromatic hydrocarbons metabolites and their affecting factors in an urban adult population in Wuhan[D].Wuhan:Huazhong University of Science and Technology,2013.
[31]岳强.广东某市部分中学生尿液中多种多环芳烃单羟基代谢物暴露水平分析[J].环境污染与防治,2010,32(8):47-50.Yue Q.The pilot analysis on the exposure level of polycyclic aromatic hydrocarbons in a middle school students of Guangdong[J].Environmental Pollution&Control,2010,32(8):47-50.
[32]Guo Y,Senthilkumar K,Alomirah H,et al.Concentrations and profiles of urinary polycyclic aromatic hydrocarbon metabolites(OH-PAHs)in several Asian countries[J].Environmental Science&Technology,2013,47(6):2932-2938.
[2]杜芳芳,杨毅,刘敏,等.上海市表层土壤中多环芳烃的分布特征与源解析[J].中国环境科学,2014,34(4):989-995.Du F F,Yang Y,Liu M,et al.Distribution and source apportionment of polycyclic aromatic hydrocarbons in surface soils in Shanghai[J].China Environmental Science,2014,34(4):989-995.
[3]Kuppusamy S,Thavamani P,Megharaj M,et al.Pyrosequencing analysis of bacterial diversity in soils contaminated long-term with PAHs and heavy metals:Implications to bioremediation[J].Journal of Hazardous Materials,2016,317(5):169-179.
[4]杨发忠,颜阳,张泽志,等.多环芳烃研究进展[J].云南化工,2005,32(2):44-48.Yang F Z,Yan Y,Zhang Z Z,et al.Research advance of polycyclic aromatic hydrocarbons[J].Yunnan Chemical Technology,2005,32(2):44-48.
[5]Lin M,Ning X A,An T,et al.Degradation of polycyclic aromatic hydrocarbons(PAHs)in textile dyeing sludge with ultrasound and Fenton processes:Effect of system parameters and synergistic effect study[J].Journal of Hazardous Materials,2016,307(15):7-16.
[6]Hu T,Zhang J,Chen Y,et al.Status,source and health risk assessment of polycyclic aromatic hydrocarbons(PAHs)in soil from the water level fluctuation zone of the Three Gorges Reservoir,China[J].Journal of Geochemical Exploration,2017,172(1):20-28.
[7]Vanrooij J G,Bodelierbade M M,Jongeneelen F J.Estimation of individual dermal and respiratory uptake of polycyclic aromatic hydrocarbons in 12 coke oven workers[J].British Journal of Industrial Medicine,1993,50(7):623.
[8]Estabrook R W,Saeki Y,Chacos N,et al.Polycyclic hydrocarbon metabolism:A plethora of phenomena[J].Advances in Enzyme Regulation,1981,19(81):3-17.
[9]Grover P L.Pathways involved in the metabolism and activation of polycyclic hydrocarbons[J].Xenobiotica,1986,16(10):915-931.
[10]牛红云,蔡亚岐,魏复盛,等.多环芳烃暴露的生物标志物--尿中羟基多环芳烃[J].化学进展,2006,18(10):1381-1390.Niu H Y,Cai Y Q,Wei F S,et al.Hydroxyl polycyclic aromatic hydrocarbons in human urine as biomarkers of exposure to PAHs[J].Progess in Chemistry,2006,18(10):1381-1390.
[11]Li Z,Sandau C D,Romanoff L C,et al.Concentration and profile of22 urinary polycyclic aromatic hydrocarbon metabolites in the USpopulation[J].Environmental Research,2008,107(3):320-331.
[12]夏凌.石化区环境空气中多环芳烃的健康风险评估及其对周边居民内暴露的影响[D].广州:暨南大学,2014.Xia L,Health risk assessment of atmospheric PAHs and its impact on internal exposure in the residents around a petrochemical area[D].Guangzhou:Jinan University,2014.
[13]庞月红,马芸,崔燕,等.多环芳烃暴露生物标志物羟基多环芳烃检测方法的研究进展[J].环境与健康杂志,2012,29(6):567-569.Pang Y H,Ma Y,Cui Y,et al.Progress on detection methods for hydroxyl polycyclic aromatic hydrocarbons as a biomarker of exposure to polycyclic aromatic hydrocarbons[J].Journal of Environment and Health,2012,29(6):567-569.
[14]金梦,王梓,黎玉清,等.石化企业周边儿童多环芳烃内暴露负荷的时间变异性[J].中国环境科学,2018,38(5):345-352.Jin M,Wang Z,Li Y Q,et al.The research on the temporal variability of the internal exposure levels of polycyclic aromatic hydrocarbons in children around the petrochemical enterprise[J].China Environmental Science,2018,38(5):345-352.
[15]李新荣,赵同科,于艳新,等.北京地区人群对多环芳烃的暴露及健康风险评价[J].农业环境科学学报,2009,28(8):1758-1765.Li X R,Zhao T K,Yu Y X,et al.Population exposure to PAHS and the health risk assessment in Beijing area[J].Journal of AgroEnvironment Science,2009,28(8):1758-1765.
[16]张娟,吴建芝,刘燕.北京市绿地土壤多环芳烃分布及健康风险评价[J].中国环境科学,2017,37(3):1146-1153.Zhang J,Wu J Z,Liu Y.Polycyclic aromatic hydrocarbons in urban green space of Beijing:distribution and potential risk[J].China Environmental Science,2017,37(3):1146-1153.
[17]路玲,张爱武,康孝岩.北京市大气污染物时空变化特征[J].地球科学前沿,2018,8(3):673-682.Lu L,Zhang A W,Kang X Y.Spatial and temporal variation characteristics of air pollutants in Beijing[J].Frontiers of Earth Science,2018,8(3):673-682.
[18]孟倩倩,李炜宾,周小林,等.非污染区普通人群尿中多环芳烃羟基代谢产物初步调查[J].环境与健康杂志,2016,33(4):360-363.Meng Q Q,Li W B,Zhou X L,et al.Preliminary investigation of polycyclic aromatic hydrocarbons(PAHs)hydroxyl metabolites in urine of general population in non-polluted areas[J].Journal of Environment and Health,2016,33(4):360-363.
[19]谭振,陆少游,吴宏海,等.非职业暴露居民多环芳烃内暴露水平调查[J].环境与健康杂志,2013,30(9):830-831.Tan Z,Lu S Y,Wu H H,et al.Survey of PAHs exposure levels in non-occupational exposed residents[J].Journal of Environment and Health,2013,30(9):830-831.
[20]U.S.CDC.Fourth National Report on Human Exposure to Environmental Chemicals[R].Atlanta,GA:CDC,2013.
[21]岳强,范瑞芳,于志强,等.焦化工人尿中多种多环芳烃单羟基代谢物的调查[J].环境与健康杂志,2010,27(8):86-689.Yue Q,Fan R F,Yu Z Q,et al.Levels of urinary mono-hydroxylated metabolites of PAHs in coke-oven workers[J].Journal of Environment and Health,2010,27(8):686-689.
[22]陆少游,龚诗涵,袁晶,等.我国某塑料垃圾拆解地周边居民多环芳烃内暴露水平调查[J].环境化学,2012,31(5):593-598.Lu S Y,Gong S H,Yuan J,et al.The exposure level of polycyclic aromatic hydrocarbons(PAHs)in the neighborhood of a plastic waste disposal site in China[J].Environmental Chemistry,2012,31(5):593-598.
[23]范瑞芳.广州等城市中学生与电子垃圾拆解地-贵屿镇人群尿中多环芳烃羟基代谢物的初步研究[D].北京:中国科学院研究生院,2007.Fan R F.Preliminary study of urinary PAHs metabolites for students in Pearl River Delta and occupational population in Guiyu-an electronic waste recycling site[D].Beijing:Chinese academy of sciences.2007.
[24]王英锋,张姗姗,李杏茹,等.北京大气颗粒物中多环芳烃浓度季节变化及来源分析[J].环境化学,2010,29(3):369-375.Wang Y F,Zhang S S,Li X R,et al.Seasonal variation and source analysis of PAHs concentration in atmospheric particulate matter in Beijing[J].Environmental Chemistry,2010,29(3):369-375.
[25]Ding Y S,Trommel J S,Yan X J,et al.Determination of 14 polycyclic aromatic hydrocarbons in mainstream smoke from domestic cigarettes[J].Environmental Science&Technology,2015,39(2):471-478.
[26]黄曙海.香烟主流烟雾有毒化学物质含量检测结果[J].应用预防医学,2008,14(6):378-381.Huang S H.Test results of toxic chemicals in mainstream cigarette smoke[J].Journal of Applied Preventive Medicine,2008,14(6):378-381.
[27]张慧涛,张红杰,范燕峰,等.焦化厂工人尿中多环芳烃代谢物浓度的影响因素[J].环境与职业医学,2016,33(4):345-349.Zhang H T,Zhang H J,Fan Y F,et al.Impact factors of urinary polycyclic aromatic hydrocarbon metabolite concentrations in coke oven workers[J].Journal of Environmental&Occupational Medicine,2016,33(4):345-349.
[28]Sherson D,Sigsgaard T,Overgaard E,et al.Interaction of smoking,uptake of polycyclic aromatic hydrocarbons,and cytochrome P450IA2activity among foundry workers[J].British Journal of Industrial Medicine,1992,49(3):197.
[29]Martin F,Hoepfner I,Scherer G,et al.Urinary excretion of hydroxyphenanthrenes after intake of polycyclic aromatic hydrocarbons[J].Environment International,1989,15(1):41-47.
[30]鲍俊哲.城市成年居民尿多环芳烃羟基代谢物水平及其影响因素研究[D].武汉:华中科技大学,2013.Bao J Z.Levels of urinary polycyclic aromatic hydrocarbons metabolites and their affecting factors in an urban adult population in Wuhan[D].Wuhan:Huazhong University of Science and Technology,2013.
[31]岳强.广东某市部分中学生尿液中多种多环芳烃单羟基代谢物暴露水平分析[J].环境污染与防治,2010,32(8):47-50.Yue Q.The pilot analysis on the exposure level of polycyclic aromatic hydrocarbons in a middle school students of Guangdong[J].Environmental Pollution&Control,2010,32(8):47-50.
[32]Guo Y,Senthilkumar K,Alomirah H,et al.Concentrations and profiles of urinary polycyclic aromatic hydrocarbon metabolites(OH-PAHs)in several Asian countries[J].Environmental Science&Technology,2013,47(6):2932-2938.