本文關(guān)鍵詞： 肺癌 燃煤 單顆粒 毒性 相關(guān)系數(shù)　出處：《中國(guó)礦業(yè)大學(xué)(北京)》2016年博士論文　論文類型：學(xué)位論文

【摘要】：本文通過(guò)環(huán)境科學(xué)、單顆粒分析、元素分析與多種生物毒理學(xué)研究方法,詳細(xì)分析了宣威肺癌高發(fā)區(qū)虎頭和對(duì)照點(diǎn)肺癌低發(fā)區(qū)西澤室內(nèi)大氣顆粒物(包括PM10、PM2.5和分級(jí)顆粒物)的物理化學(xué)特征及其毒性,分析其相互關(guān)系,并提出顆粒物毒性表征的方法。研究結(jié)果發(fā)現(xiàn):宣威夏季PM10的24小時(shí)質(zhì)量濃度均值區(qū)間為203.06μg/m3-365.26μg/m3,高于我國(guó)PM10二級(jí)標(biāo)準(zhǔn)(150μg/m3);冬季樣品中,生物質(zhì)燃燒產(chǎn)物的質(zhì)量濃度最大(達(dá)到350μg/m3),其次是用電(夜晚燃煤)農(nóng)戶室內(nèi)顆粒物,最后是燃煤排放顆粒物。夏季樣品中,燃煤產(chǎn)物的質(zhì)量濃度最大(達(dá)到350μg/m3),其次是用電和生物質(zhì)燃燒產(chǎn)物,最后是室外顆粒物。冬夏季節(jié)兩個(gè)采樣點(diǎn)顆粒物的平均濃度并無(wú)大的波動(dòng);冬季宣威地區(qū)虎頭舊戶PM2.5,虎頭新戶PM2.5和西澤舊戶PM10對(duì)應(yīng)的I/O值(室內(nèi)外顆粒物質(zhì)量濃度比)分別為1.10,1.78和2.27,都大于1,說(shuō)明宣威地區(qū)室內(nèi)顆粒物來(lái)源于室內(nèi)污染源。宣威地區(qū)虎頭室內(nèi)外PM2.5質(zhì)量濃度范圍為38.54-102.64μg/m3,西澤室內(nèi)外PM2.5質(zhì)量濃度范圍為32.94μg/m3-54.70μg/m3,其中虎頭舊戶PM2.5質(zhì)量濃度明顯高于其他采樣點(diǎn)。宣威地區(qū)虎頭室內(nèi)外PM10質(zhì)量濃度范圍為84.09μg/m3-355.75μg/m3,西澤室內(nèi)外PM10質(zhì)量濃度范圍為51.23μg/m3-661.49μg/m3,其中西澤舊戶白天PM10質(zhì)量濃度明顯高于其他采樣點(diǎn),幾乎達(dá)到三倍之多,可見相對(duì)于燃煤產(chǎn)物,生物質(zhì)燃燒會(huì)產(chǎn)生更多的大氣可吸入顆粒物濃度;對(duì)于質(zhì)量濃度均值來(lái)說(shuō),2013年冬季虎頭村PM10均值無(wú)論白天還是夜晚都幾乎是2011年冬季的1/2,而2013年冬季白天PM2.5均值幾乎為2011年冬季的1/3,夜晚幾乎相同。三年過(guò)去,虎頭室內(nèi)的顆粒物平均濃度都顯著降低,相應(yīng)的污染減小。使用帶能譜的透射電鏡對(duì)宣威各采樣點(diǎn)的單顆粒樣品進(jìn)行分析發(fā)現(xiàn),虎頭和西澤采樣點(diǎn)的單顆粒粒徑范圍都在0.2μm-3μm,粒徑大于2μm的顆粒在兩個(gè)采樣點(diǎn)的數(shù)量都比較少。兩個(gè)采樣點(diǎn)的粒度分布規(guī)律相似,且粒徑在1μm以下的顆粒物數(shù)量都比粒徑大于1μm的多�；㈩^和西澤地區(qū)樣品中硫元素和硅元素最為豐富,西澤作為低肺癌發(fā)病率的采樣點(diǎn)相比高肺癌發(fā)病率地區(qū)虎頭,其樣品中檢測(cè)到的元素種類少八種,然而只有西澤樣品中檢測(cè)出了砷元素;根據(jù)透射電鏡及能譜分析結(jié)果將宣威地區(qū)室內(nèi)單顆粒樣品劃分為五種類型:飛灰,有機(jī)質(zhì)(煙塵,焦油球和生物顆粒),礦物顆粒,硫酸鹽和混合顆粒物;在兩個(gè)采樣點(diǎn)中混合顆粒為主要顆粒類型,所占的數(shù)量也最多。固體單顆粒如飛灰,有機(jī)質(zhì)和礦物顆粒與大氣中酸性氣體以及空氣中的水蒸氣接觸并反應(yīng),形成h+,so42-和no3-等離子,進(jìn)一步化學(xué)反應(yīng)會(huì)產(chǎn)生混合顆粒。大部分混合顆粒物為外混或內(nèi)混顆粒,內(nèi)混包括煙塵,有機(jī)質(zhì),礦物質(zhì)與硫酸和有機(jī)質(zhì)等的混合;混合顆粒物的老化程度可以參考典型的核殼結(jié)構(gòu)顆粒物及其核殼比。核殼顆粒物的等效粒徑范圍為0.5μm-2.5μm,平均粒徑為1.6μm,幾乎所有核殼顆粒的核殼比在0.4到0.8之間,平均比例為0.6。使用質(zhì)粒dna損傷評(píng)價(jià)法對(duì)宣威地區(qū)室內(nèi)大氣顆粒物進(jìn)行毒性分析,得出在50,100,150,200,250μg/ml劑量下,宣威冬季不同采樣點(diǎn)pm10的dna損傷率范圍為6%-98%,最高值出現(xiàn)在冬季西澤生物質(zhì)燃燒產(chǎn)生的顆粒物樣品中。宣威夏季不同采樣點(diǎn)pm10的dna損傷率范圍為24%-72%,最高值出現(xiàn)在夏季虎頭燃煤產(chǎn)物中。夏季大氣顆粒物dna損傷率整體高于冬季,無(wú)論冬季夏季,西澤地區(qū)生物質(zhì)燃燒產(chǎn)生的pm10的dna損傷率都較高。在50,100,150,200,250,500,1000μg/ml劑量下,宣威所有pm10樣品的dna損傷率范圍從15%到95%,樣品的損傷率在50μg/ml到500μg/ml的劑量范圍內(nèi)隨劑量增大而增大;虎頭村冬季樣品中,居民在做飯時(shí)采集的顆粒物損傷率明顯比不做飯時(shí)高。對(duì)比虎頭和西澤兩個(gè)采樣點(diǎn)白天和夜晚的顆粒物樣品,夜晚的顆粒物dna損傷率明顯較高,在西澤尤為明顯。對(duì)比燃煤,生物質(zhì)燃燒和用電農(nóng)戶大氣顆粒物的dna損傷率可以得到,燃煤產(chǎn)物dna損傷率最高,其次是生物質(zhì)燃燒,最后是用電農(nóng)戶采集的大氣顆粒物。宣威地區(qū)部分農(nóng)戶沒有帶煙囪的廚房,而是直接在客廳做飯,對(duì)比發(fā)現(xiàn)有煙囪的房間采集的大氣顆粒物的dna損傷率低于沒有煙囪的房間;dna損傷率與質(zhì)量濃度之間沒有明顯的相關(guān)趨勢(shì),主要是因?yàn)轭w粒物對(duì)人體的危害主要是與顆粒物的化學(xué)組成和表面吸附的有毒有害物質(zhì)有關(guān),因此不能僅僅利用顆粒物的質(zhì)量濃度來(lái)評(píng)價(jià)顆粒物對(duì)人體健康的影響。在細(xì)胞凋亡實(shí)驗(yàn)中,在6.25μg/ml到50μg/ml的劑量范圍內(nèi),宣威樣品的細(xì)胞凋亡率較小,且呈現(xiàn)微弱的上升趨勢(shì),且宣威室內(nèi)樣品在實(shí)驗(yàn)設(shè)置的最高劑量下(50μg/ml)的細(xì)胞凋亡率最高。在紅細(xì)胞溶解實(shí)驗(yàn)中,在實(shí)驗(yàn)所用50、250、500、1000、2000μg/ml各劑量下,宣威樣品的紅細(xì)胞溶劑率較小,說(shuō)明宣威樣品在劑量高達(dá)2000μg/ml時(shí)都不足以對(duì)人血紅細(xì)胞造成較大的溶解率,則對(duì)于宣威樣品來(lái)說(shuō),人體只有在接觸足夠高濃度的大氣顆粒顆粒物后,人體的血紅細(xì)胞才有可能被溶解損害。使用電感耦合等離子質(zhì)譜法(icp-ms)對(duì)宣威大氣顆粒物樣品中所含微量元素進(jìn)行分析,結(jié)果得出zn,ti和ni元素的濃度在所有樣品中都含量較高,冬季樣品中zn元素含量范圍是676ppm-16978ppm,ti元素含量范圍是577ppm-25560ppm,ni元素含量范圍是459ppm-6508ppm。夏季樣品的zn元素含量范圍是2013ppm-22220ppm,Ti元素含量范圍是755ppm-1620ppm,Ni元素含量范圍是1058ppm-9200ppm。各元素濃度相對(duì)較高的出現(xiàn)在冬季虎頭新戶樣品和冬季西澤舊戶樣品,且前者所含元素總濃度較高,為81841.96ppm,可能由于冬季虎頭新戶雖用電做飯,但是每天夜晚燃煤取暖,且屋內(nèi)不通風(fēng)。冬季樣品總元素含量高于夏季樣品,其中,最高值出現(xiàn)在冬季虎頭用電農(nóng)戶中,為36590.45ppm。最低值出現(xiàn)在冬季虎頭燃煤農(nóng)戶中,為8157.45ppm。夏季樣品中元素總含量最高值出現(xiàn)在虎頭室外,為30318.82ppm,最低值出現(xiàn)在夏季虎頭燃煤農(nóng)戶中,為9226.74 ppm;宣威樣品中,Zn元素含量與DNA損傷率呈現(xiàn)正相關(guān),在0.05的顯著性水平下相關(guān)系數(shù)為0.67,說(shuō)明顆粒物中的水溶性鋅有可能是造成質(zhì)粒DNA氧化性損傷的主要原因之一;將顆粒物中微量元素的含量轉(zhuǎn)換為標(biāo)準(zhǔn)狀況下空氣中微量元素質(zhì)量濃度(ng/m3),在大氣中濃度最高的三種元素依次為Zn,Ni,Ti,其中Zn元素在空氣中的濃度范圍為11.1916ng/m3-424.4598ng/m3,Ni元素在空氣中的濃度范圍為8.9197ng/m3-118.1527 ng/m3,Ti元素在空氣中的濃度范圍為16.3403ng/m3-639.0148 ng/m3。2013年冬季燃煤室內(nèi)大氣微量元素的含量降低,沒有出現(xiàn)質(zhì)量濃度高于500 ng/m3的的元素,且質(zhì)量濃度在10ng/m3以下的元素種類更多。在2011年和2013年冬季燃煤室內(nèi)大氣微量元素中,Zn元素含量都為最高,但是在2013年冬季檢測(cè)到的Zn元素比2011年低一個(gè)等級(jí);對(duì)比EDX(Energy Dispersive X-ray)和ICP-MS兩種方法,其分析結(jié)果相互照應(yīng)。在無(wú)機(jī)組分方面,將Zn元素作為定義顆粒物毒性的基準(zhǔn)元素,使用DNA損傷率與之所有元素之間的相關(guān)系數(shù),以及所有與Zn元素有相關(guān)性的元素的相關(guān)系數(shù)可以來(lái)表征顆粒物的毒性。
[Abstract]:This article through environmental science, single particle analysis, elemental analysis and various biological toxicology research methods, detailed analysis of lung cancer in high incidence area of the tiger and the control point in low incidence area of lung cancer Cesar indoor atmospheric particles (including PM10, PM2.5 and graded particles) physical and chemical characteristics and toxicity analysis and their relationship, and puts forward the method of particle characterization of toxicity. The results showed: Xuanwei summer PM10 24 hours mean concentration range of 203.06 mu g/m3-365.26 mu g/m3, higher than China's PM10 standard level two (150 g/m3); winter samples, biomass combustion product concentration maximum (up to 350 g/m3), followed by electricity (night coal) indoor particulate matter, finally the emission of particles of coal samples. In summer, the quality of the product (the largest coal concentration reached 350 g/m3), followed by electricity and biomass combustion products, finally the outdoor particulate matter. The season two average concentration of particles is no big fluctuations in winter; the Xuanwei Tiger Old PM2.5, new PM2.5 and Cesar old tiger households households PM10 the corresponding I/O value (indoor and outdoor particle concentration ratio) were 1.10,1.78 and 2.27, are greater than 1, explain the sources of indoor particles in Xuanwei the indoor pollution source. The Xuanwei tiger indoor and outdoor PM2.5 concentration range of 38.54-102.64 g/m3, Cesar indoor and outdoor PM2.5 concentration range of 32.94 g/m3-54.70 g/m3, the old tiger households PM2.5 concentration was significantly higher than that of other sampling points. Xuan Weihai tiger indoor and outdoor PM10 concentration range of 84.09 mu g/m3-355.75 mu g/m3, Cesar indoor PM10 mass concentration of 51.23 Mu g/m3-661.49 mu g/m3, the mass concentration of PM10 during the day old Cesar households was higher than that of other sampling points, almost three times, compared to the visible combustion products Biomass combustion, will produce more atmospheric PM10 concentration; the mean concentration for quality, in the winter of 2013, Steller village PM10 means both day and night is almost in the winter of 2011 1/2, 2013 PM2.5 winter day in the winter of 2011 the mean value is 1/3, the night is almost the same. Over the past three years, the average particle concentration of tiger the indoor were significantly reduced, the corresponding reduction of pollution. With the use of transmission electron microscopy spectrum of single particle Xuanwei samples of each sampling point was found, the tiger and the Cesar sampling point of single particle size in the range of 0.2 M-3 m, the particle size of more than 2 mu m particles in two sampling points the number is less. The size distribution of the two sampling points of similarity in the number and the size of 1 mu m or less than the particle diameter greater than 1 m. The tiger and Cesar area samples of sulfur and silicon is the most abundant, Cesar as low incidence rate of lung cancer with high incidence of lung cancer samples compared to the tiger area, the kinds of elements in samples detected eight samples, but only Cesar detected arsenic; according to transmission electron microscopy and energy spectrum analysis results in Xuanwei indoor single particle samples were divided into five types: fly ash. Organic matter (soot, tar balls and biological particles), mineral particles, sulfate and mixed particles; in two sampling points in the mixed particles as the main types of particles, the number of accounts for the most. The solid particles such as fly ash, organic matter and mineral particles in the atmosphere and acidic gases and water vapor in the air the contact and reaction, the formation of h+, so42- and no3- in plasma, further chemical reactions will produce mixed particles. Most mixed particles for external mixing or mixed particles, including mixed dust, organic matter, mineral acid and sulfur and organic matter mixed ; the aging degree of mixed particles can refer to core-shell structure particles and core-shell ratio. Typical core-shell particles of the equivalent diameter range of 0.5 mu m-2.5 mu m, the average particle size of 1.6 m, almost all the core-shell particles with core-shell ratio between 0.4 to 0.8, the average ratio of 0.6. evaluation of DNA damage plasmid by analyze the toxicity of Xuanwei in atmospheric particulate matter in indoor, obtained 50100150200250 g/ml doses, Xuanwei in different sampling points of PM10 DNA damage rate in the range of 6%-98%, the highest value in biomass combustion in winter Cesar particulate samples. Xuanwei summer in different sampling points of PM10 DNA damage the rate range is 24%-72%, the maximum value appeared in summer. The summer tiger in the residues of atmospheric particulate matter DNA damage rate is higher than that in winter, regardless of winter summer, burning area Cesar biomass of PM10 DNA damage rate are higher. In the 501001502002505001000 g/ml dose, Xuanwei of all PM10 samples DNA damage rate ranges from 15% to 95%, the rate of injury to the sample dose range of 500 g/ml with increasing doses of 50 g/ml increases; Steller village residents in the winter samples, when cooking collected particles damage significantly than cooking high contrast. The tiger and Cesar two sampling points of the day and night particulate samples, night particles DNA damage rate was significantly higher in Xizeyou obviously. Compared with coal, biomass burning and electric household atmospheric particulate DNA damage rate can be obtained, combustion products DNA damage rate is the highest, followed by biomass burning finally is the use of atmospheric particles collected. Some farmers household electrical Xuanwei with no chimney in the kitchen, but the living room directly in the cooking, found that DNA damage the room collected atmospheric particles with the chimney No room rate is lower than the chimney; no obvious correlation between DNA damage rate and the mass concentration of particles is mainly because the harm to human body is mainly toxic and harmful substances in chemical composition and surface adsorption and particle related, so just use particle mass concentrations to evaluate the effects of particulate matter on human health in the cell apoptosis in the experiment, 6.25 g/ml to 50 g/ml within the dose range, the apoptosis rate of Xuanwei samples is small, and showed a weak upward trend, Xuanwei and laboratory samples at the highest dose under the experimental setup (50 g/ml). The apoptosis rate was the highest in red cell lysis experiments. In 5025050010002000 experiments with different doses of g/ml, red blood cell sample solvent Xuanwei rate is smaller, indicating Xuanwei samples at doses up to 2000 g/ml are not enough to cause a larger dissolution of human red blood cells The sample rate, Xuanwei, only in the human body exposed to sufficient atmospheric particulate high concentrations of particles, human red blood cells can be dissolved damage. Using inductively coupled plasma mass spectrometry (ICP-MS) analysis of the trace elements contained in Xuanwei atmospheric particles in the Zn, the concentration of Ti. And the Ni element content in all samples are higher in winter, samples of the Zn element content in the range of 676ppm-16978ppm, the content of Ti is in the range of 577ppm-25560ppm, the content of Ni is in the range of Zn elements in the 459ppm-6508ppm. summer sample range is 2013ppm-22220ppm, the content of Ti is in the range of 755ppm-1620ppm, the content of Ni is in the range of 1058ppm-9200ppm. of each element was relatively high the tiger appeared in winter and winter samples of new households Cesar old household sample, and the elements contained in the total concentration of 81841.96ppm, probably due to the winter Although the new tiger households use electricity for cooking, but every night of coal-fired heating, and the house is not ventilated. The winter samples of total element content is higher than that in summer samples, among them, the highest in winter stellers electricity households, the minimum value for 36590.45ppm. in winter is the highest in the coal tiger farmers, the total content of element 8157.45ppm. in summer samples value the tiger outside, 30318.82ppm, the lowest in the summer stellers coal-fired households, 9226.74 ppm; Xuanwei samples, Zn element content and DNA injury rate showed positive correlation at the 0.05 level correlation coefficient was 0.67, indicating particles in the water soluble zinc may be one of the main causes of oxidative DNA damage plasmid; the content of trace elements in particles into quality concentrations of trace elements in standard condition in the air (ng/m3), the atmospheric concentrations of the three elements of the highest order of Zn, Ni Ti, Zn, the concentration range of elements in the air is 11.1916ng/m3-424.4598ng/m3, the concentration range of Ni elements in the air for 8.9197ng/m3-118.1527 ng/m3, the concentration of Ti elements in the air in order to reduce the 16.3403ng/m3-639.0148 ng/m3.2013 winter indoor coal atmospheric trace element contents, no concentration higher than 500 ng/m3 elements, and the mass concentration in 10ng/m3 the following elements more. Trace elements in the 2011 and 2013 winter indoor coal in the atmosphere, the content of Zn were the highest, but the Zn elements in the winter of 2013 detected a grade lower than 2011; compared with the EDX (Energy Dispersive X-ray) and ICP-MS two methods, the results of each other in the inorganic. The components, the Zn element as a reference element to define the toxic effect of particles using correlation coefficients between DNA and the damage rate of all elements, and The correlation coefficient of all elements associated with the Zn element can be used to characterize the toxicity of particles.

【學(xué)位授予單位】：中國(guó)礦業(yè)大學(xué)(北京)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：R122.26;X513

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