齊 麗,任 玥,李 楠,鄭 森,趙 虎,范 爽,周志廣,許鵬軍,劉愛民,張 烴,黃業(yè)茹 (國家環(huán)境分析測試中心,國家環(huán)境保護二污染控制重點實驗室,北京 100029)

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齊 麗*,任 玥,李 楠,鄭 森,趙 虎,范 爽,周志廣,許鵬軍,劉愛民,張 烴,黃業(yè)茹 (國家環(huán)境分析測試中心,國家環(huán)境保護二污染控制重點實驗室,北京 100029)

摘要：2013年4月至2014年1月對北京市某生活垃圾焚燒廠周邊4km范圍內(nèi)5個采樣點環(huán)境空氣中二含量、組成特征及季節(jié)變化特征進行了分析.結(jié)果表明該垃圾焚燒廠周邊環(huán)境空氣中PCDD/Fs質(zhì)量濃度的變化范圍為8.3～115pg/m3,毒性當量(TEQ)變化范圍為0.11～1.9pg I-TEQ/m3,其中秋季1個采樣點和冬季全部采樣點超出日本環(huán)境空氣質(zhì)量標準限值(0.6pg I-TEQ/m3).1,2,3,4,6,7,8-HpCDF和OCDF均是四季空氣中PCDD/Fs質(zhì)量濃度的主要貢獻單體,而2,3,4,7,8-PeCDF是總TEQ貢獻最大的單體.空間分布特征表現(xiàn)為近源點位(～400m)濃度水平較高而其他點位(>1000m)濃度水平與距污染源距離遠近沒有顯著相關(guān)性;季節(jié)變化特征表現(xiàn)為冬季值顯著高于其他季節(jié),分析可能與冬季采暖及大氣擴散條件差導致的大氣整體污染較重有關(guān).樣品中二同族體及異構(gòu)體分布指紋譜圖與焚燒設(shè)施排放煙氣存在差別,主成分分析(PCA)源解析結(jié)論與指紋譜圖特征分析結(jié)論一致,體現(xiàn)為多種污染源共同作用的影響.二呼吸暴露劑量估算結(jié)果表明該區(qū)域人群呼吸暴露風險總體處于較為安全的水平(0.034～0.161pg I-TEQ/(kg?d)),但仍需關(guān)注大氣重污染天氣發(fā)生時的呼吸暴露風險.

關(guān)鍵詞：生活垃圾焚燒；環(huán)境空氣；二；季節(jié)變化；主成分分析；呼吸暴露

* 責任作者, 高級工程師, ql_cneac@163.com

多介質(zhì)歸趨模型模擬研究表明:大氣傳輸和從空氣相—土壤(水)相干濕沉降是二類在環(huán)境中的主要遷移途徑[1-3],即排放至大氣中的二類通過和各個環(huán)境介質(zhì)間的相間遷移,在全球范圍內(nèi)分布并進入食物鏈,危害生態(tài)系統(tǒng)和人體健康[4-6].大氣中的二主要來自金屬冶煉、廢棄物焚燒等人類生產(chǎn)活動[7-11],其中生活垃圾焚燒排放是城市地區(qū)大氣二來源的最重要途徑之一.自O(shè)lie等[12]首次發(fā)現(xiàn)城市生活垃圾焚燒的煙氣和飛灰中存在二以來,許多國家和地區(qū)對城市生活垃圾焚燒廠二排放的環(huán)境影響進行了深入的科學研究[7,13-18].研究表明大部分生活垃圾焚燒廠周圍大氣中的二分布與生活垃圾焚燒廠廢氣二的排放濃度成正比[19-20].如Oh等[21]對韓國某生活垃圾焚燒廠1999～2006年的跟蹤監(jiān)測表明周邊大氣中二濃度水平在采用煙氣凈化裝置前后明顯降低,推斷此生活垃圾焚燒廠周圍大氣主要受該垃圾焚燒廠的影響.我國對垃圾焚燒廠周邊大氣中二含量水平的研究起步相對較晚,目前僅有少量研究報道.如徐夢俠等[22]對杭州市某垃圾焚燒廠周邊環(huán)境介質(zhì)中二的分布規(guī)律進行研究,發(fā)現(xiàn)規(guī)范運行的垃圾焚燒排放對周邊環(huán)境空氣二濃度的影響有限.除污染源外,不同的氣候也是影響大氣二濃度水平及其行為特征的重要因素[23].由于季節(jié)的交替伴隨著主導風向、溫度、干濕沉降等因素的改變,研究大氣中二的濃度與季節(jié)變化的關(guān)系,一方面可以揭示其來源問題[24],另一方面也反映二在大氣中的某種虧損過程或去向問題.

北京作為國家經(jīng)濟金融的決策中心和管理中心,隨著經(jīng)濟的高速持續(xù)增長,城市規(guī)模不斷擴大和人民生活水平的迅速提高,城市生活垃圾的產(chǎn)生量急劇增加.除衛(wèi)生填埋外,垃圾焚燒已逐漸發(fā)展成為一種重要的垃圾處理方式.考慮到垃圾焚燒產(chǎn)生的二次污染物如二等可能對周邊環(huán)境及居民的健康造成負面影響,此處理方式一度受到公眾的強烈反對.因此,本研究選取北京市某大型垃圾焚燒發(fā)電廠周邊環(huán)境作為研究區(qū)域于2013年至2014年不同季節(jié)開展共計四次監(jiān)測,綜合評價其周邊環(huán)境空氣中二類污染物的含量、組成及分布規(guī)律,以及周邊人群經(jīng)呼吸途徑的二類暴露水平,探討該設(shè)施二排放對周邊地區(qū)可能造成的環(huán)境影響及健康風險,為環(huán)境管理部門有效開展垃圾焚燒處理提供技術(shù)支持.

1　材料與方法

1.1 研究區(qū)域及樣品采集

生活垃圾焚燒發(fā)電廠設(shè)計垃圾處理規(guī)模為1600t/d,安裝有800t/d×2爐排爐以及煙氣處理系統(tǒng)(脫酸塔+活性炭噴射+布袋除塵器).以廠區(qū)(圖1中梯形區(qū)域所示)為中心,采用同心圓布點法力求覆蓋各方位的原則,并根據(jù)周邊居民分布情況,在周邊4km范圍內(nèi)不同方位選取4個居民聚集區(qū)(S1、S3～S5)和1個廠界區(qū)(S2)進行環(huán)境空氣二監(jiān)測,各采樣點距污染源的距離分別約為1.8、0.4、1.4、2.7和3.6km.采樣儀器均設(shè)置于開闊院落地面上,周邊15m內(nèi)無較大障礙物,分別位于排放源的東北、東南、西北、西南方向及廠區(qū)邊界.各采樣點位置如圖1所示.

圖1　環(huán)境空氣采樣布點示意(梯形區(qū)域為廠區(qū))Fig.1　Ambient air sampling sites around the MSWI

1.2 樣品前處理、分析及質(zhì)控

空白加標的檢出結(jié)果均低于檢出限,所有樣品在分析過程添加的PCDD/Fs標記物的回收率均處于35%～115%之間,符合HJ77.2-2008的質(zhì)量控制要求.在數(shù)據(jù)處理過程中,低于檢出限的目標污染物質(zhì)量濃度以0計算.

2　結(jié)果與討論

5個采樣點四期監(jiān)測得到的大氣PCDD/Fs濃度如表1所示,其4～8氯代PCDD/Fs同族體總濃度范圍為8.3～115pg/m3,各采樣點季平均值為24.7～52.7pg/m3,17種2,3,7,8位取代的PCDD/Fs毒性當量濃度范圍為0.11～1.9pg I-TEQ/m3,季平均值為0.40～0.77pg I-TEQ/m3.除冬季監(jiān)測數(shù)據(jù)外,其余各采樣點監(jiān)測結(jié)果基本與之前報道的城市環(huán)境空氣PCDD/Fs含量水平相當:北京市區(qū)(2006年0.268pg I-TEQ/m3;2011- 2012年0.251pg I-TEQ/m3)[26-27]、廣州市區(qū)(0.364pg I-TEQ/m3)[28]及上海市區(qū)(0.268pg I-TEQ/m3)[29], 除S2采樣點秋季監(jiān)測結(jié)果達到被Fielder等[30]定義為受點源污染的標準范圍(0.350～1.60pg I-TEQ/m3)外,其余點位均在Lohmann等[23]提出的城市環(huán)境空氣中二標準濃度范圍0.100～0.400pg I-TEQ/m3之內(nèi).與日本規(guī)定的空氣PCDD/Fs的年均值標準(0.6pg I-TEQ/m3)[31]相比較,S2采樣點秋季監(jiān)測結(jié)果略高于此排放限值,而冬季各采樣點均超出該標準限值83%～ 217%.

從分布情況可知,近源采樣點S2(<1000m)在各采樣期二濃度水平較高,表明廠界區(qū)域可能受到此垃圾焚燒設(shè)施的影響相對高于其他采樣點.風向是影響排放源二擴散的最基本因素.本研究中,由于采樣時段涵蓋一年四季,北京冬季主導風向為西北方向;夏季主導風向為東南方向;春秋季多為西北風,各期采樣期間氣象條件:風力小于三級,風向為無持續(xù)風向天氣,天氣以晴或晴間多云為主(www.bjmb.gov.cn).因此,非近源采樣點在主導風向上、下風向的濃度差異不明顯.張振全等[32]對華南某工業(yè)區(qū)垃圾焚燒設(shè)施周邊環(huán)境空氣中PCDD/Fs含量研究發(fā)現(xiàn)點源煙氣的影響存在“燈下黑”的特點,即下風向最大落地濃度點位置(距離源一般1km左右)附近含量較高.本研究中S1采樣點夏季位于主導風向的下風向且與污染源距離接近最大落地濃度點位置,但其在夏季濃度略低于其他采樣點,表明除近源區(qū)域外該垃圾焚燒發(fā)電廠排放對周邊的影響不顯著.

表1　各采樣點大氣中PCDD/Fs總質(zhì)量濃度(pg/m3)及毒性當量濃度(pg I-TEQ/m3)Table 1　Mass and TEQ concentrations of PCDD/Fs in the samples at each sampling site

從表1可見,各采樣點最高值均出現(xiàn)在冬季,最低值均出現(xiàn)在春季,其次是夏季和冬季.各點位不同季節(jié)PCDD/Fs平均濃度高低順序為冬季(85.2pg/m3)>秋季(32.4pg/m3)>夏季(18.6pg/m3)>春季(12.6pg/m3);二毒性當量濃度的季節(jié)變化也遵循相同的規(guī)律,即冬季(1.4pg I-TEQ/m3)>秋季(0.41pg I-TEQ/m3)>夏季(0.20pg I-TEQ/m3)>春季(0.16pg I-TEQ/m3).這與天津、香港等地城市冬季大氣二濃度水平最高相似[33-34],而與廣州地區(qū)春季大氣二明顯高于秋、冬、夏三季不同[35].

2.3 PCDD/Fs毒性異構(gòu)體分布特征

PCDD/Fs的17種毒性異構(gòu)體分布特征是重要的指紋特性之一,常用作最基本的溯源分析,可以采用單體對總質(zhì)量濃度的貢獻率和單體對總毒性當量濃度的貢獻率進行表述.

2.4 PCDD/Fs同族體分布特征

2.5 多變量來源分析

為進一步了解焚燒設(shè)施周邊環(huán)境空氣中PCDD/Fs與垃圾焚燒源的關(guān)系,應(yīng)用主成分分析方法(PCA)對典型排放源煙氣和空氣樣品之間PCDD/Fs的17種2,3,7,8-位取代二異構(gòu)體特征相似度進行了分析.調(diào)研發(fā)現(xiàn)周邊除垃圾焚燒設(shè)施外重要的熱排放源還有無組織燃煤鍋爐、殯葬焚燒廠和交通源等.為了分辨多種源對環(huán)境空氣的影響,對采集樣品和典型城市大氣二排放源17種異構(gòu)體相對豐度進行主成分分析(PCA),主要包括生活垃圾焚燒廠煙氣、燃煤鍋爐煙氣、殯儀館火化機煙氣、汽油機動車尾氣和柴油機動車尾氣等(注:由于缺乏本地數(shù)據(jù),燃煤鍋爐及汽(柴)油車參考U. S. EPA二排放源數(shù)據(jù)庫[39],殯儀館及生活垃圾焚燒煙氣二數(shù)據(jù)為排放源實測數(shù)據(jù)).

圖6顯示了以不同季節(jié)采樣點樣品為變量的主成分分析結(jié)果,提取2個主成分因子,因子1和因子2分別解釋44.2%和22.4%的總方差.二異構(gòu)體譜圖類似的相距較近,反之較遠.從圖6可知,5個采樣點四季的結(jié)果分布集中,說明研究區(qū)域大氣中的二異構(gòu)體分布特征相似,細微差別可能由各采樣點不同季節(jié)周邊具體活動程度及微氣象條件差異所致,這也從各采樣點結(jié)果在每個季節(jié)更為靠近得到佐證.環(huán)境空氣中的二來源較廣,除焚燒排放源外,所有采樣點特征譜圖與燃煤鍋爐和汽油機動車相距更近,表明研究區(qū)域可能同時受到這3種源共同作用且受到燃煤鍋爐和交通源的影響更大.另外,冬季西北主導風向的下風向(S4和S5)采集的空氣樣品中二毒性當量與上風向(S1和S3)相當,進一步說明焚燒源煙氣排放通過擴散遷移對環(huán)境空氣中的二貢獻率較小;較高濃度的二來源較為復雜,并非受該生活垃圾焚燒設(shè)施煙氣排放的主導影響.PCA的分析結(jié)果與上文提及的各采樣點異構(gòu)體和同族體分布特征指紋譜圖與生活垃圾焚燒煙氣二譜圖存在一定差異的分析結(jié)果一致.

圖2　各點位17種2,3,7,8-位取代PCDD/Fs單體占總質(zhì)量濃度的相對豐度Fig.2　Relative abundance of 2,3,7,8-substituted PCDD/Fs congeners in the samples at each sampling site

圖3　各點位17種2,3,7,8-位取代PCDD/Fs單體占總毒性當量濃度的相對豐度Fig.3　Relative I-TEQ abundance of 2,3,7,8-substituted PCDD/Fs congeners in the samples at each sampling site

圖4　焚燒廠煙氣2,3,7,8-PCDD/Fs異構(gòu)體質(zhì)量濃度、毒性當量及四～八氯代同族體質(zhì)量濃度相對豐度Fig.4　Relative contributions of individual congener and homologue to the total mass and TEQ of PCDD/Fs in flue gas

圖5　各點位PCDD/Fs同族體分布特征譜圖Fig.5　PCDD/Fs homologue profiles of the samples at each sampling site

式中:IPad/ch指經(jīng)呼吸二暴露量(pg I-TEQ/ (kg?d));Cair為空氣中PCDD/Fs濃度水平(pg I-TEQ/m3),取每個采樣點四季采樣監(jiān)測的濃度均值;Vrad/ch指吸入速率(m3/d),取《中國人群環(huán)境暴露行為模式研究報告(成人卷)》和《中國人群暴露參數(shù)手冊(成人卷)》中推薦的吸入速率值0.25m3/(kg?d),兒童取值0.51m3/(kg?d);?r指肺中停留系數(shù),成人和兒童取均值0.75,Wad/ch指人體體重,成人取我國居民成人平均體重60.6kg, 兒童取15kg;(Nso,ad/ch+ Nwo,ad/ch+ Nsl,ad/ch+ Nwi,ad/ch+ Nsi,ad/ch)指肺中停留時間,取美國EPA推薦的估算值,成人0.457,兒童0.616.

圖6　排放源與環(huán)境空氣中PCDD/Fs相關(guān)性分析(采樣點名稱指代季節(jié)+點位)Fig.6　Correlation of PCDD/Fs profiles in emission sources and air samples

3　結(jié)論

3.1 生活垃圾焚燒廠周邊大氣中PCDD/Fs質(zhì)量濃度和毒性當量濃度的變化范圍分別為8.3～ 115pg/m3和0.11～1.9pg I-TEQ/m3,其中1,2,3,4,6, 7,8-HpCDF和OCDF是四季環(huán)境空氣中PCDD/Fs質(zhì)量濃度的主要貢獻單體,2,3,4,7,8-PeCDF是總TEQ貢獻最大的單體.

3.5 對焚燒廠周邊區(qū)域人群的PCDD/Fs呼吸暴露劑量的估算結(jié)果表明其處于較為安全的水平,但大氣重污染季節(jié)的呼吸暴露風險應(yīng)該得到足夠的重視.

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Concentrations, spatial and seasonal variations of PCDD/Fs in ambient air around a municipal solid waste incinerator—a case study in Beijing.

QI Li*, REN Yue, LI Nan, ZHENG Sen, ZHAO Hu, FAN Shuang, ZHOU Zhi-guang, XU Peng-jun, LIU Ai-min, ZHANG Ting, HUANG Ye-ru (State Environmental Protection Key Laboratory of Dioxin Pollution Control, National Research Center for Environmental Analysis and Measurement, Beijing 100029, China). China Environmental Science, 2016,36(4)：1000～1008

Abstract：The concentrations, profiles and seasonal variations of PCDD/Fs in ambient air around a municipal solid waste incinerator (MSWI) in Beijing from April 2013 to January 2014 were investigated. The mass concentrations and TEQ of 2,3,7,8-substituted PCDD/Fs in the air samples ranged from 8.3 to 115pg/m3and from 0.11to 1.9pg I-TEQ/m3, respectively. The concentration values at 1sampling site in autumn and all 5sampling sites in winter were higher than the ambient air standard of 0.6pg I-TEQ/m3for dioxins regulated in Japan. 1,2,3,4,6,7,8-HpCDF and OCDF dominated PCDD/Fs in all the samples for all four seasons, while 2,3,4,7,8-PeCDF was the dominant congener contributing to TEQ. The spatial distribution basically exhibited a trend that the concentrations at site close to the MSWI (～400m) are higher whereas those at other sites (>1000m) are comparable and not related to the distances from the source. Seasonal variation showed obviously higher concentration in winter than the other three seasons, which may attribute to domestic heating and worse atmospheric dispersion that occur in winter. The homologue and congener profiles of PCDD/Fs in the air samples differed from those of the flue gas emission from the MSWI, consistent with the principal component analysis results, indicating that the concentrations of PCDD/Fs in ambient air were not affected by the MSWI exclusively, but jointly influenced by multiple sources. Dioxin inhalation exposure dose estimation showed that the dioxin inhalation exposure risk of residents living in the studied area was at a relative safe level (0.034～0.161pg I-TEQ/(kg?d)). However, the dioxin inhalation exposure risk in heavily polluted seasons still needed great concerns.

Key words：MSWI；ambient air；PCDD/Fs；seasonal variation；principal component analysis；inhalation exposure

作者簡介：齊 麗(1980-),女,河北邢臺人,高級工程師,博士,主要從事二類及有機氣溶膠研究.發(fā)表論文20余篇.

基金項目：國家重點基礎(chǔ)研究發(fā)展計劃(973計劃)項目(2015CB453101)

收稿日期：2015-08-30

中圖分類號：X510.2,X831 文獻識別碼：A

文章編號：1000-6923(2016)04-1000-09