黃亮，張經(jīng)，吳瑩

1. 九江學(xué)院化學(xué)與環(huán)境工程學(xué)院 江西省生態(tài)化工工程技術(shù)中心，九江 332005 2. 華東師范大學(xué) 資源與環(huán)境科學(xué)學(xué)院，上海 200062 3. 華東師范大學(xué) 河口海岸國(guó)家重點(diǎn)實(shí)驗(yàn)室，上海 200062

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長(zhǎng)江流域表層沉積物中多環(huán)芳烴分布特征及來(lái)源解析

黃亮1,2,*，張經(jīng)3，吳瑩3

1. 九江學(xué)院化學(xué)與環(huán)境工程學(xué)院 江西省生態(tài)化工工程技術(shù)中心，九江 332005 2. 華東師范大學(xué) 資源與環(huán)境科學(xué)學(xué)院，上海 200062 3. 華東師范大學(xué) 河口海岸國(guó)家重點(diǎn)實(shí)驗(yàn)室，上海 200062

長(zhǎng)江流域沉積物多環(huán)芳烴分析表明，多環(huán)芳烴濃度總和(不包括苝)約為10.31～1 239 ng·g-1，與國(guó)內(nèi)外其他區(qū)域相比，整體處于一個(gè)低至中等程度的污染水平。長(zhǎng)江自上游至下游，沉積物中多環(huán)芳烴含量呈上升趨勢(shì)，與沿途各省多環(huán)芳烴的排放狀況相吻合。揚(yáng)州(YZ)和湘江(XJ)采樣點(diǎn)沉積物中多環(huán)芳烴含量最高，污染最嚴(yán)重。根據(jù)多環(huán)芳烴的比值特征，長(zhǎng)江流域沉積物中多環(huán)芳烴主要受以煤、木材、油類的燃燒影響較大，還有部分來(lái)自油類的泄漏，極少量來(lái)自自然成因。

多環(huán)芳烴；長(zhǎng)江；沉積物；分布；源解析

Received 26 November 2015 accepted 9 January 2016

多環(huán)芳烴(polycyclic aromatic hydrocarbons, PAHs)是指2個(gè)或2個(gè)以上苯環(huán)以稠環(huán)形式相連的化合物，是一類廣泛存在于環(huán)境中的持久污染物[1]。它主要來(lái)源于各種化石燃料、生物質(zhì)燃料的不完全燃燒、天然火災(zāi)、火山爆發(fā)、石油泄漏、植物及微生物的生物合成，以及沉積環(huán)境中的成巖作用過(guò)程中形成[1-4]。多環(huán)芳烴是一類強(qiáng)致癌劑和誘變劑，因而其在環(huán)境介質(zhì)中的分布、遷移及生態(tài)風(fēng)險(xiǎn)已被廣泛研究[5-8]。

長(zhǎng)江作為世界最長(zhǎng)的河流之一，伴隨著經(jīng)濟(jì)的深入發(fā)展，人文活動(dòng)對(duì)長(zhǎng)江的改造及影響不斷增加，導(dǎo)致水污染問(wèn)題越來(lái)越突出，尤其是有機(jī)物污染呈惡化趨勢(shì)，比如多環(huán)芳烴。據(jù)估算，長(zhǎng)江流經(jīng)的沿途各省排放的多環(huán)芳烴通量約為9.3×103t·y-1，占到全國(guó)總量的三分之一[9-10]。因此在長(zhǎng)江某些江段的水體、顆粒物及沉積物中均檢測(cè)出多環(huán)芳烴[11-13]，但是在整個(gè)長(zhǎng)江流域沉積物中多環(huán)芳烴的分布還未見(jiàn)報(bào)道。故此，本文選擇長(zhǎng)江流域?yàn)檠芯繀^(qū)域，探討多環(huán)芳烴在該區(qū)域沉積物中的分布特征，并結(jié)合多環(huán)芳烴的分子標(biāo)志物對(duì)其分布及污染來(lái)源進(jìn)行初步分析。

1 材料與方法 (Materials and methods)

1.1 樣品采集與前處理

長(zhǎng)江流域表層沉積物樣品采自2009年9—10月長(zhǎng)江流域考察中于河流中心處(遠(yuǎn)離人類活動(dòng)密集處，盡量減小人為影響)用抓斗采集表層沉積物，采樣站位覆蓋了長(zhǎng)江干流(9個(gè))和主要支流(11個(gè))(圖1)。采集1～2 kg沉積物樣品后立即放入冰箱在-20 ℃下冷凍保存?；氐綄?shí)驗(yàn)室后，放入烘箱中60 ℃下干燥。隨后將樣品中明顯的植物碎屑挑出，樣品研磨過(guò)100目篩，待進(jìn)一步分析處理。

稱取20 g左右沉積物樣品，加入氘代三聯(lián)苯作回收率指示物，用二氯甲烷和甲醇(V:V，2:1)索式抽提48 h，燒瓶中事先加入活化銅片以去除樣品中的硫。提取液經(jīng)濃縮、轉(zhuǎn)換溶劑，用去活化的硅膠層析柱(SiO2-10% H2O)分離凈化，加20 mL正己烷洗脫。洗脫液旋轉(zhuǎn)濃縮近干后，加入2 mL正戊烷后，再加入等體積N, N-二甲基甲酰胺(DMF)-5%H2O萃取，移取DMF層，共萃取2次；再在DMF中加入4 mL H2O后，用4 mL正己烷萃取2次收集PAHs，多環(huán)芳烴經(jīng)濃縮后進(jìn)行GC- MS分析。詳細(xì)步驟參見(jiàn)Mandalakis等的方法[14]進(jìn)行。

圖1 長(zhǎng)江流域采樣站位示意圖Fig. 1 The map of sampling stations in the Yangtze River from China

1.2 多環(huán)芳烴測(cè)定

定量測(cè)試由Aglient 6890氣相色譜配5973N質(zhì)譜檢測(cè)器完成。進(jìn)樣口溫度為290 ℃，無(wú)分流進(jìn)樣，進(jìn)樣量為1 μL，在DB-5MS毛細(xì)管柱(30 m×0.25 mm×0.25 μm)中分離。升溫程序?yàn)槌跏紲囟葹?0 ℃，保持2 min，以6 ℃·min-1升到290 ℃，保持10 min。通過(guò)多環(huán)芳烴混合標(biāo)準(zhǔn)的保留時(shí)間鑒定譜峰。

以12個(gè)樣品為一個(gè)批次，每批次中加入質(zhì)量控制樣品，包括空白樣品和空白加標(biāo)實(shí)驗(yàn)，所有空白樣品均未檢測(cè)到PAHs，并在所有樣品中加入氘代三聯(lián)苯作為回收率內(nèi)標(biāo)。加標(biāo)空白除萘、苊、二氫苊及芴的回收率小于60%，其他PAHs的回收率在80%～110%之間，平行樣的相對(duì)偏差不超過(guò)10%，因此在本論文討論中的PAHs只包括菲(Phe)、蒽(An)、1-甲基菲(Mphe)、熒蒽(Fl)、芘(Py)、苯并[a]蒽(BaA)、屈(Chry)、苯并[b]熒蒽(BbF)、苯并[k]熒蒽(BkF)、苯并[e]芘(BeP)、苯并[a]芘(BaP)、苝(Pery)、茚并[1,2,3-cd]芘(Ip)、二苯并[a,h]蒽(DhA)、苯并[ghi]苝(BghiP)，不包括低分子量的萘、苊、二氫苊及芴。

2 結(jié)果與討論(Results and discussion)

2.1 長(zhǎng)江流域沉積物中PAHs含量與分布

圖2和表1顯示了多環(huán)芳烴(TPAH，不包括Pery在內(nèi)的其余多環(huán)芳烴總和)在整個(gè)研究區(qū)域的變化狀況，其濃度范圍在10.31～1 239 ng·g-1之間，平均為(178.0±272.2) ng·g-1，這與許士奮等[15]的在長(zhǎng)江南京段的研究(213.8～550.3 ng·g-1)接近，低于生物毒性影響實(shí)驗(yàn)獲得的生物影響閥值低值(ERL=4 022 ng·g-1)[16]。其中，支流沉積物PAHs含量最高在XJ站，為512.1 ng·g-1；最低在GJ站，為10.31 ng·g-1。而干流含量最高在YZ站，為1 239 ng·g-1；最低在XLJ，為16.94 ng·g-1。從整體上看，長(zhǎng)江自上游至下游，沉積物中多環(huán)芳烴含量呈上升趨勢(shì)，與流域內(nèi)各省多環(huán)芳烴的排放狀況相吻合。如圖3所示，盡管在上游的四川省的多環(huán)芳烴排放量最高，但是其地域廣闊，致使其排放密度下降，對(duì)應(yīng)的沉積物中PAHs也較低；而位于下游的各省市多環(huán)芳烴的排放量變化趨勢(shì)并不明顯，但是其面積相對(duì)狹小，以致排放密度呈上升趨勢(shì)，尤其是上海，排放密度最高[17]。相對(duì)發(fā)達(dá)的工業(yè)、交通，城市和工業(yè)區(qū)及其周邊區(qū)域的多環(huán)芳烴污染水平高于山區(qū)、遠(yuǎn)郊區(qū)和農(nóng)業(yè)用地[18]。比如，XJ站于污染嚴(yán)重的湘江[19]，YZ站位于經(jīng)濟(jì)發(fā)達(dá)的揚(yáng)州，工業(yè)活動(dòng)劇烈，因此這2個(gè)站位的PAHs含量較高。AQ站附近有大型的煉油廠，故PAHs含量亦相對(duì)較高(為460.7 ng·g-1)。GJ站位于經(jīng)濟(jì)欠發(fā)達(dá)的地區(qū)江西省，PAHs含量較低。位于長(zhǎng)江口的XLJ站，附近有裝卸沙石的碼頭，因此該站位的表層沉積物可能是來(lái)自運(yùn)砂船只的泄漏，因而TPAH較低(29.07 ng·g-1)，在此檢出高含量的苝(占總量的84.1%)，由于高含量的苝主要源于有機(jī)質(zhì)成巖作用[20]，也證明該站的沉積物可能主要來(lái)自運(yùn)砂船只的泄漏。

圖2 長(zhǎng)江流域支流及干流沉積物中多環(huán)芳烴含量分布Fig. 2 Distribution of PAHs contents in sediments from main steam and tributary of the Yangtze River

圖3 長(zhǎng)江流域各省PAHs的排放量及排放密度，數(shù)據(jù)引自[17]Fig. 3 PAHs emissions and density of emission in the provinces along the Yangtze River[17]

站位SamplingstationPheAnFlPyBaAChryBbFBkFBaPIPDhABghiPMpheBePPeryTPAHYLJ8.681.516.544.082.962.793.421.592.812.45n.d.2.812.982.572.1245.18HSH15.512.7122.0415.046.575.905.572.474.643.57n.d.4.592.414.502.5698.82NLJ5.560.243.032.030.681.893.161.031.830.71n.d.0.742.462.200.4426.53DDH11.412.5220.5512.339.959.409.384.977.576.210.464.973.067.132.71111.61MJ16.082.3913.732.605.075.905.092.394.313.570.084.222.605.192.2976.23NX20.572.5818.9311.9910.3314.582.830.9510.6313.956.8810.9520.3813.956.11163.72CSH12.131.817.935.333.604.565.752.303.573.720.134.383.104.602.9066.25FJ31.353.2018.1913.429.1818.2218.645.679.6910.651.4212.255.0718.014.42180.85JLJ12.591.536.014.342.764.084.351.642.672.750.003.823.003.944.6656.76JJ8.071.235.793.502.883.481.870.632.832.830.523.197.253.741.7249.63WJ31.123.2731.5521.4014.4418.6223.639.2314.8619.7510.4315.2115.6416.896.43249.04WZ16.642.459.025.834.696.028.333.184.935.59n.d.6.2913.686.6189.5897.94XJ85.5614.3961.435.6538.0050.6254.6713.742.042.3658.253.03101.622.0416.90512.11HH7.660.391.391.030.250.57n.d.n.d.0.260.000.000.343.440.763.4216.94HS5.550.443.252.270.630.980.810.360.490.43n.d.0.453.331.224.4720.86GJ4.590.200.690.440.300.18n.d.n.d.n.d.n.d.n.d.n.d.1.57n.d.3.8610.31AQ56.138.2245.9132.5323.7135.4846.9515.2226.3729.6114.1428.3048.2235.92100.44460.69WH11.322.397.655.204.234.487.012.924.644.600.005.8111.265.2917.3380.43YZ49.229.09136.89120.8999.66103.39173.4331.981.9550.22390.7918.5842.981.951.951238.85XLJ8.590.532.501.680.571.351.840.430.000.920.000.895.061.33136.3629.06

注：TPAH指不包含Pery的其余多環(huán)芳烴之和。

Note: TPAH stands for the total contents of all PAHs without Pery.

圖4 長(zhǎng)江支流及干流沉積物中多環(huán)芳烴的環(huán)數(shù)分布Fig. 4 Distribution of rings of PAHs in sediments from main steam and tributary of the Yangtze River

從多環(huán)芳烴組成上看(如圖4所示)，位于上游支流各站(包括YLJ、HSH、NLJ、DDH、CSH、FJ、JLJ和WJ)的PAHs的組成非常相似，主要以下列順序排列：四環(huán)>三環(huán)>五環(huán)>六環(huán)>苝。位于主流的各站位來(lái)說(shuō)，NX、AQ和YZ三個(gè)站位的環(huán)數(shù)組成相似，以四環(huán)和五環(huán)為主，三環(huán)和六環(huán)較少；而JJ、WZ和HH等站位卻主要以三環(huán)、四環(huán)為主，其次為五環(huán)和六環(huán)。另外在WZ、XLJ和GJ這3個(gè)站位還含有高含量的苝。

圖5 長(zhǎng)江支流及干流沉積物中Fl/(Fl+Py)與(a) An/(An+Phe)；(b) BaA/(BaA+Chry)；(c)IP/(IP+BghiP)；(d) Mphe/Phe散點(diǎn)圖Fig. 5 Plot of Fl/(Fl+Py) v.s. (a) An/(An+Phe); (b) BaA/(BaA+Chry); (c)IP/(IP+BghiP); (d) Mphe/Phe in sediments from main steam and tributary of the Yangtze River

2.2 多環(huán)芳烴的來(lái)源

不同來(lái)源的PAHs其組成并不一致，同時(shí)PAHs的同分異構(gòu)體具有類似的物理化學(xué)性質(zhì)，它們進(jìn)入環(huán)境后的分配和稀釋行為接近，因此常使用多環(huán)芳烴某些單體的比值來(lái)判斷其來(lái)源，比如：An/(Phe+An)、Fl/(Fl+Py)、BaA/(BaA+Chry)和IP/(IP+BghiP)[21-24]。甲基多環(huán)芳烴主要來(lái)自低溫燃燒及石油泄漏[25]，因而有研究認(rèn)為Mphe/Phe小于1及大于1分別代表燃燒源和石油源[24]。如圖5所示，研究區(qū)域的大多數(shù)站位的Mphe/Phe比值都小于1，在0.34～0.99之間，說(shuō)明這些站位的PAHs主要以熱成因?yàn)橹?；NLJ、FJ、JLJ、XJ這些站位的比值都大于1，說(shuō)明它們的PAHs可能混有油來(lái)源。所有站位的Fl/(Fl+Py)均大于0.5和IP/(IP+BghiP)大于0.2，說(shuō)明該區(qū)域的PAHs主要來(lái)自木材、煤等及油類的燃燒[24]。少量站位，例如HH、FJ、XLJ、NLJ的BaA/(BaA+Chry)在0.2～0.35之間，顯示混合源的特征[24]。綜上所述，研究區(qū)域表層沉積物的PAHs主要來(lái)以源于煤、木材、油類的燃燒為主，還有部分來(lái)自油類的泄漏，極少量來(lái)自自然成因。這也符合Xu等[17]的研究，他們證實(shí)中國(guó)的多環(huán)芳烴主要來(lái)自生物質(zhì)燃料、煤的燃燒，分別占到總量的60%和20%

表2 世界其他地區(qū)河流、湖泊及近岸沉積物中多環(huán)芳烴含量比較

2.3 與國(guó)內(nèi)外其他地區(qū)沉積物中多環(huán)芳烴含量的比較

長(zhǎng)江流域沉積物與國(guó)內(nèi)外其他湖泊、河流、近岸沉積物中多環(huán)芳烴的比較見(jiàn)表2。本研究區(qū)域的多環(huán)芳烴與廈門(mén)西港(195～675 ng·g-1)[26]、閩江口(174～817 ng·g-1)[27]、安徽巢湖(116.0～2 832 ng·g-1)[28]等地處于一個(gè)水平，要高于淮河(淮南-蚌埠段)(5～78 ng·g-1)[29]、江蘇云龍湖(5～19 ng·g-1)[30]和臺(tái)州灣海域(85～168 ng·g-1)[29]，但要遠(yuǎn)遠(yuǎn)低于一些高度工業(yè)化和城市化的河口和海岸帶地區(qū)，例如歐洲波羅的海(3～30 100 ng·g-1)[31]、美國(guó)紐約港(1 900～70 000 ng·g-1)[32]、新加波海岸(13 630～ 84 920 ng·g-1)[33]等。綜上所述長(zhǎng)江流域的PAHs污染程度的國(guó)際對(duì)比處于一個(gè)低至中等程度的污染。

綜上可知：

(1)長(zhǎng)江流域沉積物中多環(huán)芳烴處于一個(gè)低至中等程度的污染水平，TPAH在10.31～1 239 ng·g-1之間，且自上游至下游，其含量呈上升趨勢(shì)，這與流域內(nèi)各省多環(huán)芳烴的排放狀況、具體站位的環(huán)境狀況有關(guān)。

(2)通過(guò)多環(huán)芳烴組成特征判斷，研究區(qū)域沉積物中多環(huán)芳烴的來(lái)源主要來(lái)以源于煤、木材、油類的燃燒為主，還有部分來(lái)自油類的泄漏，極少量來(lái)自自然成因。

(3)與國(guó)內(nèi)外其他河流、湖泊及海灣沉積物多環(huán)芳烴含量相比，研究區(qū)域沉積物中多環(huán)芳烴處于低至中等污染水平。

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Distribution and Sources of Polycyclic Aromatic Hydrocarbons in Surface Sediments from the Yangtze River

Huang Liang1,2,*, Zhang Jing3, Wu Ying3

1. Jiangxi Province Engineering Research Center of Ecological Chemical Industry, College of Chemistry and Environmental Engineering, Jiujiang University, Jiujiang 332005, China 2. School of Ecological and Environmental Sciences, East China Normal University, Shanghai 200062, China 3. State Key Laboratory of Estuarine and Coastal Research, East China Normal University, Shanghai 200062, China

Polycyclic aromatic hydrocarbons (PAHs) were determined in surface sediments from the Yangtze River basin. Total PAH concentrations (TPAH, perylene not included) varied from 10.31 ng·g-1to 1 239 ng·g-1, indicating a moderate to low level when compared with samples from the other regions worldwide. Concentrations of TPAH in sediments increased from the upper to the lower reaches, suggesting its emission along the Yangtze River. PAHs contents in sediments from the two highly polluted stations of YZ (Yangzhou) and XJ (Xiangjiang) were highest. According to the PAH ratio index calculations, these PAH molecules were primarily derived from petroleum combustion, biomass combustion and coal burning, followed by oil spillage, and the contribution of the direct input from nature origin was quite minor.

PAHs; Yangtze River; sediment; distribution; source

10.7524/AJE.1673-5897.20151126006

國(guó)家自然科學(xué)基金(41076052)

黃亮(1978-), 男, 江西九江人, 講師, 在讀博士, 研究方向?yàn)榄h(huán)境地球化學(xué)，Email: huangliang2002@126.com

2015-11-26 錄用日期：2016-01-09

1673-5897(2016)2-568-07

X171.5

A

黃亮, 張經(jīng), 吳瑩. 長(zhǎng)江流域表層沉積物中多環(huán)芳烴分布特征及來(lái)源解析[J]. 生態(tài)毒理學(xué)報(bào)，2016, 11(2): 566-572

Huang L, Zhang J, Wu Y. Distribution and sources of polycyclic aromatic hydrocarbons in surface sediments from the Yangtze River [J]. Asian Journal of Ecotoxicology, 2016, 11(2): 566-572 (in Chinese)