二英的污染現狀及健康效應

武亞鳳，陳建華，張國寧，武雪芳，趙鑫，李琴

中國環境科學研究院環境標準研究所，北京 100012

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武亞鳳，陳建華*，張國寧，武雪芳，趙鑫，李琴

中國環境科學研究院環境標準研究所，北京 100012

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

1)1997年世界衛生組織會議提出并于1998年發表在學術期刊上；2)2005年世界衛生組織會議提出并于2006年發表在學術期刊上。

表2 美國PCDDFs的主要來源[12]Table 2 Main sources of dioxins in American

表2 美國PCDDFs的主要來源[12]Table 2 Main sources of dioxins in American

來源所占比例∕%醫院廢物焚燒45垃圾和固體廢物焚燒42危險廢物、黏合劑焚燒4漂白加工3木材燃燒3銅的再循環利用2森林火災和農業秸稈燃燒0.7汽車燃燒0.7下水道污染物燃燒0.2含PCDD∕Fs的化學物<1鉛循環利用<0.1

表3 部分國家和地區大氣中PCDDFs的毒性當量濃度Table 3 The atmospheric toxicity equivalent concentration of PCDDFs in some countries and regions pg I-TEQm3

表3 部分國家和地區大氣中PCDDFs的毒性當量濃度Table 3 The atmospheric toxicity equivalent concentration of PCDDFs in some countries and regions pg I-TEQm3

地區時間區域類型濃度范圍(平均值)數據來源北京2006-02—2006-12城市0.018～0.644(0.268)文獻[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(7.123)冬季電子垃圾拆解場文獻[23]深圳2009-02-25—2009-03-31城市0.014～0.29(0.135)文獻[24]廣州2010—2011城市0.112～5.620文獻[25]重慶2011-01—2011-10城市0.017～0.21(0.094±0.054)文獻[26]臺灣南部2005-04—2005-12工業區0.0319～0.256文獻[27]日本2007國家0.04文獻[28]加泰羅尼亞(西班牙東北部)1994—2000工業區城市和郊區農村0.018～0.9540.013～0.3570.005～0.125文獻[29]葡萄牙1999-01—2004-12國家0.0017～0.4568文獻[30]美國休斯頓2002-09—2003-04城市0.004～0.055文獻[31]

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

根據中國人群暴露參數手冊(成人卷)[35]，我國人群(≥18歲)長期呼吸量推薦值為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，成人通過呼吸攝入的PCDDFs為30.3 pg I-TEQd。成人體質量按60.6 kg計，則通過呼吸攝入的PCDDFs毒性當量濃度約為0.5 pg-TEQ(kg·d)。世界衛生組織標準規定：PCDDFs通過呼吸對人體健康產生影響的限值為0.4 pg-TEQ(kg·d)[36]，從長期角度來看，我國廣州等工業城市空氣中高毒性當量濃度的PCDDFs對人群健康及壽命均具有潛在的風險。

2.2.1 污染狀況

20世紀60—80年代，由于五氯酚鈉的大量使用，導致洞庭湖淡水受到污染，PCDDFs濃度為36～345 pgL，平均濃度為191 pgL，對應的毒性當量濃度為0.17～0.37 pg-TEQL，平均毒性當量濃度為0.28 pg-TEQL[37]，超過了日本2007年地下水PCDDFs平均毒性當量濃度(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濃度達標。相對發達國家而言，我國雖然缺乏有說服力的PCDDFs污染數據，但根據國外經驗和有限的數據來看，PCDDFs確實在我國水體環境中存在，且部分超標。故未來幾年甚至幾十年內，開展PCDDFs的水體污染調查和控制研究非常有意義[38]。

在科學研究中，常用水體中生活的魚類體內或者是水體沉積物中PCDDFs的毒性當量濃度來反映水體的污染程度，如為評估西班牙圖里亞河流中的PCDDFs的污染狀況，學者選取長期生活在該河流的淡水魚——鱒魚和鰻魚，測試其體內PCDDFs和多氯聯苯(PCBs)的濃度(圖2)。由圖2可以看出，鱒魚和鰻魚體內PCDDs毒性當量濃度占總毒性當量濃度比例都很大，分別為56%和63%。鱒魚體內總PCDDFs濃度為1.22～1.69 pgg(濕質量)；鰻魚體內總PCDDFs濃度為1.62～4.39 pgg(濕質量)[39]；對應的毒性當量濃度分別為0.18和0.37 pg WHO-TEQg，低于歐洲社區當局設定的魚類以及漁產品肉的鮮質量最大限值(4 pg WHO-TEQg)[39]。根據BAF(生物蓄積因子)推斷出水體中PCDDFs類物質的濃度相對較低，未超出食物鏈的耐受值。

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

圖2 多氯聯苯和PCDDFs在總毒性當量 (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70年代芬蘭南部Valkjg?rvi湖被氯酚污染，后來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。結果表明，PCDDFs極易吸附于底泥土壤顆粒物中，呈現出在湖中沉積物巖心PCBs濃度高而PCDDFs濃度低的現象。反映出被氯酚污染的水體經過地下水庫，底泥土壤對PCDDFs具有相對高的凈化能力，且水體PCDDFs污染程度隨深度增加具有降低趨勢。

2.2.2 暴露情況

飲水中污染物暴露劑量的計算公式[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為飲水攝入量，mLd；EF為暴露頻次，da；ED為暴露持續時間，a；BW為體質量，kg；AT為平均暴露時間，d。

表5 近年來發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是越南戰爭期間“橙劑”集運儲存空軍基地。對這2個地區食物中PCDDFs進行風險評估，發現放養式雞的肉蛋類、淡水魚、蝸牛以及牛肉為高污染風險的食物，PCDDFs濃度為3.8～95 pg-TEQg[43]。而圈養式雞的肉蛋類、海鮮、豬肉、多葉蔬菜、水果、水稻等食物中PCDDFs的濃度相對較低(0.03～6.1 pg-TEQg)。當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)。可見當暴露于高污染的食品時，人體PCDDFs的日攝入量遠超過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 職業暴露

通常情況下，有害物質主要通過呼吸道吸入、消化道攝入、皮膚滲入3種暴露方式進入人體[45]。對于一般人群而言，PCDDFs主要通過飲食產生暴露。而諸如焚燒廠、造紙廠、鑄造廠等工人的職業暴露主要來自呼吸以及皮膚暴露。PCDDFs對人體健康的危害程度還取決于PCDDFs的性質、空氣動力學直徑、暴露濃度以及暴露時間[46]。針對職業工人高濃度長時間的暴露，有研究表明[47]，鑄造廠一線工人在一天工作時間內經由呼吸途徑攝入的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個木材廠(使用氯苯酚鈉作為防腐劑)，發現職業接觸工人血液中PCDDFs濃度分別為743、1 124和844 pg-TEQg(以脂肪質量計)，顯著高于一般人群。對作為職業暴露常見的生物標志物的頭發，采用高分辨氣相色譜-高分辨質譜儀檢測發現，不同工作環境下的工人頭發中的TCDD濃度接近0.1 pgg。而焚化廠、五氯酚生產廠等工人頭發中的PCDDFs檢測呈陽性[49]。Takata等[50]在2003年對垃圾焚燒廠和造紙廠的職工進行調查，發現其血液中的PCDDFs顯著高于對照組。同年，Kumagai等[51]也做了類似的調查，結果與Takata一致。2007年，Paola Zambon對焚化爐工人的病例對照研究表明，暴露于PCDDFs的人群肉瘤的發病風險是對照組的3.3倍[52]。Lee等[53]對中國臺灣電弧廠、再生銅冶煉廠和再生鋁冶煉廠周圍空氣和人體血液中PCDDFs水平的調查表明：工人血液中PCDDFs濃度表現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以內居民血液內的濃度(14.0 pg WHO-TEQg)高。因此針對職業暴露人群，應及時根據生產工藝摸清PCDDFs產生和存在環節，對這些環節采取工程控制、個體防護、健康監護等防控措施，盡可能降低暴露風險。

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，在誘導人體黃體化粒層細胞凋亡中存在一定的劑量-效應關系。最新的一項研究表明：使黃體化粒層細胞分泌的雌二醇-17β(E2)分別暴露于3.1 nmolL、3.1 pmolL和3.1 fmolL劑量的TCDD，發現體外培養皿中E2的積累量與暴露時間在統計學上呈顯著的關系，與暴露劑量并無太大關系。E2濃度的減少是由于在雌性激素生物合成過程中，CYP11A1和CYP19A1這2種酶的mRNA表達受阻。目前基于細胞系和嚙齒動物模型的代謝物組學評估TCDD毒性研究還比較少[67]。大多研究結果只強調氨基酸和脂質(脂肪酸和膽汁酸)代謝的變化情況。而事實上，在醫療保健意識日益提升的環境下，PCDDFs長期暴露毒性臨床代謝物組學研究已經是人類最關切的問題。目前，四級桿-飛行時間串聯質譜(quadrupole time-of-flight mass spectrometry)技術支持代謝物非目標性篩選，從而可用于尋找新的生物標志物。該技術用極端表現型作為參考標準，采用生物學知識和統計學工具對初始數據進行處理而獲得可表征TCDD中毒的生物標志物組。代謝物組學較基因組學和蛋白質組學還相對不成熟，但是作為一種可尋找新生物標志物、發現新代謝途徑的研究組學方法，在臨床醫學上更具研究價值。

5 結語

目前我國經濟高速發展，城市垃圾的數量種類與城市規模同步增長。環境中PCDDFs的污染問題日益嚴重，而我國又缺乏比較完善的PCDDFs污染防治體系和長期監管機制。從國家監管層面，我國應該學習日本以及歐盟國家逐步建立PCDDFs不同排放源于不同環境介質的排放限值以及管理政策；參考《二英和呋喃排放識別和量化標準工具包》并結合我國于2010年10月19日發布的《關于加強二英污染防治的指導意見》，在京津冀、長三角、珠三角等重點區域逐步開展PCDDFs排放總量控制試點工作；篩選主要類別源，細化對應的子類別活動過程，通過調查問卷獲得更為準確詳細的信息，從而逐步更新完善我國主要行業涉及鋼鐵、再生有色金屬和廢物焚燒等多個領域的PCDDFs排放清單；從源頭進行治理。從公司企業層面，特別針對職業暴露，應大力提高企業監管力度，從根本上弄清楚PCDDFs的排放環節，開發簡易、快速、低廉的分析方法和暴露監測技術，開展小型零散企業關停計劃。從民眾層面，應該提高自我保護意識，調整飲食結構，并提高知情權意識。

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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

國家自然科學基金項目(21277132)； 國家環境保護公益性行業科研專項(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，主要從事大氣環境化學和環境標準研究工作，chenjh@craes.org.com

X512

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

10.3969j.issn.1674-991X.2016.03.035