硅穩(wěn)定同位素用于大氣顆粒物和二氧化硅納米顆粒的來源分析
發(fā)布時間：2019-06-14 00:48
【摘要】：二氧化硅納米顆粒作為生產(chǎn)量和使用量最大的納米材料,其毒理學效應逐漸引起了人們的關注,前人的研究指出,來自天然源與來自人為源的二氧化硅納米顆粒具有不同的毒理學效應。但是,目前還沒有方法能夠有效甄別二氧化硅納米顆粒的來源。本文表征了天然源和人為源二氧化硅顆粒的形貌、晶體結構和氧硅比等基本信息。經(jīng)過大量樣品的測定發(fā)現(xiàn),人為源與天然源二氧化硅顆粒中硅穩(wěn)定同位素分布范圍差異明顯,δ~（30）Si(‰)= 0.08可作為人為源和天然源的區(qū)分閾值。此外,4個不同廠家生產(chǎn)的二氧化硅顆粒的硅穩(wěn)定同位素分布范圍較窄,具有同位素指紋識別特征。說明在一定情況下,可以通過二氧化硅顆粒的硅天然穩(wěn)定同位素的差異實現(xiàn)對不同廠家來源的甄別。來自同一工廠,原料相同,合成工藝不同的二氧化硅納米顆粒硅同位素分布也存在明顯差異,說明不同合成工藝造成了不同程度的同位素分餾,這為通過硅同位素分布來甄別二氧化硅顆粒不同合成工藝提供了理論基礎。實驗結果說明,硅穩(wěn)定同位素可以作為甄別二氧化硅納米顆粒的來源的有利工具。近幾十年來,隨著我國工業(yè)化與城市化進程的日益推進,大氣污染現(xiàn)象呈現(xiàn)出愈發(fā)嚴峻的態(tài)勢。李克強總理在2017年的政府工作報告中特別指出中國目前大氣污染的嚴峻性,亟需加強對大氣灰霾成因與防治措施的研究。因此,對于灰霾的來源及其成因的進一步研究有利于減少大氣污染對于人體健康的影響,這已成為目前一段時期內(nèi)一項極其迫切的任務。目前,已有一些大氣溯源模型可用來解析大氣顆粒物(PM)的來源,但這些方法大多基于多元素濃度信息,需要多種儀器設備才能實現(xiàn),結果爭議也比較大。在本研究中,我們基于硅元素的普遍存在性,利用天然硅穩(wěn)定同位素組成作為一種新的示蹤劑,對大氣PM的來源進行了研究。我們用電感耦合等離子體質(zhì)譜儀(inductively coupled plasma mass spectrometry,ICP-MS))和多接收器電感耦合等離子體質(zhì)譜儀(multicollector inductively coupled plasma mass spectrometry,MC-ICP-MS)等儀器對 2015 年 12月北京地區(qū)不同粒徑的大氣顆粒物樣品(TSP和PM_（2.5）)進行了硅濃度和硅穩(wěn)定同位素組成的測量,并計算出硅比重(硅元素占PM重量的比重)。研究發(fā)現(xiàn),隨著污染程度的增加,PM_（2.5）中硅濃度和硅比重不斷下降,而硅穩(wěn)定同位素卻保持相對穩(wěn)定,既驗證了顆粒物粒徑不斷增大的過程,同時也證明了在灰霾形成的過程中,大氣顆粒物一次來源對灰霾的貢獻比重不斷減小。因此,2015年12月北京地區(qū)大氣顆粒物爆發(fā)性增長,主要來自二次顆粒物的貢獻。
[Abstract]:As the most widely produced and used nanomaterials, the toxicological effects of silica nanoparticles have gradually attracted people's attention. previous studies have pointed out that silica nanoparticles from natural sources and from artificial sources have different toxicological effects. However, at present, there is no method to effectively identify the source of silica nanoparticles. In this paper, the morphology, crystal structure and oxygen-silicon ratio of natural and artificial silica particles have been characterized. Through the determination of a large number of samples, it is found that the distribution range of silicon stable isotopes in silicon dioxide particles from artificial source and natural source is obviously different, and 未 ~ (30) Si (per thousand) can be used as the threshold for distinguishing artificial source from natural source. In addition, the stable isotopic distribution of silicon in silica particles produced by four different manufacturers is narrow and has the characteristics of isotopic fingerprint recognition. It is shown that under certain circumstances, the discrimination of different sources of silicon can be realized by the difference of natural stable isotopes of silicon dioxide particles. From the same factory, the raw materials are the same, and the silicon isotopic distribution of silica nanoparticles with different synthesis processes is also obviously different, which indicates that different synthesis processes result in different degrees of isotopic fractionation, which provides a theoretical basis for identifying different synthesis processes of silica particles by silicon isotope distribution. The experimental results show that silicon stable isotopes can be used as a useful tool to identify the source of silica nanoparticles. In recent decades, with the development of industrialization and urbanization in China, the phenomenon of air pollution is becoming more and more serious. In his 2017 government work report, Premier Li Keqiang pointed out the seriousness of air pollution in China and the urgent need to strengthen the study on the causes and prevention measures of atmospheric haze. Therefore, further study on the source and causes of haze is helpful to reduce the impact of air pollution on human health, which has become an extremely urgent task in a period of time. At present, some atmospheric traceability models can be used to analyze the source of atmospheric particulate matter (PM), but most of these methods are based on multi-element concentration information and need a variety of instruments and equipment to achieve it, and the results are controversial. In this study, based on the universal existence of silicon elements, the source of atmospheric PM was studied by using natural silicon stable isotopic composition as a new tracer. The silicon concentration and stable isotopic composition of atmospheric particulate samples (TSP and PM_) with different particle sizes in Beijing in December 2015 were measured by inductively coupled plasma mass spectrometer (inductively coupled plasma mass spectrometry,ICP-MS) and multi-receiver inductively coupled plasma mass spectrometer (multicollector inductively coupled plasma mass spectrometry,MC-ICP-MS), and the specific gravity of silicon (the proportion of silicon to the weight of PM) was calculated. It is found that with the increase of pollution degree, the concentration of silicon and the specific gravity of silicon in PM_ (2.5) continue to decrease, while the stable isotopes of silicon remain relatively stable, which not only verifies the process of increasing particle size, but also proves that the contribution of atmospheric particles to haze decreases during the formation of haze. Therefore, the explosive growth of atmospheric particles in Beijing in December 2015 mainly comes from the contribution of secondary particles.
【學位授予單位】：山東大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X513
[Abstract]:As the most widely produced and used nanomaterials, the toxicological effects of silica nanoparticles have gradually attracted people's attention. previous studies have pointed out that silica nanoparticles from natural sources and from artificial sources have different toxicological effects. However, at present, there is no method to effectively identify the source of silica nanoparticles. In this paper, the morphology, crystal structure and oxygen-silicon ratio of natural and artificial silica particles have been characterized. Through the determination of a large number of samples, it is found that the distribution range of silicon stable isotopes in silicon dioxide particles from artificial source and natural source is obviously different, and 未 ~ (30) Si (per thousand) can be used as the threshold for distinguishing artificial source from natural source. In addition, the stable isotopic distribution of silicon in silica particles produced by four different manufacturers is narrow and has the characteristics of isotopic fingerprint recognition. It is shown that under certain circumstances, the discrimination of different sources of silicon can be realized by the difference of natural stable isotopes of silicon dioxide particles. From the same factory, the raw materials are the same, and the silicon isotopic distribution of silica nanoparticles with different synthesis processes is also obviously different, which indicates that different synthesis processes result in different degrees of isotopic fractionation, which provides a theoretical basis for identifying different synthesis processes of silica particles by silicon isotope distribution. The experimental results show that silicon stable isotopes can be used as a useful tool to identify the source of silica nanoparticles. In recent decades, with the development of industrialization and urbanization in China, the phenomenon of air pollution is becoming more and more serious. In his 2017 government work report, Premier Li Keqiang pointed out the seriousness of air pollution in China and the urgent need to strengthen the study on the causes and prevention measures of atmospheric haze. Therefore, further study on the source and causes of haze is helpful to reduce the impact of air pollution on human health, which has become an extremely urgent task in a period of time. At present, some atmospheric traceability models can be used to analyze the source of atmospheric particulate matter (PM), but most of these methods are based on multi-element concentration information and need a variety of instruments and equipment to achieve it, and the results are controversial. In this study, based on the universal existence of silicon elements, the source of atmospheric PM was studied by using natural silicon stable isotopic composition as a new tracer. The silicon concentration and stable isotopic composition of atmospheric particulate samples (TSP and PM_) with different particle sizes in Beijing in December 2015 were measured by inductively coupled plasma mass spectrometer (inductively coupled plasma mass spectrometry,ICP-MS) and multi-receiver inductively coupled plasma mass spectrometer (multicollector inductively coupled plasma mass spectrometry,MC-ICP-MS), and the specific gravity of silicon (the proportion of silicon to the weight of PM) was calculated. It is found that with the increase of pollution degree, the concentration of silicon and the specific gravity of silicon in PM_ (2.5) continue to decrease, while the stable isotopes of silicon remain relatively stable, which not only verifies the process of increasing particle size, but also proves that the contribution of atmospheric particles to haze decreases during the formation of haze. Therefore, the explosive growth of atmospheric particles in Beijing in December 2015 mainly comes from the contribution of secondary particles.
【學位授予單位】：山東大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X513
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