秦曉雷,章濤,孫紅文,*
1. 南開(kāi)大學(xué)環(huán)境科學(xué)與工程學(xué)院 環(huán)境污染過(guò)程與基準(zhǔn)教育部重點(diǎn)實(shí)驗(yàn)室,天津 300350 2. 中山大學(xué)環(huán)境科學(xué)與工程學(xué)院 環(huán)境污染控制與修復(fù)技術(shù)廣東省重點(diǎn)實(shí)驗(yàn)室,廣州 510275
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中國(guó)室內(nèi)和室外灰塵中鄰苯二甲酸酯的分布和健康風(fēng)險(xiǎn)評(píng)價(jià)
秦曉雷1,章濤2,#,孫紅文1,*
1. 南開(kāi)大學(xué)環(huán)境科學(xué)與工程學(xué)院 環(huán)境污染過(guò)程與基準(zhǔn)教育部重點(diǎn)實(shí)驗(yàn)室,天津 300350 2. 中山大學(xué)環(huán)境科學(xué)與工程學(xué)院 環(huán)境污染控制與修復(fù)技術(shù)廣東省重點(diǎn)實(shí)驗(yàn)室,廣州 510275
鄰苯二甲酸酯(PAEs)是一類內(nèi)分泌干擾物,作為塑料添加劑被大量生產(chǎn)和使用,其環(huán)境污染和風(fēng)險(xiǎn)評(píng)價(jià)已成為當(dāng)今關(guān)注的焦點(diǎn)。對(duì)中國(guó)各地區(qū)88個(gè)室內(nèi)灰塵樣品和86個(gè)室外灰塵樣品進(jìn)行了調(diào)查,發(fā)現(xiàn)鄰苯二甲酸酯在兩類灰塵中廣泛存在,10種鄰苯二甲酸酯的總濃度分別為9.60~4 130 μg·g-1dw和0.102~1 430 μg·g-1dw,且室內(nèi)灰塵中鄰苯二甲酸酯含量高于室外灰塵。研究還表明,不同地區(qū)的鄰苯二甲酸酯含量差異很大,但鄰苯二甲酸(2-乙基己基)酯(DEHP)、鄰苯二甲酸二丁酯(DnBP)和鄰苯二甲酸二異丁酯(DiBP)在各地區(qū)都是主要組分,三者總量占總PAEs的95%以上。估算了成人和兒童每天通過(guò)灰塵攝入DEHP、DnBP、鄰苯二甲酸二乙酯(DEP)的總量分別為5.32×10-2~1.81、2.21×10-2~0.595、1.90×10-4~5.62×10-3μg·kg-1bw·d-1和1.20~8.32、0.704~3.47、4.48×10-3~2.43×10-2μg·kg-1bw·d-1;灰塵中DEHP對(duì)成人和兒童的致癌風(fēng)險(xiǎn)(R)分別為7.45×10-7~2.53×10-6和1.68×10-5~1.16×10-4。上述研究結(jié)果為進(jìn)一步評(píng)價(jià)該類物質(zhì)健康風(fēng)險(xiǎn)提供科學(xué)依據(jù)和基礎(chǔ)資料。
鄰苯二甲酸酯;室內(nèi)灰塵;室外灰塵;分布;健康風(fēng)險(xiǎn)評(píng)價(jià)
Received 30 November 2015 accepted 27 January 2016
鄰苯二甲酸酯(phthalate esters)是一種廣泛應(yīng)用的有機(jī)合成化學(xué)品,主要用作塑料增塑劑,還廣泛應(yīng)用于印染、涂料及個(gè)人護(hù)理品等的生產(chǎn)[1-3]。其中,應(yīng)用最為廣泛的是鄰苯二甲酸(2-乙基己基)酯(DEHP),其他重要的還有鄰苯二甲酸二甲酯(DMP)、鄰苯二甲酸二乙酯(DEP)、鄰苯二甲酸二丁酯(DnBP)、鄰苯二甲酸二異丁酯(DiBP)、鄰苯二甲酸二辛酯(DnOP)、鄰苯二甲酸二己酯(DnHP)、鄰苯二甲酸丁基芐基酯(BBP)、鄰苯二甲酸二環(huán)己酯(DCHP)以及鄰苯二甲酸二壬酯(DnNP)等。PAEs作為增塑劑是以范德華力或氫鍵與塑料分子結(jié)合,因此在使用過(guò)程中,遇水或有機(jī)溶劑時(shí)極易被釋放出來(lái),對(duì)環(huán)境造成污染[4]。近年來(lái),在各種環(huán)境介質(zhì)甚至人體中都發(fā)現(xiàn)了PAEs的存在,其已成為地球上最廣泛的污染之一[5]。
PAEs具有雌激素作用,能夠干擾人體正常的內(nèi)分泌系統(tǒng),從而影響生殖[6-9];也有研究發(fā)現(xiàn)該類化合物有致癌、致畸、致突變[10]和致哮喘[11]的作用。
本研究對(duì)中國(guó)各地區(qū)的室內(nèi)和室外灰塵中10種鄰苯二甲酸酯(DEHP、DMP、DEP、DnBP、DiBP、DnOP、DnHP、BBP、DCHP和DnNP)的含量和分布進(jìn)行了調(diào)查,并對(duì)其人體暴露進(jìn)行了初步評(píng)價(jià),從而為進(jìn)一步研究該類物質(zhì)的健康風(fēng)險(xiǎn)提供科學(xué)依據(jù)和基礎(chǔ)資料。
1.1 樣品采集
所有樣品采集于2013年1~4月,包括全國(guó)各個(gè)地區(qū)(表1)。室內(nèi)灰塵樣品包括家庭(n=59)和工作場(chǎng)所(包括商場(chǎng)和學(xué)校,n=29)兩類。
表1 采樣點(diǎn)在我國(guó)6個(gè)行政區(qū)分布[12]
表2 儀器分析參數(shù)
室外灰塵是離地面1 m以上的窗臺(tái)或建筑表面的落塵。所有樣品用毛刷和錫箔紙采集,然后風(fēng)干,過(guò)金屬網(wǎng)篩,再轉(zhuǎn)移到高錳酸鉀-硫酸洗液清洗過(guò)的玻璃離心管中,在-20 ℃保存待用。
1.2 樣品分析
分析純的標(biāo)準(zhǔn)品及d4標(biāo)記的內(nèi)標(biāo)購(gòu)自AccuStandard (New Haven,CT,USA),純度> 99%。分析純的正己烷和丙酮購(gòu)自J T Baker (Phillipsburg,NJ,USA)。
取0.05~0.1 g室內(nèi)或室外灰塵樣品于15 mL玻璃離心管中,加入250 ng內(nèi)標(biāo),室溫下振蕩平衡3 h。然后用正己烷:丙酮(4:1 V/V)萃取,每次加入正己烷:丙酮(4:1 V/V)4 mL,振蕩30 min。然后在4 000 r·min-1離心5 min,移出上清液。這一過(guò)程重復(fù)3次,合并上清液,氮吹濃縮至1 mL,待測(cè)。
采用島津GC/MS-QP 2010 Plus系統(tǒng),儀器條件見(jiàn)表2。m/z 163、279、149分別用來(lái)定量DMP、DnOP和其他8種物質(zhì)。方法回收率76%~130%,10種物質(zhì)定量限(LOQ)均為0.01 μg·g-1。
1.3 室內(nèi)灰塵中PAEs的暴露評(píng)價(jià)
根據(jù)美國(guó)環(huán)保局(USEPA)提供的模型略微改進(jìn)(1)[13],估算成人和兒童每天通過(guò)3種不同途徑(經(jīng)口、皮膚、呼吸)從灰塵攝入的PAEs量(ADD):
(1)
其中,ADDingest、ADDdermal、ADDinhale分別表示經(jīng)口、皮膚、呼吸途徑攝入灰塵中PAEs量,μg·kg-1bw·d-1;IngR為灰塵攝食率,mg·d-1,對(duì)于成人和學(xué)前兒童分別為110和200 mg·d-1;F表示每天在各場(chǎng)所時(shí)間比例,對(duì)成人,在室內(nèi)與室外比例為100%和0%,對(duì)兒童,在室內(nèi)和室外比例分別為83%和17%;SA表示皮膚接觸面積,cm2,對(duì)成人為3 300 cm2,對(duì)兒童為2 800 cm2;AFdust表示皮膚吸附因子,0.2 mg·cm-2;ABS表示皮膚吸附比,對(duì)DEHP、DnBP和DEP,其值分別為2.3%、0.45%和0.74%;BW為體重,kg,成人和兒童分別為61.5和15 kg;IRinhalation為呼吸速率,m3·d-1,成人和兒童分別為20和10 m3·d-1;PEF為顆粒物消除因子,1.36×106m3·g-1。
灰塵中PAEs的致癌風(fēng)險(xiǎn)(R)估算如模型(2)[14]:
R=q×ADD
(2)
表3 室內(nèi)和室外灰塵中PAEs的濃度
其中,q表示劑量-反應(yīng)關(guān)系確定的致癌斜率因子,(mg·kg-1bw·d-1)-1,對(duì)于DEHP,其值為0.014 (mg·kg-1bw·d-1)-1[15];ADD表示每天通過(guò)灰塵攝入PAEs量,mg·kg-1bw·d-1。
2.1 室內(nèi)和室外灰塵中PAEs分布
室內(nèi)灰塵中的PAEs濃度水平見(jiàn)表3。10種PAEs中DEHP、DiBP、DnBP、DMP和DEP可100%檢出,DnHP和DCHP檢出率較低,分別為75%和69%。10種PAEs的總濃度范圍9.60~4130 μg·g-1dw,均值為599 μg·g-1dw。DEHP含量最高,均值為470 μg·g-1dw;DiBP含量次之,均值為62.1 μg·g-1dw。
圖1 室內(nèi)和室外灰塵中PAEs分布Fig. 1 Distribution of phthalate esters in indoor and outdoor dust samples
圖2 不同場(chǎng)所室內(nèi)灰塵PAEs分布比較Fig. 2 Comparison of phthalate esters in indoor dust in different types of places
室外灰塵中總PAEs濃度范圍0.102~1 430 μg·g-1dw,均值濃度為216 μg·g-1dw(表3),其中DnBP和DEHP檢出率最高(100%),DnHP檢出率最低(55%)。DEHP在室外灰塵的均值最高,為159 μg·g-1dw,DnBP次之,為25.2 μg·g-1dw。
本文還比較了來(lái)自不同場(chǎng)所的室內(nèi)灰塵中鄰苯二甲酸酯的水平(圖2),家庭室內(nèi)灰塵中鄰苯二甲酸酯含量變化范圍相對(duì)較窄,平均值低于工作場(chǎng)所。這可能與某些工作場(chǎng)所較多使用塑料、紙張等含有鄰苯二甲酸酯的相關(guān)產(chǎn)品有關(guān)。
2.2 灰塵中PAEs的人體暴露評(píng)價(jià)
表4列出了成人和兒童對(duì)于3種重要PAEs的每日平均攝入量(ADD)。成人每天通過(guò)灰塵攝入DEHP、DnBP和DEP的總量分別為5.32×10-2~1.81、2.21×10-2~0.595、1.90×10-4~5.62×10-3μg·kg-1bw·d-1。兒童每天通過(guò)灰塵攝入DEHP、DnBP和DEP的總量分別為1.20~8.32、0.704~3.47、4.48×10-3~2.43×10-2μg·kg-1bw·d-1。進(jìn)一步估算灰塵中DEHP對(duì)成人和兒童的致癌風(fēng)險(xiǎn)(R)分別為7.45×10-7~2.53×10-6和1.68×10-5~1.16×10-4??梢?jiàn)這3種物質(zhì)對(duì)兒童的暴露風(fēng)險(xiǎn)要高于成人。
鄰苯二甲酸酯在中國(guó)室內(nèi)和室外灰塵中廣泛存在,室內(nèi)灰塵中10種所監(jiān)測(cè)PAEs的總濃度均值為599 μg·g-1dw。DEHP、DiBP和DnBP是主要的鄰苯二甲酸酯類化合物,其中DEHP是優(yōu)先污染物,其最高濃度可達(dá)4 012 μg·g-1dw,均值為470 μg·g-1dw,略低于中國(guó)其他報(bào)道[16-18];與其他國(guó)家相比,低于挪威(640 μg·g-1dw)[19]和丹麥(858 μg·g-1dw)[20],但高于美國(guó)(187 μg·g-1dw)[16]和德國(guó)(416 μg·g-1dw)[21]。DnBP含量遠(yuǎn)遠(yuǎn)低于DEHP,其最高濃度僅為266 μg·g-1dw,均值為53.3 μg·g-1dw,低于瑞典(150 μg·g-1dw)[22]、德國(guó)(87 μg·g-1dw)[21]和意大利(799 μg·g-1dw)[23],但高于美國(guó)(10.3 μg·g-1dw)[24]和日本(16.6 μg·g-1dw)[25]。因此可以判斷,中國(guó)PAEs污染在世界上處于中等水平。
室外灰塵中PAEs濃度遠(yuǎn)低于室內(nèi)灰塵,其均值是室內(nèi)灰塵的1/3,說(shuō)明DEHP主要來(lái)自于室內(nèi),這與其用途有關(guān),PAEs主要用于與人民生活或工作中息息相關(guān)的產(chǎn)品中。在室外灰塵中DEHP仍為優(yōu)先污染物,其均值為159 μg·g-1dw,DnBP的均值25.2 μg·g-1dw,兩者的差異較室內(nèi)低,再次說(shuō)明室內(nèi)空氣是污染的來(lái)源,某些室內(nèi)場(chǎng)所具有異常高值的污染水平,造成室內(nèi)灰塵DEHP的平均濃度異常高。本文調(diào)查的全國(guó)(159 μg·g-1dw)或中南地區(qū)(105 μg·g-1dw)室外灰塵中DEHP含量低于中南地區(qū)的廣州(205 μg·g-1dw)[26],但是高于香港(92.4 μg·g-1dw)[26]。而本研究中室外灰塵中DnBP含量在全國(guó)(25.2 μg·g-1dw)或中南地區(qū)(13.6 μg·g-1dw)的平均水平都高于廣州(12.5 μg·g-1dw)[26]和香港(1.28 μg·g-1dw)[26]。比較PAEs在我國(guó)6個(gè)行政區(qū)的水平,發(fā)現(xiàn)具有很大差異,只是經(jīng)濟(jì)社會(huì)水平不能完全解釋這種差異,還與溫度等自然條件有關(guān)。如,在東北地區(qū)溫度低,有機(jī)污染物向顆粒物分配的傾向性增高,這可以部分解釋東北地區(qū)PAEs在灰塵中有較高的水平,特別是室內(nèi)灰塵與室外灰塵差別較小,而其他地區(qū)的室內(nèi)外灰塵中PAEs的水平則具有較大差異[27]。
人體暴露的初步評(píng)價(jià)表明,由于生活與活動(dòng)習(xí)慣不同,兒童對(duì)于PAEs的攝入量和致癌風(fēng)險(xiǎn)要高于成人。本文的估算印證了文獻(xiàn)中發(fā)現(xiàn)在兒童尿液中PAEs代謝產(chǎn)物的水平明顯高于成人[28-29]。但無(wú)論成人還是兒童,DEHP和DnBP的攝入量都未超過(guò)USEPA的參考值(DEHP:20 μg·kg-1bw·d-1;DnBP:100 μg·kg-1bw·d-1)[10]。對(duì)3種途徑各自貢獻(xiàn),這兩類人群,經(jīng)口攝入都是最主要的暴露途徑,其次是經(jīng)皮膚,通過(guò)呼吸的貢獻(xiàn)率遠(yuǎn)小于其他兩種途徑。值得注意的是,對(duì)成人及兒童,灰塵中DEHP的都有一定的致癌風(fēng)險(xiǎn),特別是兒童,其致癌風(fēng)險(xiǎn)最低值為USEPA所規(guī)定參考值(1.0×10-6)[15]的16.8倍。因此,這清楚地表明了灰塵中PAEs污染已經(jīng)對(duì)國(guó)人構(gòu)成較大威脅。
表4 DEHP、DnBP和DEP每日平均攝入量(ADD)估算值
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Occurrence of Phthalate Esters in Indoor and Outdoor Dust in China: Distribution and Risk Assessment
Qin Xiaolei1, Zhang Tao2,#, Sun Hongwen1,*
1. Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Sciences and Engineering, Nankai University, Tianjin 300071, China 2. Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology,School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China
Phthalate esters (PAEs) are known as endocrine disruptors and have been widely produced and used, and hence the environment pollution and risk assessment of PAEs has become a hot topic currently. In this study, a total of 88 indoor dust and 86 outdoor dust samples were investigated in China. PAEs were widely found in the two types of dust samples, and total concentrations of the 10 PAEs were 9.60~4 130 μg·g-1dw and 0.102~1 430 μg·g-1dw, respectively. The levels of PAEs in indoor dust were higher than those in outdoor dust. The concentrations of PAEs varied greatly in different areas; however, bis(2-ethylhexyl) phthalate (DEHP), di-n-butyl phthalate (DnBP) and di-iso-butyl phthalate (DiBP) were always the main analogues in various areas, and the sum of the three accounts for over 95% of the total PAEs. Average daily dose (ADD) was estimated via indoor and outdoor dust; and the ADDs of DEHP, DnBP, diethyl phthalate (DEP) for adults and children were 5.32×10-2~1.81, 2.21×10-2~0.595, 1.90×10-4~5.62×10-3μg·kg-1bw·d-1and 1.20~8.32, 0.704~3.47, 4.48×10-3~2.43×10-2μg·kg-1bw·d-1, respectively. The calculated cancer risks (R) caused by dust DEHP exposure for adults and children were 7.45×10-7~2.53×10-6and 1.68×10-5~1.16×10-4, respectively. These results have provided basic data for further evaluation on health risk of PAEs.
phthalate esters; indoor dust; outdoor dust; distribution; risk assessment
10.7524/AJE.1673-5897.20151130004
國(guó)家自然科學(xué)基金(No. 21207071,No. 41225014)
秦曉雷(1987-),男,博士研究生,研究方向?yàn)樾滦臀廴疚锱c健康,E-mail: leiix@163.com;
*通訊作者(Corresponding author), E-mail: sunhongwen@nankai.edu.cn;
2015-11-30 錄用日期:2016-01-27
1673-5897(2016)2-231-07
X171.5
A
簡(jiǎn)介:章濤(1982-),男,環(huán)境科學(xué)博士,副教授,主要研究方向新型污染物與健康。
孫紅文(1967-),女,環(huán)境化學(xué)博士,教授,主要研究方向環(huán)境化學(xué),發(fā)表學(xué)術(shù)論文130余篇。
秦曉雷, 章濤, 孫紅文. 中國(guó)室內(nèi)和室外灰塵中鄰苯二甲酸酯的分布和健康風(fēng)險(xiǎn)評(píng)價(jià)[J]. 生態(tài)毒理學(xué)報(bào),2016, 11(2): 231-237
Qin X L, Zhang T, Sun H W. Occurrence of phthalate esters in indoor and outdoor dust in China: Distribution and risk assessment [J]. Asian Journal of Ecotoxicology, 2016, 11(2): 231-237 (in Chinese)
#共同通訊作者(Co-corresponding author), E-mail: bkzhangtao010@163.com