哈日巴拉,拓 飛,胡碧濤,王成國(guó),格日勒滿達(dá)呼,許 瀟,張 帥,包山虎,李玉紅?(.蘭州大學(xué)核科學(xué)與技術(shù)學(xué)院,甘肅 蘭州 70000；.內(nèi)蒙古綜合疾病預(yù)防控制中心,內(nèi)蒙古 呼和浩特 000；.中國(guó)疾病預(yù)防控制中心,輻射防護(hù)與核安全醫(yī)學(xué)所,北京 00088；.內(nèi)蒙古師范大學(xué)地理科學(xué)學(xué)院,內(nèi)蒙古 呼和浩特000)

巴彥烏拉鈾礦周圍飲用水中放射性及健康風(fēng)險(xiǎn)

哈日巴拉1,2,拓 飛3,胡碧濤1,王成國(guó)2,格日勒滿達(dá)呼2,許 瀟2,張 帥2,包山虎4,李玉紅1?(1.蘭州大學(xué)核科學(xué)與技術(shù)學(xué)院,甘肅 蘭州 370000；2.內(nèi)蒙古綜合疾病預(yù)防控制中心,內(nèi)蒙古 呼和浩特 010031；3.中國(guó)疾病預(yù)防控制中心,輻射防護(hù)與核安全醫(yī)學(xué)所,北京 100088；4.內(nèi)蒙古師范大學(xué)地理科學(xué)學(xué)院,內(nèi)蒙古 呼和浩特010022)

為了解巴彥烏拉鈾礦周圍居民飲用水中放射性水平及其存在的健康風(fēng)險(xiǎn),開采前采集了鈾礦周圍37份井水飲用水樣品并測(cè)量了總α、總β放射性水平和放射性核素238U、232Th、226Ra和40K的活度濃度.采用世界衛(wèi)生組織(WHO)推薦的方法計(jì)算了飲用井水引起的成人年有效劑量,利用美國(guó)環(huán)保部(USEPA)提出的致癌風(fēng)險(xiǎn)因子評(píng)估了居民終身健康風(fēng)險(xiǎn),同時(shí)將測(cè)量結(jié)果與其它國(guó)家飲用水中放射性水平進(jìn)行了對(duì)比分析.結(jié)果表明,巴彥烏拉鈾礦周圍飲用水中總α和總β平均值分別為1.059Bq/L和0.624Bq/L,其中分別有81.1%和5.4%樣品中總放射性超出了WHO推薦的篩選值0.5Bq/L(總α)和1.0Bq/L(總β).飲用水中238U、232Th、226Ra和40K的活度濃度分別為(2.349±1.593)、(0.058 ±0.041)、(0.070±0.057)和(0.571±0.419)Bq/L.鈾礦周圍居民通過(guò)飲水產(chǎn)生的全年累計(jì)有效劑量為 0.104mSv/a.終生接觸情形下居民經(jīng)飲用水中的放射性暴露引起的終身致癌風(fēng)險(xiǎn)為2.4×10-11.巴彥烏拉鈾礦周圍居民飲用水中放射性活度濃度處于正常水平,對(duì)周圍居民產(chǎn)生的健康風(fēng)險(xiǎn)非常低.

飲用水；總α和總β；放射性核素；巴彥烏拉鈾礦

飲用水通常含有天然放射性核素(包括鈾系、釷系和40K,特別是226Ra、228Ra、234U、238U和210Pb等放射性核素)[1].這些放射性核素通過(guò)飲用會(huì)產(chǎn)生內(nèi)照射并可能產(chǎn)生健康風(fēng)險(xiǎn)[2-3].因此測(cè)量和評(píng)估飲用水中放射性水平對(duì)人體健康危害風(fēng)險(xiǎn)評(píng)估、環(huán)境污染風(fēng)險(xiǎn)評(píng)估、核安全和社會(huì)的穩(wěn)定發(fā)展都有重要的意義[4].近幾十年,飲用水放射性水平的報(bào)道很多,其中多數(shù)均測(cè)量了總α和總β活度濃度水平并估算出了對(duì)居民受照輻射劑量[3,5–19].在 1983～1990年間,我國(guó)完成了一次大范圍的飲用水中放射性水平的測(cè)量和評(píng)估工作[20],之后相關(guān)的報(bào)道數(shù)據(jù)減少[18,21–25].近年來(lái),由人為活動(dòng)引起的天然輻射水平引起了很大的關(guān)注[26-27].隨著大量核電站的建設(shè),我國(guó)加大了對(duì)鈾礦的找礦和開采力度,并發(fā)現(xiàn)了大型甚至特大型的鈾礦床.在內(nèi)蒙古地區(qū)鄂爾多斯盆地、二連盆地巴彥烏拉等地區(qū)發(fā)現(xiàn)了特大型的砂巖型鈾礦,并對(duì)部分鈾礦進(jìn)行了地浸(原位浸出)開采方式[28-29].鈾礦的開采同其它礦產(chǎn)的開采一樣可能對(duì)周圍環(huán)境(水、土壤、草地和生態(tài)環(huán)境)造成不同程度的影響.21世紀(jì)初,鈾礦的開采由露天開采轉(zhuǎn)為地浸開采方法,減少了環(huán)境污染風(fēng)險(xiǎn).目前地浸開采,特別是酸性溶液地浸開采方式,對(duì)地下水中的影響受到了關(guān)注,并已有地下水受到污染的報(bào)道[30-31].國(guó)內(nèi)對(duì)鈾礦周圍環(huán)境污染情況的報(bào)道甚少,于 2012年,有了廣東省北部某鈾礦周圍地表水受到放射性污染的報(bào)道[32];于 2014年,退役后的新疆某鈾礦地下水也受到嚴(yán)重污染[33].然而,此類報(bào)道中均沒(méi)有鈾礦開采本底數(shù)據(jù)和研究結(jié)果.因此,鈾礦開采前周圍居民飲用水的放射性水平尤為重要[34].

目前,我國(guó)已開展了對(duì)核電站及鈾(釷)礦周圍食品放射性污染風(fēng)險(xiǎn)監(jiān)測(cè)工作,其中內(nèi)蒙古鈾(釷)礦周圍為重點(diǎn)監(jiān)測(cè)地區(qū),巴彥烏拉鈾礦與內(nèi)蒙古地區(qū)其它鈾礦相比將采用酸性溶液開采方式,鈾礦層深度與居民飲用水水井深度相近,放射性污染風(fēng)險(xiǎn)較大.本研究對(duì)內(nèi)蒙古巴彥烏拉鈾礦開采之前對(duì)周圍居民的飲用水進(jìn)行了采樣,測(cè)量了飲用水的放射性水平,評(píng)估了對(duì)周圍居民產(chǎn)生的有效劑量和健康風(fēng)險(xiǎn),將檢測(cè)結(jié)果與其他國(guó)家的相關(guān)文獻(xiàn)數(shù)據(jù)進(jìn)行了對(duì)比分析.本研究結(jié)果,不僅建立了巴彥烏拉鈾礦周圍地下飲用水中放射性本底水平,而且對(duì)開采之后可能的放射性污染評(píng)估和后期的環(huán)境修復(fù)工作提供了極為寶貴的基線值,所取得的結(jié)果對(duì)我國(guó)砂巖型鈾礦周圍放射性水平測(cè)量和評(píng)估提供重要的參考依據(jù).

1 材料與方法

1.1 研究區(qū)域和采樣

巴彥烏拉鈾礦位于內(nèi)蒙古錫林郭勒盟蘇尼特左旗西北部,其中心距滿都拉圖鎮(zhèn)北約 30km,在巴彥烏拉蘇木.海拔為1040～1255m.于2004年被發(fā)現(xiàn),是我國(guó)儲(chǔ)量較大的砂巖型鈾礦之一[29].巴彥烏拉鈾礦地區(qū)有著我國(guó)內(nèi)陸氣候的特點(diǎn),夏天熱,冬天冷,四季分明,年均降水量不超過(guò)200mm,處于錫林郭勒大草原的西側(cè),周圍沒(méi)有農(nóng)耕地和企業(yè),居民以放牧為生.居民和牲畜的飲用水全部來(lái)自地下水.采樣工作在2015年6月(雨季)進(jìn)行.以鈾礦為中心30km半徑范圍內(nèi)隨機(jī)選取并采集了37份地下飲用水樣品.樣品均為淺層水井飲用水.

圖1 巴彥烏拉鈾礦位置及采樣點(diǎn)分布Fig.1 Map of the location Bayanwula uranium mining area and sampling points

飲用水樣品均按照我國(guó)國(guó)家標(biāo)準(zhǔn)[35]和世界衛(wèi)生組織推薦的采樣指南[1]進(jìn)行采集.每個(gè)樣品采樣量為 10L,提前將聚乙烯容器用純水洗凈,將井水抽出3～5min再取樣,用硝酸酸化至PH為2左右,密封保存,貼好唯一性標(biāo)簽之后送至實(shí)驗(yàn)室進(jìn)行測(cè)量和分析.巴彥烏拉鈾礦位置及飲用水樣品的采樣點(diǎn)分布見圖 1.其中采樣位置采用全球衛(wèi)星定位系統(tǒng)記錄,通過(guò) ESRI Arc GIS desktop 10.1軟件繪制而成.

1.2 總α和總β的測(cè)量

樣品前處理:將 1L水樣倒進(jìn)玻璃燒杯中,以50～60℃的溫度在電爐上蒸發(fā);當(dāng)水量蒸發(fā)至50mL左右時(shí),轉(zhuǎn)移到蒸發(fā)皿中,滴1mL硫酸,一直燒至無(wú)煙為止,然后放入馬弗爐內(nèi),以 350℃溫度燒 1h;再放置至干燥器中冷卻至室溫,取出研磨待測(cè)[1,36].采用德國(guó) Berthold公司生產(chǎn)的低本底LB770型10道氣流式α、β計(jì)數(shù)器進(jìn)行測(cè)量.為了屏蔽環(huán)境本底輻射的干擾,計(jì)數(shù)器探頭和樣品盒均用 10cm 厚的鉛磚包圍.設(shè)備測(cè)量高壓為1650V.測(cè)量系統(tǒng)由中國(guó)計(jì)量科學(xué)研究院提供的α粉末標(biāo)準(zhǔn)物質(zhì)(241Am,比活度14.7Bq/g)和β粉末標(biāo)準(zhǔn)物質(zhì)(40K,比活度16.1Bq/g)進(jìn)行了校準(zhǔn).每次測(cè)量前后進(jìn)行本底測(cè)量,取平均值從樣品計(jì)數(shù)率中扣除,本底測(cè)量時(shí)間為 1000min.每個(gè)樣品均用2道計(jì)數(shù)器測(cè)量總α和總β的活度濃度.樣品的測(cè)量和系統(tǒng)的刻度采用相同規(guī)格的測(cè)量盤.探測(cè)下限由公式(1)確定[36]:

式中:CR為本底計(jì)數(shù)率,counts/min;ε為探測(cè)效率;t為測(cè)量時(shí)間,min;V為樣品體積,L.總α和總β探測(cè)下限分別為0.0028和0.0412Bq/L.每個(gè)樣品的總α和總β活度濃度通過(guò)公式(2)計(jì)算.

式中:A為總α和總β的活度濃度,Bq/L;Nsample為樣品計(jì)數(shù)率,cpm;Nbackground為本底計(jì)數(shù)率,cpm;60為分至秒的轉(zhuǎn)換系數(shù);其他與公式(1)相同.

1.3 放射性核素238U、232Th、226Ra和40K的測(cè)定

每份樣品取8L水倒入燒杯中以50～60℃溫度在電爐上蒸發(fā)至2L,冷卻至室溫,轉(zhuǎn)移至2L馬林杯樣品盒中,密封放置30d以上至到226Ra和子體之間達(dá)到放射性平衡,待測(cè).測(cè)量系統(tǒng)為美國(guó)ORTEC?公司生產(chǎn)的高純鍺(HPGe)γ譜儀;探測(cè)器為 p型同軸圓柱形探測(cè)器;探測(cè)相對(duì)效率為32%以上,在60Co核素1.33MeV能量上的分辨率為1.82keV.測(cè)量范圍在40keV～2MeV之間,軟件系統(tǒng)為Gamma Vision 6.01?版本,8192道分析器.鉛室厚度為 10mmPb.整個(gè)樣品的測(cè)量前后分別測(cè)量一次24h本底譜,從樣品譜中減去本底計(jì)數(shù).探測(cè)下限(MDA)由式(3)得出[38-39]:

式中:Kα為95%置信度下的統(tǒng)計(jì)因子1.645;Nb本底計(jì)數(shù);P為γ衰變率;ε為γ特定全能峰效率;t為測(cè)量時(shí)間,s;V 為裝樣體積,L;探測(cè)下限為238U: 0.343Bq/L、232Th:0.015Bq/L、226Ra:0.011Bq/L和40K:0.159Bq/L.能量刻度和效率刻度均采用中國(guó)計(jì)量科學(xué)研究院認(rèn)證的 2L馬林杯水體標(biāo)準(zhǔn)源(標(biāo)準(zhǔn)編號(hào):14NST/2L-080501).樣品和水體標(biāo)準(zhǔn)源的規(guī)格重量相同,測(cè)量條件相同,測(cè)量時(shí)間為24h.238U的活度濃度由234Th(63.2keV)獲得;232Th由212Pb (238.6keV)和228Ac (911.2keV)得出;226Ra的活度濃度由214Pb(351.9keV)和214Bi(609.3keV)得出;40K的活度濃度由能量1460.8keV獲取.通過(guò)公式(4)計(jì)算活度濃度[37-38]:

式中:A為核素的活度濃度,Bq/L;Nnet為凈計(jì)數(shù)率, s-1,這里已減去本底計(jì)數(shù).其他與式(3)相同.

1.4 年有效劑量

通過(guò)飲用引起的水中γ射線對(duì)人體的年有效劑量由式(5)得出[1]:

式中:AED為年有效劑量,mSv/a;2為成人每天平均飲水量[1],L/d;365d/a;DCi劑量轉(zhuǎn)換系數(shù), mSv/Bq.

1.5 終身健康風(fēng)險(xiǎn)

通過(guò)飲用引起的水中放射性核素對(duì)居民終身致癌的風(fēng)險(xiǎn)由式(6)估算[39]:

LTRA為終身致癌風(fēng)險(xiǎn);DL為壽命,76.1年[40]; RF為致癌風(fēng)險(xiǎn)轉(zhuǎn)換因子,Sv-1.

2 結(jié)果與討論

2.1 地下飲用水放射性概況

巴彥烏拉鈾礦周圍30km半徑內(nèi)37份井水飲用水樣品中總α和總β的活度濃度結(jié)果見表1.總α活度濃度范圍在 MDA～2.436Bq/L之間,平均值為 1.059Bq/L,已超出了我國(guó)飲用水中總α活度濃度測(cè)量范圍0.01～0.25Bq/L[41].總β的平均值為 0.624Bq/L,變化范圍為 0.258～1.057Bq/L,在我國(guó)飲用水中的結(jié)果范圍 0.04～1.22Bq/L[42]之內(nèi).總α的平均值高于總β平均值.在37份井水飲用水樣品中有 30份樣品中總α超出了WHO和我國(guó)飲用水標(biāo)準(zhǔn)規(guī)定的篩選值 0.5Bq/L[1],占81.1%;2份井水飲用水樣品中總β值超出了規(guī)定的篩選值1.0Bq/L[1],占5.4%.根據(jù)WHO和我國(guó)飲用水標(biāo)準(zhǔn)規(guī)定,如果飲用水中總α和總β活度濃度超出了篩選值(總α:0.5Bq/L,總β:1.0Bq/L),則應(yīng)進(jìn)行放射性核素分析;如果一種或多種核素超出了指導(dǎo)水平,則可以考慮采取相應(yīng)的措施減少對(duì)公眾輻射劑量的貢獻(xiàn).由表 1可知,放射性核素238U、232Th、226Ra和40K的活度濃度分別為(2.349±1.593)、(0.058±0.041)、(0.070± 0.057)和(0.351±0.278Bq/L).其中238U、232Th和226Ra的活度濃度均低于WHO推薦的指導(dǎo)水平10,1和1Bq/L.對(duì)于40K(β放射性核素),由于K是人體內(nèi)重要元素之一并主要通過(guò)食入攝取,當(dāng)飲用水中總β活度濃度超出 1.0Bq/L時(shí)應(yīng)減去40K對(duì)總β的貢獻(xiàn).因此WHO沒(méi)有規(guī)定對(duì)40K在飲用水中的指導(dǎo)水平.對(duì)于總β活度濃度超出的30和 31號(hào)樣品,若減去40K的活度濃度(包括MDA),則總β活度濃度則低于1.0Bq/L.因此可以不考慮井水飲用水中總β對(duì)巴彥烏拉鈾礦周圍居民健康風(fēng)險(xiǎn).

表1 巴彥烏拉鈾礦周圍飲用水樣品的放射水平Table 1 The radioactivity level in drinking water samples around Bayanwula uranium mining area

續(xù)表1

表2 測(cè)量結(jié)果與世界其他地區(qū)的結(jié)果對(duì)比Table 2 Comparison between theresults in this studyand the drinking water radioactivity levels from other partsof the world

表 2列出了本研究結(jié)果和世界其他地區(qū)的檢測(cè)結(jié)果.瑞典地下水中238U活度濃度較高,最高位5.3Bq/L,但葡萄牙Horta da Vilari?a鈾礦開采之前周圍井水飲用水中238U 活度濃度在 0.1～48.1Bq/L之間變化,本研究結(jié)果處于較高水平.對(duì)于232Th的活度濃度,也門的地下水中最高,其次為我國(guó)飲用水中的本底測(cè)量結(jié)果,本研究結(jié)果低于我國(guó)平均值.也門地下水中226Ra的活度濃度較高,但在美國(guó)Wyoming鈾礦周圍井水飲用水中本底水平為 21.4Bq/L,本研究結(jié)果處于我國(guó)飲用水中的正常范圍之內(nèi).40K的測(cè)量結(jié)果較少,本研究結(jié)果中40K活度濃度處于我國(guó)飲用水中的正常范圍之內(nèi).

2.2 經(jīng)口飲水途徑放射性核素的健康風(fēng)險(xiǎn)

環(huán)境放射性核素主要通過(guò)3種途徑(吸入、食入和通過(guò)皮膚)對(duì)人體產(chǎn)生放射性劑量貢獻(xiàn).對(duì)飲用水而言,主要為食入途徑的貢獻(xiàn).表3給出了4種天然放射性核素WHO推薦的劑量轉(zhuǎn)換系數(shù)[1]、USEPA提出的致癌風(fēng)險(xiǎn)轉(zhuǎn)換因子[39]、年有效劑量和終身致癌風(fēng)險(xiǎn).巴彥烏拉鈾礦周圍居民通過(guò)飲用產(chǎn)生的年有效劑量為 0.104mSv/a,飲用水中238U、232Th、226Ra和40K核素對(duì)巴彥烏拉鈾礦周圍居民產(chǎn)生的終身致癌風(fēng)險(xiǎn)均小于1.1×10-11,是非常低的概率.利用公式(6)中的參數(shù),葡萄牙Horta da Vilari?a鈾礦開采前周圍井水飲用水238U最高活度濃度對(duì)居民的終身致癌風(fēng)險(xiǎn)為2.1×10-10,美國(guó)Wyoming鈾礦周圍井水飲用水中226Ra對(duì)居民的終身致癌風(fēng)險(xiǎn)為3.5×10-9,均高于巴彥烏拉鈾礦周圍井水飲用水對(duì)居民的終身致癌風(fēng)險(xiǎn)1.1×10-11,但都屬于非常低的致癌風(fēng)險(xiǎn).

表3 年有效劑量和終身致癌風(fēng)險(xiǎn)Table 3 Annual effective dose and lifetime cancer risk

由于本次研究只是在豐水期進(jìn)行采樣和測(cè)量的結(jié)果,所以還需要研究枯水期的情況,可進(jìn)一步對(duì)鈾礦周圍食品中開展放射性水平測(cè)量,并結(jié)合膳食結(jié)構(gòu)對(duì)居民產(chǎn)生的劑量貢獻(xiàn)進(jìn)行評(píng)估和研究.

3 結(jié)論

通過(guò)對(duì)巴彥烏拉鈾礦開采前周圍30km半徑內(nèi)居民井水飲用水中總α和總β的測(cè)量,發(fā)現(xiàn)了總α活度濃度超出了WHO和我國(guó)飲用水中規(guī)定的篩選值.因此進(jìn)一步確定了飲用水樣品中主要天然放射性核素238U、232Th,226Ra和40K的活度濃度,估算了年有效劑量和患癌風(fēng)險(xiǎn)概率.結(jié)果表明巴彥烏拉鈾礦周圍居民經(jīng)井水飲用引起的成人年有效劑量很小,終身致癌風(fēng)險(xiǎn)非常低.巴彥烏拉鈾礦周圍居民飲用水中放射性水平與世界其他國(guó)家飲用水中結(jié)果相比,處于正常范圍之內(nèi).

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致謝：作者要感謝錫林郭勒盟疾病預(yù)防控制中心的白桂林和蘇尼特左旗疾病預(yù)防控制中心的呼和吉樂(lè)圖在采樣工作中的幫助.

Radioactivity and health risk of drinking water around Bayanwula uranium mining area.

BAI Haribala1,2, TUO Fei3, HU Bi-tao1, WANG Cheng-guo2, SAI Ge-ri-le-man-da-hu2, ZHANG Shuai2, XU Xiao2, BAO Shan-hu4, LI Yu-hong1*(1.School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, China；2.Inner Mongolia Center for Disease Control and Prevention, Huhhot 010031, China；3.College of Geographical Science, Inner Mongolia Normal University, Huhhot 010022, China；4.National Institute for Radiological Protection, Chinese Center for Disease Control and Prevention, BeiJing 100088, China). China Environmental Science, 2017,37(9)：3583～3590

The total of 37 drinking water samples from the wells around Bayanwula prospective uranium mining area were collected to estimate the lifetime health risks for the residents. The concentrations of gross α, gross β,238U,232Th,226Ra and40K were analyzed. The method recommended by World Health Organization (WHO) was used to calculate the adult annual effective dose via the consumption of thedrinking water. The cancer risk coefficients recommended by the United States Environmental Protection Agency (USEPA) were applied to assess the life-time health risk cancer for the residents. The radioactivity levels in the drinking water samples were compared to the data obtained from other part of the world. The results indicated thatthe average activity concentrations of gross α and gross β were 1.059Bq/L and 0.624Bq/L, respectively, which showed the 81.1% and 5.4% out of the 37water samples exceed the screening values 0.5Bq/L and 1.0Bq/L recommended by WHO, respectively. The activity concentrations of238U,232Th,226Ra and40K were determined to be (2.349±1.593), (0.058±0.041), (0.070±0.057) and (0.571±0.419)Bq/L, respectively. The annual effective dose to adult via the consumption of the drinking water was calculated to be 0.104mSv/aand the lifetime cancer riskwas assessed to 2.4×10-11for the residents. In conclusion, the activity concentrations in drinking water around Bayanwula uranium mining area were at normal level and the radioactivity health risk to the local residentswas at very low level.

drinking water；gross α and gross β；radionuclide；Bayanwula uranium mining area

X82

A

1000-6923(2017)09-3583-08

2017-03-05

內(nèi)蒙古自治區(qū)自然科學(xué)基金資助項(xiàng)目(2013MS0816);內(nèi)蒙古自治區(qū)衛(wèi)生和計(jì)劃生育委員會(huì)醫(yī)療衛(wèi)生科研計(jì)劃項(xiàng)目(201301028)

? 責(zé)任作者, 教授, liyuhong@lzu.edu.cn

哈日巴拉(1981-),男(蒙古族),內(nèi)蒙古興安盟人,蘭州大學(xué)博士研究生,主要從事輻射防護(hù)監(jiān)測(cè)與評(píng)價(jià)研究.發(fā)表論文8篇.