六級大氣顆粒物中超痕量鈾釷的HR-ICP-MS分析方法研究
本文選題:大氣顆粒物 切入點:天然放射性鈾 出處:《中國疾病預(yù)防控制中心》2017年碩士論文 論文類型:學(xué)位論文
【摘要】:鈾釷作為天然放射性元素,廣泛存在于環(huán)境介質(zhì)(土壤、水、空氣)中,其在土壤和水中的含量分別約為μg/g和μg/L量級,釷的天然平均本底含量高于鈾。目前空氣中的鈾釷主要有地殼、土壤揚塵等幾方面來源,人類生產(chǎn)活動(如開采礦山和冶煉、燃煤發(fā)電等)在一定程度上也影響了空氣中放射性鈾釷的濃度水平。鈾釷進(jìn)入人體的途徑主要有飲水、食物和空氣等,其中吸入是最主要、最危險的途徑之一。天然放射性鈾釷既表現(xiàn)放射性毒性,又表現(xiàn)化學(xué)毒性,進(jìn)入人體后主要滯留在骨骼、肝臟、腎臟等人體器官,可能導(dǎo)致造血、神經(jīng)、免疫等系統(tǒng)病變,同時還可能誘發(fā)白血病等疾病。放射性物質(zhì)被空氣中的懸浮顆粒物吸附會形成放射性氣溶膠,其對人體的危害程度與放射性物質(zhì)的濃度水平、機(jī)體本身生理狀態(tài)、氣溶膠的空氣動力學(xué)直徑等有密切關(guān)系。國外針對大氣顆粒物中鈾釷總的含量開展了相關(guān)的監(jiān)測與研究工作,聯(lián)合國原子輻射影響科學(xué)委員會(UNSCEAR)報告了氣溶膠中鈾釷濃度參考值。國內(nèi)針對氣溶膠中天然放射性鈾釷主要在鈾礦等礦區(qū)周圍開展相關(guān)的調(diào)查,目前未制定氣溶膠中鈾釷分析的標(biāo)準(zhǔn)方法和濃度限值。開展大氣顆粒物中鈾釷的分析方法研究,監(jiān)測探討我國氣溶膠中(特別是細(xì)顆粒物中)鈾釷的濃度水平,對于保護(hù)公眾健康和大氣污染防治具有重要的意義。本課題研究了六級大氣顆粒物中超痕量鈾釷的分析方法,優(yōu)化實驗條件,分析討論不同粒徑大氣顆粒物中鈾釷的濃度水平、劑量估算、污染溯源等;主要的研究內(nèi)容如下:(1)六級大氣顆粒物中超痕量鈾釷的分析方法實驗研究通過考察不同材質(zhì)濾膜、酸消解體系以及質(zhì)譜相關(guān)測定條件對本底和樣品中鈾釷含量分析的影響,確定選擇本底鈾釷含量較低的纖維素濾膜進(jìn)行空氣采樣,前處理消解的方法選擇HN03-HC1(王水)-H202的混合酸系,建立了微波消解-電感耦合等離子體質(zhì)譜法測量六級大氣顆粒物中超痕量鈾釷的分析方法。通過含鈾釷標(biāo)準(zhǔn)濾膜的實驗驗證,該方法鈾釷的相對誤差均在10%以下,方法精密度針對鈾釷分別為3%、8%,方法檢出限分別達(dá)到2×10-4ng/m3、1.3×10-3ng/m3,本方法擴(kuò)展相對不確定度U鈾=8%、U釷=4%,實驗方法有效可靠。(2)鈾釷的質(zhì)量濃度水平與氣象因子相關(guān)關(guān)系及分布特征研究運用建立的分析方法,對實際連續(xù)采集的氣溶膠樣品進(jìn)行了分析討論。通過Spearrnan非參數(shù)分析檢驗得出不同粒徑顆粒物中超痕量鈾釷的質(zhì)量濃度與空氣質(zhì)量指數(shù)、濕度呈正相關(guān)關(guān)系;與溫度、風(fēng)速呈負(fù)相關(guān)關(guān)系;鈾釷質(zhì)量濃度在分布特征上表現(xiàn)為夏季低、冬季高,白天低、夜間高的趨勢;鈾釷集中分布在細(xì)顆粒物中,且細(xì)顆粒物受氣象條件的影響比粗顆粒物大。(3)不同粒徑大氣顆粒物中超痕量鈾釷的濃度水平研究運用建立的分析方法,對在北京市實際采集的360個氣溶膠樣品進(jìn)行測量分析。鈾在PM2.1、PM10.2、TSP的質(zhì)量濃度范圍分別是0.039~0.145 ng/m3、0.088~0.238 ng/m3,0.113~0.275 ng/m3;釷在 PM2.1、PM10.2、TSP 的質(zhì)量濃度范圍分別是 0.070~0.227ng/m3、0.166~0.461ng/m3,0.222~0.546ng/m3。天然鈾-238活度濃度范圍為0.291~5.007 μBq/m3,平均值2.194 μBq/m3,釷-232活度濃度范.圍為 0.334~3.712 μBq/m3,平均值 1.541 μBq/m3。(4)吸入所致內(nèi)照射劑量估算與含鈾釷顆粒物溯源分析運用生物動力學(xué)模型和國家標(biāo)準(zhǔn)GB18871-2002提供的劑量轉(zhuǎn)換系數(shù)進(jìn)行待積有效劑量的估算。本次研究表明公眾因吸入天然放射性鈾釷引起的年待積有效劑量均值是0.345 μSv/a,范圍為0.073 μSv/a~0.828 μSv/a,遠(yuǎn)遠(yuǎn)小于UNSCEAR報告給出的天然輻射源所致公眾年有效劑量2.4 mSv/a。通過HYSPLIT模型對北京市2016年采樣期間三次空氣中鈾釷濃度較高的污染過程進(jìn)行了 72小時氣流追蹤溯源分析,境外氣流方向主要來自西北部和北部方向;境內(nèi)氣流方向主要來自礦產(chǎn)豐富、人口密集的相關(guān)地區(qū)和省份。
[Abstract]:Uranium and thorium as natural radioactive elements, widely exist in the environment (soil, water, air medium), its content in soil and water were about g/g and g/L level, the average natural thorium content is higher than the bottom of uranium. Uranium and thorium in the air are the main aspects of soil crust, dust source and human activities (such as mining and smelting, coal-fired power generation etc.) to a certain extent, also affected the concentration of radioactive uranium and thorium in air. Uranium and thorium into the body of the main ways of drinking water, food and air, which is the main way of inhalation, the most dangerous is the performance of natural radioactive uranium and thorium. Radioactive toxicity and chemical toxicity, enters the human body mainly located in bone, liver, kidney and other organs of the body, may cause the blood, nerve, immune system diseases, but also may cause leukemia and other diseases. The radioactive material is in the air The suspended particles attached to the formation of absorbing radioactive aerosol concentration, its harm to the human body and the degree of radioactive substances, the body itself physiological state, there is a close relationship between the aerosol aerodynamic diameter. In foreign countries the total content of uranium and thorium in atmospheric particulates carried out monitoring and related research work, the United Nations Scientific Committee on atomic radiation effect of (UNSCEAR) report of uranium and thorium concentration reference values of aerosol. Investigation for domestic natural radioactive aerosols of uranium and thorium mainly carried out around the uranium mining related, is not currently formulating the limitation standard method and concentration of uranium and thorium in aerosols. To carry out the analysis of uranium and thorium in atmospheric particulates, monitoring of me the aerosol (especially fine particulate) concentrations of uranium and thorium, is of great significance for the protection of public health and the prevention and control of air pollution. The subject of research The analytical method of the six level in the atmospheric particles of trace uranium and thorium, optimizing the experimental conditions, discussed different concentration levels of uranium and thorium in the atmospheric particles dose estimation, pollution source; the main contents are as follows: (1) analysis of the experiments of the six super atmospheric particles of trace uranium and thorium. Through the investigation of different membrane material, acid digestion system and mass spectrometry measurement conditions on the bottom and the content of uranium and thorium in the samples, determine the choice of cellulose membrane of uranium and thorium content in the lower end of the air sampling method, digestion pretreatment HN03-HC1 (aqua regia) mixed acid system -H202, established the analysis method of measurement six super atmospheric particles of trace uranium and thorium by microwave digestion inductively coupled plasma mass spectrometry. The uranium thorium standard membrane experiment, the relative error of the method of uranium and thorium are below 10%, fine method According to the density of uranium and thorium were 3%, 8%, the detection limit reached 2 * 10-4ng/m3,1.3 * 10-3ng/m3 respectively, this method extends the relative uncertainty of U =8% U =4% uranium, thorium, experimental method is effective and reliable. (2) the quality level of concentration of uranium and thorium associated with meteorological factors and distribution characteristics of using the established method the actual, aerosol samples were continuously collected were analyzed and discussed. Through Spearrnan non parametric analysis of different diameter particles of ultra trace uranium and thorium concentration and air quality index, humidity was positively correlated with temperature, wind speed; there was a negative correlation between the concentration of uranium and thorium; distribution characteristics of low in summer in winter, high, low in daytime, nighttime high trend; uranium and thorium are concentrated in fine particles, and the effect of fine particles by meteorological conditions than coarse particle. (3) different particle size of ultra trace uranium and thorium. The concentration level of study using the established method, measurement and analysis of 360 aerosol samples collected in the city of Beijing. Uranium in PM2.1, PM10.2, the concentration of TSP was 0.039 ~ 0.145 ng/m3,0.088 ~ 0.238 ng/m3,0.113 ~ 0.275 ng/m3; in PM2.1 PM10.2, thorium, concentration of TSP were 0.070 ~ 0.227ng/m3,0.166 0.546ng/m3. ~ 0.461ng/m3,0.222 ~ -238 activity of natural uranium concentration range of 0.291 ~ 5.007 Bq/m3, average 2.194 Bq/m3, th -232 activity concentration is 0.334 ~ 3.712. Van Wai Bq/m3, the average value of 1.541 Bq/m3. (4) inhalation and containing uranium and thorium particle tracing analysis using bio kinetic model and the national standard provided by GB18871-2002 dose conversion coefficients to estimate the accumulated effective dose of radiation dose estimation. This study shows that due to the public caused by inhalation of natural radioactive thorium to uranium The mean effective dose of product is 0.345 Sv/a, a range of 0.073 Sv/a ~ 0.828 Sv/a, far less than the UNSCEAR report gives the source of natural radiation caused by the public annual effective dose of 2.4 mSv/a. by sampling the pollution process of uranium and thorium concentration three times higher in the air of Beijing city during the 2016 HYSPLIT model of the source analysis of 72 hours of air track outside the air flow direction mainly from the northwest and north direction; the airflow direction mainly from the territory rich in mineral resources, and related areas of densely populated provinces.
【學(xué)位授予單位】:中國疾病預(yù)防控制中心
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:R14
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