武亞鳳，陳建華，張國(guó)寧，武雪芳，趙鑫，李琴

中國(guó)環(huán)境科學(xué)研究院環(huán)境標(biāo)準(zhǔn)研究所，北京 100012

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武亞鳳，陳建華*，張國(guó)寧，武雪芳，趙鑫，李琴

中國(guó)環(huán)境科學(xué)研究院環(huán)境標(biāo)準(zhǔn)研究所，北京 100012

表1 二英毒性當(dāng)量因子[8,28]Table 1 Toxic equivalency factors of dioxins

1)1997年世界衛(wèi)生組織會(huì)議提出并于1998年發(fā)表在學(xué)術(shù)期刊上；2)2005年世界衛(wèi)生組織會(huì)議提出并于2006年發(fā)表在學(xué)術(shù)期刊上。

表2 美國(guó)PCDDFs的主要來(lái)源[12]Table 2 Main sources of dioxins in American

表2 美國(guó)PCDDFs的主要來(lái)源[12]Table 2 Main sources of dioxins in American

來(lái)源所占比例∕%醫(yī)院廢物焚燒45垃圾和固體廢物焚燒42危險(xiǎn)廢物、黏合劑焚燒4漂白加工3木材燃燒3銅的再循環(huán)利用2森林火災(zāi)和農(nóng)業(yè)秸稈燃燒0.7汽車燃燒0.7下水道污染物燃燒0.2含PCDD∕Fs的化學(xué)物<1鉛循環(huán)利用<0.1

表3 部分國(guó)家和地區(qū)大氣中PCDDFs的毒性當(dāng)量濃度Table 3 The atmospheric toxicity equivalent concentration of PCDDFs in some countries and regions pg I-TEQm3

表3 部分國(guó)家和地區(qū)大氣中PCDDFs的毒性當(dāng)量濃度Table 3 The atmospheric toxicity equivalent concentration of PCDDFs in some countries and regions pg I-TEQm3

地區(qū)時(shí)間區(qū)域類型濃度范圍(平均值)數(shù)據(jù)來(lái)源北京2006-02—2006-12城市0.018～0.644(0.268)文獻(xiàn)[22]天津2008-06—2009-01城市0.0142～0.172(0.0693)夏季0.0898～1.01(0.509)冬季(1.04)夏季電子垃圾拆解場(chǎng)(7.123)冬季電子垃圾拆解場(chǎng)文獻(xiàn)[23]深圳2009-02-25—2009-03-31城市0.014～0.29(0.135)文獻(xiàn)[24]廣州2010—2011城市0.112～5.620文獻(xiàn)[25]重慶2011-01—2011-10城市0.017～0.21(0.094±0.054)文獻(xiàn)[26]臺(tái)灣南部2005-04—2005-12工業(yè)區(qū)0.0319～0.256文獻(xiàn)[27]日本2007國(guó)家0.04文獻(xiàn)[28]加泰羅尼亞(西班牙東北部)1994—2000工業(yè)區(qū)城市和郊區(qū)農(nóng)村0.018～0.9540.013～0.3570.005～0.125文獻(xiàn)[29]葡萄牙1999-01—2004-12國(guó)家0.0017～0.4568文獻(xiàn)[30]美國(guó)休斯頓2002-09—2003-04城市0.004～0.055文獻(xiàn)[31]

圖1 日本二英排放量和大氣環(huán)境水平Fig.1 Dioxin emissions and atmospheric environment levels in Japan

根據(jù)中國(guó)人群暴露參數(shù)手冊(cè)(成人卷)[35]，我國(guó)人群(≥18歲)長(zhǎng)期呼吸量推薦值為15.7 m3d。在PCDDFs暴露濃度為120 pgm3(1.93 pg I-TEQm3)的城市中，按該呼吸量估算，成人通過(guò)呼吸攝入的PCDDFs為30.3 pg I-TEQd。成人體質(zhì)量按60.6 kg計(jì)，則通過(guò)呼吸攝入的PCDDFs毒性當(dāng)量濃度約為0.5 pg-TEQ(kg·d)。世界衛(wèi)生組織標(biāo)準(zhǔn)規(guī)定：PCDDFs通過(guò)呼吸對(duì)人體健康產(chǎn)生影響的限值為0.4 pg-TEQ(kg·d)[36]，從長(zhǎng)期角度來(lái)看，我國(guó)廣州等工業(yè)城市空氣中高毒性當(dāng)量濃度的PCDDFs對(duì)人群健康及壽命均具有潛在的風(fēng)險(xiǎn)。

2.2.1 污染狀況

20世紀(jì)60—80年代，由于五氯酚鈉的大量使用，導(dǎo)致洞庭湖淡水受到污染，PCDDFs濃度為36～345 pgL，平均濃度為191 pgL，對(duì)應(yīng)的毒性當(dāng)量濃度為0.17～0.37 pg-TEQL，平均毒性當(dāng)量濃度為0.28 pg-TEQL[37]，超過(guò)了日本2007年地下水PCDDFs平均毒性當(dāng)量濃度(0.055 pg-TEQL)[28](表4)。2007年，日本97.5%的公用水和99.7%的地下水PCDDFs濃度達(dá)標(biāo)。相對(duì)發(fā)達(dá)國(guó)家而言，我國(guó)雖然缺乏有說(shuō)服力的PCDDFs污染數(shù)據(jù)，但根據(jù)國(guó)外經(jīng)驗(yàn)和有限的數(shù)據(jù)來(lái)看，PCDDFs確實(shí)在我國(guó)水體環(huán)境中存在，且部分超標(biāo)。故未來(lái)幾年甚至幾十年內(nèi)，開(kāi)展PCDDFs的水體污染調(diào)查和控制研究非常有意義[38]。

在科學(xué)研究中，常用水體中生活的魚(yú)類體內(nèi)或者是水體沉積物中PCDDFs的毒性當(dāng)量濃度來(lái)反映水體的污染程度，如為評(píng)估西班牙圖里亞河流中的PCDDFs的污染狀況，學(xué)者選取長(zhǎng)期生活在該河流的淡水魚(yú)——鱒魚(yú)和鰻魚(yú)，測(cè)試其體內(nèi)PCDDFs和多氯聯(lián)苯(PCBs)的濃度(圖2)。由圖2可以看出，鱒魚(yú)和鰻魚(yú)體內(nèi)PCDDs毒性當(dāng)量濃度占總毒性當(dāng)量濃度比例都很大，分別為56%和63%。鱒魚(yú)體內(nèi)總PCDDFs濃度為1.22～1.69 pgg(濕質(zhì)量)；鰻魚(yú)體內(nèi)總PCDDFs濃度為1.62～4.39 pgg(濕質(zhì)量)[39]；對(duì)應(yīng)的毒性當(dāng)量濃度分別為0.18和0.37 pg WHO-TEQg，低于歐洲社區(qū)當(dāng)局設(shè)定的魚(yú)類以及漁產(chǎn)品肉的鮮質(zhì)量最大限值(4 pg WHO-TEQg)[39]。根據(jù)BAF(生物蓄積因子)推斷出水體中PCDDFs類物質(zhì)的濃度相對(duì)較低，未超出食物鏈的耐受值。

表4 1998—2007年日本水體二英毒性當(dāng)量濃度[28]Table 4 The dioxins toxicity equivalent concentration in Japanese water during 1998-2007 pg-TEQL

圖2 多氯聯(lián)苯和PCDDFs在總毒性當(dāng)量 (WHO)中所占比例Fig.2 Contribution of ortho-PCBs, non-ortho PCBs and PCDDFs to the total WHO-TEQ value assuming that non-detected values are equal to the limit of detection

早在20世紀(jì)70年代芬蘭南部Valkjg?rvi湖被氯酚污染，后來(lái)Vartiainen等[40]分別在該湖中央最深處和湖口處選取沉積物巖心，研究被氯酚污染的湖是否伴隨有PCDDFs污染。結(jié)果表明，PCDDFs極易吸附于底泥土壤顆粒物中，呈現(xiàn)出在湖中沉積物巖心PCBs濃度高而PCDDFs濃度低的現(xiàn)象。反映出被氯酚污染的水體經(jīng)過(guò)地下水庫(kù)，底泥土壤對(duì)PCDDFs具有相對(duì)高的凈化能力，且水體PCDDFs污染程度隨深度增加具有降低趨勢(shì)。

2.2.2 暴露情況

飲水中污染物暴露劑量的計(jì)算公式[35]：

(1)

式中：ADD為污染物的日平均暴露量，mg(kg·d)；C為水中污染物的濃度，mgmL；IR為飲水?dāng)z入量，mLd；EF為暴露頻次，da；ED為暴露持續(xù)時(shí)間，a；BW為體質(zhì)量，kg；AT為平均暴露時(shí)間，d。

表5 近年來(lái)發(fā)生的飼料添加劑二英污染事件[41]Table 5 Several events of dioxins pollution in feed additives in recent years

Bien Hoa和Da Nang是越南戰(zhàn)爭(zhēng)期間“橙劑”集運(yùn)儲(chǔ)存空軍基地。對(duì)這2個(gè)地區(qū)食物中PCDDFs進(jìn)行風(fēng)險(xiǎn)評(píng)估，發(fā)現(xiàn)放養(yǎng)式雞的肉蛋類、淡水魚(yú)、蝸牛以及牛肉為高污染風(fēng)險(xiǎn)的食物，PCDDFs濃度為3.8～95 pg-TEQg[43]。而圈養(yǎng)式雞的肉蛋類、海鮮、豬肉、多葉蔬菜、水果、水稻等食物中PCDDFs的濃度相對(duì)較低(0.03～6.1 pg-TEQg)。當(dāng)人體暴露于高污染的食物，Bien Hoa和Da Nang的PCDDFs攝入量分別為60.4～102.8和27.0～148.0 pg-TEQ(kg·d)；而暴露于低污染的食物，Bien Hoa和Da Nang的PCDDFs攝入量分別為3.2～6.2和1.2～4.3 pg-TEQ(kg·d)?？梢?jiàn)當(dāng)暴露于高污染的食品時(shí)，人體PCDDFs的日攝入量遠(yuǎn)超過(guò)1998年WHO-ECEHIPCS重新審議的二英每日可耐受攝入量(tolerable daily intake,TDI，1～4 pg-TEQkg)[44]。

表6 2006年日本二英日均攝入量 [28]Table 6 Daily intake of dioxins at 2006 in Japan

注：每日可耐受攝入量(TDI)為4 pg-TEQ(kg·d)。

2.4 職業(yè)暴露

通常情況下，有害物質(zhì)主要通過(guò)呼吸道吸入、消化道攝入、皮膚滲入3種暴露方式進(jìn)入人體[45]。對(duì)于一般人群而言，PCDDFs主要通過(guò)飲食產(chǎn)生暴露。而諸如焚燒廠、造紙廠、鑄造廠等工人的職業(yè)暴露主要來(lái)自呼吸以及皮膚暴露。PCDDFs對(duì)人體健康的危害程度還取決于PCDDFs的性質(zhì)、空氣動(dòng)力學(xué)直徑、暴露濃度以及暴露時(shí)間[46]。針對(duì)職業(yè)工人高濃度長(zhǎng)時(shí)間的暴露，有研究表明[47]，鑄造廠一線工人在一天工作時(shí)間內(nèi)經(jīng)由呼吸途徑攝入的PCDDFs高出附近成人居民的1.14～9.43倍。另外，Kontsas等[48]研究了芬蘭3個(gè)木材廠(使用氯苯酚鈉作為防腐劑)，發(fā)現(xiàn)職業(yè)接觸工人血液中PCDDFs濃度分別為743、1 124和844 pg-TEQg(以脂肪質(zhì)量計(jì))，顯著高于一般人群。對(duì)作為職業(yè)暴露常見(jiàn)的生物標(biāo)志物的頭發(fā)，采用高分辨氣相色譜-高分辨質(zhì)譜儀檢測(cè)發(fā)現(xiàn)，不同工作環(huán)境下的工人頭發(fā)中的TCDD濃度接近0.1 pgg。而焚化廠、五氯酚生產(chǎn)廠等工人頭發(fā)中的PCDDFs檢測(cè)呈陽(yáng)性[49]。Takata等[50]在2003年對(duì)垃圾焚燒廠和造紙廠的職工進(jìn)行調(diào)查，發(fā)現(xiàn)其血液中的PCDDFs顯著高于對(duì)照組。同年，Kumagai等[51]也做了類似的調(diào)查，結(jié)果與Takata一致。2007年，Paola Zambon對(duì)焚化爐工人的病例對(duì)照研究表明，暴露于PCDDFs的人群肉瘤的發(fā)病風(fēng)險(xiǎn)是對(duì)照組的3.3倍[52]。Lee等[53]對(duì)中國(guó)臺(tái)灣電弧廠、再生銅冶煉廠和再生鋁冶煉廠周圍空氣和人體血液中PCDDFs水平的調(diào)查表明：工人血液中PCDDFs濃度表現(xiàn)為再生鋁冶煉廠工人(21.9 pg WHO-TEQg)>再生銅冶煉廠工人(21.5 pg WHO-TEQg)>電弧廠工人(18.8 pg WHO-TEQg)，均較廢物焚燒廠5 km以內(nèi)居民血液內(nèi)的濃度(14.0 pg WHO-TEQg)高。因此針對(duì)職業(yè)暴露人群，應(yīng)及時(shí)根據(jù)生產(chǎn)工藝摸清PCDDFs產(chǎn)生和存在環(huán)節(jié)，對(duì)這些環(huán)節(jié)采取工程控制、個(gè)體防護(hù)、健康監(jiān)護(hù)等防控措施，盡可能降低暴露風(fēng)險(xiǎn)。

3.1 氯痤瘡

另外，在以往研究中[66]，TCDD所使用的暴露劑量一般為μmolL、nmolL量級(jí)，在誘導(dǎo)人體黃體化粒層細(xì)胞凋亡中存在一定的劑量-效應(yīng)關(guān)系。最新的一項(xiàng)研究表明：使黃體化粒層細(xì)胞分泌的雌二醇-17β(E2)分別暴露于3.1 nmolL、3.1 pmolL和3.1 fmolL劑量的TCDD，發(fā)現(xiàn)體外培養(yǎng)皿中E2的積累量與暴露時(shí)間在統(tǒng)計(jì)學(xué)上呈顯著的關(guān)系，與暴露劑量并無(wú)太大關(guān)系。E2濃度的減少是由于在雌性激素生物合成過(guò)程中，CYP11A1和CYP19A1這2種酶的mRNA表達(dá)受阻。目前基于細(xì)胞系和嚙齒動(dòng)物模型的代謝物組學(xué)評(píng)估TCDD毒性研究還比較少[67]。大多研究結(jié)果只強(qiáng)調(diào)氨基酸和脂質(zhì)(脂肪酸和膽汁酸)代謝的變化情況。而事實(shí)上，在醫(yī)療保健意識(shí)日益提升的環(huán)境下，PCDDFs長(zhǎng)期暴露毒性臨床代謝物組學(xué)研究已經(jīng)是人類最關(guān)切的問(wèn)題。目前，四級(jí)桿-飛行時(shí)間串聯(lián)質(zhì)譜(quadrupole time-of-flight mass spectrometry)技術(shù)支持代謝物非目標(biāo)性篩選，從而可用于尋找新的生物標(biāo)志物。該技術(shù)用極端表現(xiàn)型作為參考標(biāo)準(zhǔn)，采用生物學(xué)知識(shí)和統(tǒng)計(jì)學(xué)工具對(duì)初始數(shù)據(jù)進(jìn)行處理而獲得可表征TCDD中毒的生物標(biāo)志物組。代謝物組學(xué)較基因組學(xué)和蛋白質(zhì)組學(xué)還相對(duì)不成熟，但是作為一種可尋找新生物標(biāo)志物、發(fā)現(xiàn)新代謝途徑的研究組學(xué)方法，在臨床醫(yī)學(xué)上更具研究?jī)r(jià)值。

5 結(jié)語(yǔ)

目前我國(guó)經(jīng)濟(jì)高速發(fā)展，城市垃圾的數(shù)量種類與城市規(guī)模同步增長(zhǎng)。環(huán)境中PCDDFs的污染問(wèn)題日益嚴(yán)重，而我國(guó)又缺乏比較完善的PCDDFs污染防治體系和長(zhǎng)期監(jiān)管機(jī)制。從國(guó)家監(jiān)管層面，我國(guó)應(yīng)該學(xué)習(xí)日本以及歐盟國(guó)家逐步建立PCDDFs不同排放源于不同環(huán)境介質(zhì)的排放限值以及管理政策；參考《二英和呋喃排放識(shí)別和量化標(biāo)準(zhǔn)工具包》并結(jié)合我國(guó)于2010年10月19日發(fā)布的《關(guān)于加強(qiáng)二英污染防治的指導(dǎo)意見(jiàn)》，在京津冀、長(zhǎng)三角、珠三角等重點(diǎn)區(qū)域逐步開(kāi)展PCDDFs排放總量控制試點(diǎn)工作；篩選主要類別源，細(xì)化對(duì)應(yīng)的子類別活動(dòng)過(guò)程，通過(guò)調(diào)查問(wèn)卷獲得更為準(zhǔn)確詳細(xì)的信息，從而逐步更新完善我國(guó)主要行業(yè)涉及鋼鐵、再生有色金屬和廢物焚燒等多個(gè)領(lǐng)域的PCDDFs排放清單；從源頭進(jìn)行治理。從公司企業(yè)層面，特別針對(duì)職業(yè)暴露，應(yīng)大力提高企業(yè)監(jiān)管力度，從根本上弄清楚PCDDFs的排放環(huán)節(jié)，開(kāi)發(fā)簡(jiǎn)易、快速、低廉的分析方法和暴露監(jiān)測(cè)技術(shù)，開(kāi)展小型零散企業(yè)關(guān)停計(jì)劃。從民眾層面，應(yīng)該提高自我保護(hù)意識(shí)，調(diào)整飲食結(jié)構(gòu)，并提高知情權(quán)意識(shí)。

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Pollution Situation and Health Effect of Dioxins

WU Yafeng, CHEN Jianhua, ZHANG Guoning, WU Xuefang, ZHAO Xin, LI Qin

Research Institute of Environmental Standard, Chinese Research Academy of Environmental Sciences, Beijing 100012, China

As persistent toxic pollutants, dioxins, either direct or indirect exposure, are seriously harmful to human. In order to better understand the human exposure to dioxins, the current status of dioxins pollution in the air, water body and food as well as the occupational exposure risk was summarized. The detailed comparisons of the TEQ concentrations of dioxins in the air in industrial cities both at home and aboard were made. It showed that the pollution level of PCDDFs in Guangzhou city, etc. was high, bringing about great security risk to the health of residents. Although there lack representative data of water pollution of dioxins in China, by making a comparison of the TEQ concentrations of dioxins in water samples from Dongting lake (0.28 pg-TEQL) and ground water in Japan(0.055 pg-TEQL), it reflects that some part of the water body has been polluted. Diet is the main exposure pathway to dioxins for common people. An assessment of dioxins concentrations in food from Bien Hoa and Da Nang in View Nam was carried out ,which shows that chicken and eggs of stocking-style chicken, freshwater fish, snails and beef contain more dioxins and furans, while the captive-style chicken and eggs, seafood, pork, leafy vegetables, fruits and rice, etc. have relatively low levels of dioxins. The concentrations of dioxins in typical biomarkers such as blood and hair after occupational exposure were compared to that of general people, and it finds that the former is several times higher than the latter. The management mechanisms of main pollution sources are imperfect. Some suggestions were proposed to carry out pollution control and long-term supervision of dioxins, including: gradually establishing dioxins emission limits and management policies for different sources and various environmental media; gradually launching pilot works of total dioxins emissions control in key areas; gradually updating and improving dioxins emission inventory in China; developing simple, rapid and inexpensive method of analyzing and monitoring techniques for dioxins exposure; and the public raising awareness of self-protection, adjusting the dietary structures and increasing awareness of the right to be informed.

dioxin(PCDDFs); current status of dioxins pollution; exposure risks; health effect

2016-01-08

國(guó)家自然科學(xué)基金項(xiàng)目(21277132)； 國(guó)家環(huán)境保護(hù)公益性行業(yè)科研專項(xiàng)(201309046)

武亞鳳(1991—)，女，碩士，1135936652@qq.com

*通訊作者:陳建華(1970—)，女，研究員，博士，主要從事大氣環(huán)境化學(xué)和環(huán)境標(biāo)準(zhǔn)研究工作，chenjh@craes.org.com

X512

1674-991X(2016)03-0229-10

10.3969j.issn.1674-991X.2016.03.035