復(fù)合材料中工業(yè)納米顆粒的徑流沖刷釋放與機(jī)理
發(fā)布時(shí)間：2018-10-23 12:44
【摘要】：隨著納米技術(shù)的發(fā)展,通過(guò)添加工業(yè)納米顆粒(Engineered nanoparticles,ENPs)的納米復(fù)合材料因其優(yōu)異的性能,生產(chǎn)和使用量迅猛增長(zhǎng)。導(dǎo)致了ENPs不可避免的隨著材料的使用、老化被不斷地釋放至環(huán)境中,使其在水、土壤和大氣中的殘留量逐漸增多,給環(huán)境帶來(lái)了潛在的生態(tài)風(fēng)險(xiǎn)。因此,研究ENPs的釋放方式及環(huán)境行為是非常必要的。本課題通過(guò)實(shí)驗(yàn)室模擬,研究了四種環(huán)境因素(老化時(shí)間、降雨pH、降雨歷時(shí)、降雨強(qiáng)度)對(duì)三種不同涂層中(分別含SiO_2-ENPs,Ag-ENPs和TiO_2-ENPs)ENPs釋放行為的影響。通過(guò)靜態(tài)浸出實(shí)驗(yàn)發(fā)現(xiàn),三種ENPs的釋放濃度均隨著老化時(shí)間的增長(zhǎng)而升高。在較低或較高pH條件下,SiO_2-ENPs,Ag-ENPs的釋放量相對(duì)較大,而TiO_2-ENPs僅在低pH條件下有較大的釋放量。隨著降雨歷時(shí)的增長(zhǎng),SiO_2-ENPs的釋放量逐漸降低,Ag-ENPs的釋放量逐漸升高,TiO_2-ENPs無(wú)明顯規(guī)律。關(guān)于降雨強(qiáng)度對(duì)ENPs釋放的影響,結(jié)果發(fā)現(xiàn)隨著降雨強(qiáng)度的增加,徑流中Si、Ag和Ti的濃度均呈現(xiàn)出升高的趨勢(shì)。總而言之,涂層中Ag-ENPs和TiO_2-ENPs的釋放量相對(duì)較低(ppb級(jí)別),SiO_2-ENPs相對(duì)較高(ppm級(jí)別)。另外,動(dòng)態(tài)光散射檢測(cè)發(fā)現(xiàn)SiO_2-ENPs釋放到環(huán)境當(dāng)中多數(shù)以團(tuán)聚態(tài)的形式存在,只有很少一部分粒徑小于0.1μm。鑒于涂層中SiO_2-ENPs的釋放量相對(duì)較大,本研究還針對(duì)SiO_2-ENPs在環(huán)境中的行為規(guī)律(不同環(huán)境因素對(duì)ENPs的影響)進(jìn)行了研究。實(shí)驗(yàn)過(guò)程中,為了全面和深入地探究ENPs與自然環(huán)境因素的相互作用規(guī)律,主要對(duì)SiO_2-ENPs在不同的鹽離子及有機(jī)質(zhì)溶液中的平均粒徑、表面電位、納米級(jí)別顆粒含量進(jìn)行測(cè)定分析。研究結(jié)果發(fā)現(xiàn),隨著鹽離子強(qiáng)度增加,SiO_2-ENPs團(tuán)聚程度增大,二價(jià)(Ca2+)相對(duì)于單價(jià)離子(Na+)對(duì)SiO_2-ENPs團(tuán)聚有更大的促進(jìn)作用。腐殖質(zhì)(Nature organic matter,NOM;主要包括腐殖酸(Humic acid,HA)和富里酸(Fulvic acid,FA))吸附到SiO_2-ENPs表面,能使SiO_2-ENPs表面攜帶更多的負(fù)電荷,因此顆粒之間靜電斥力增大。另外,研究還發(fā)現(xiàn)SiO_2-ENPs在HA中的粒徑大于FA,這主要跟FA和HA的特性有關(guān)。在Ca2+與NOM的混合溶液中,SiO_2-ENPs的平均粒徑相對(duì)其他溶液更大,原因可能是Ca2+的離子架橋作用(Ca2+-NOM)。至于納米級(jí)別顆粒含量,結(jié)果證實(shí)NOM溶液中納米級(jí)別SiO_2質(zhì)量百分比在高pH條件下大于低pH條件。在鹽離子溶液以及混合液中,納米級(jí)別SiO_2質(zhì)量百分比符合如下規(guī)律:pH7pH9pH5。
[Abstract]:With the development of nanotechnology, the production and usage of nanocomposites with industrial nanoparticles (Engineered nanoparticles,ENPs) are increasing rapidly due to their excellent properties. As a result, ENPs is inevitably released into the environment with the use of materials, resulting in a gradual increase of residues in water, soil and atmosphere, which brings potential ecological risks to the environment. Therefore, it is necessary to study the release mode and environmental behavior of ENPs. The effects of four environmental factors (aging time, rainfall pH, rainfall duration, rainfall intensity) on the ENPs release behavior in three different coatings (including SiO_2-ENPs,Ag-ENPs and TiO_2-ENPs) were studied by laboratory simulation. The static leaching experiments showed that the release concentration of ENPs increased with aging time. Under the condition of lower or higher pH, the release of SiO_2-ENPs,Ag-ENPs was relatively larger, while that of TiO_2-ENPs was only larger under the condition of low pH. With the increase of rainfall duration, the release of SiO_2-ENPs decreased gradually, the release of Ag-ENPs increased gradually, and there was no obvious rule of TiO_2-ENPs. As to the effect of rainfall intensity on the release of ENPs, it is found that the concentration of Si,Ag and Ti in runoff increases with the increase of rainfall intensity. In a word, the release of Ag-ENPs and TiO_2-ENPs in the coating is relatively low (ppb level) and SiO_2-ENPs is relatively high (ppm grade). In addition, dynamic light scattering (DLS) measurements show that most of the SiO_2-ENPs released into the environment exist in the form of agglomeration, and only a few of the particles are less than 0.1 渭 m in size. In view of the relatively large amount of SiO_2-ENPs released in the coating, the behavior of SiO_2-ENPs in the environment (the influence of different environmental factors on ENPs) was also studied. In order to study the interaction between ENPs and natural environment factors, the average particle size, surface potential and nano-particle content of SiO_2-ENPs in different salt ions and organic solution were measured and analyzed. The results show that the degree of SiO_2-ENPs agglomeration increases with the increase of salt ion strength, and the bivalent (Ca2) ion (Na) has a greater effect on SiO_2-ENPs agglomeration than univalent ion (Na). Humus (Nature organic matter,NOM; mainly includes humic acid (Humic acid,HA) and fulvic acid (Fulvic acid,FA) adsorbed on the surface of SiO_2-ENPs, which can make the surface of SiO_2-ENPs carry more negative charges, so the electrostatic repulsion between particles increases. In addition, it is found that the diameter of SiO_2-ENPs in HA is larger than that of FA, which is mainly related to the characteristics of FA and HA. In the mixed solution of Ca2 and NOM, the average particle size of SiO_2-ENPs is larger than that of other solutions, which may be due to the Ca2 NOM). Of Ca2. As for the content of nanoparticles, the results show that the mass percentage of nano-grade SiO_2 in NOM solution is larger than that in low pH solution under the condition of high pH. In salt ion solution and mixed solution, the mass percentage of nanoscale SiO_2 conforms to the following rule: pH7pH9pH5.
【學(xué)位授予單位】：北京建筑大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X132
本文編號(hào)：2289278
[Abstract]:With the development of nanotechnology, the production and usage of nanocomposites with industrial nanoparticles (Engineered nanoparticles,ENPs) are increasing rapidly due to their excellent properties. As a result, ENPs is inevitably released into the environment with the use of materials, resulting in a gradual increase of residues in water, soil and atmosphere, which brings potential ecological risks to the environment. Therefore, it is necessary to study the release mode and environmental behavior of ENPs. The effects of four environmental factors (aging time, rainfall pH, rainfall duration, rainfall intensity) on the ENPs release behavior in three different coatings (including SiO_2-ENPs,Ag-ENPs and TiO_2-ENPs) were studied by laboratory simulation. The static leaching experiments showed that the release concentration of ENPs increased with aging time. Under the condition of lower or higher pH, the release of SiO_2-ENPs,Ag-ENPs was relatively larger, while that of TiO_2-ENPs was only larger under the condition of low pH. With the increase of rainfall duration, the release of SiO_2-ENPs decreased gradually, the release of Ag-ENPs increased gradually, and there was no obvious rule of TiO_2-ENPs. As to the effect of rainfall intensity on the release of ENPs, it is found that the concentration of Si,Ag and Ti in runoff increases with the increase of rainfall intensity. In a word, the release of Ag-ENPs and TiO_2-ENPs in the coating is relatively low (ppb level) and SiO_2-ENPs is relatively high (ppm grade). In addition, dynamic light scattering (DLS) measurements show that most of the SiO_2-ENPs released into the environment exist in the form of agglomeration, and only a few of the particles are less than 0.1 渭 m in size. In view of the relatively large amount of SiO_2-ENPs released in the coating, the behavior of SiO_2-ENPs in the environment (the influence of different environmental factors on ENPs) was also studied. In order to study the interaction between ENPs and natural environment factors, the average particle size, surface potential and nano-particle content of SiO_2-ENPs in different salt ions and organic solution were measured and analyzed. The results show that the degree of SiO_2-ENPs agglomeration increases with the increase of salt ion strength, and the bivalent (Ca2) ion (Na) has a greater effect on SiO_2-ENPs agglomeration than univalent ion (Na). Humus (Nature organic matter,NOM; mainly includes humic acid (Humic acid,HA) and fulvic acid (Fulvic acid,FA) adsorbed on the surface of SiO_2-ENPs, which can make the surface of SiO_2-ENPs carry more negative charges, so the electrostatic repulsion between particles increases. In addition, it is found that the diameter of SiO_2-ENPs in HA is larger than that of FA, which is mainly related to the characteristics of FA and HA. In the mixed solution of Ca2 and NOM, the average particle size of SiO_2-ENPs is larger than that of other solutions, which may be due to the Ca2 NOM). Of Ca2. As for the content of nanoparticles, the results show that the mass percentage of nano-grade SiO_2 in NOM solution is larger than that in low pH solution under the condition of high pH. In salt ion solution and mixed solution, the mass percentage of nanoscale SiO_2 conforms to the following rule: pH7pH9pH5.
【學(xué)位授予單位】：北京建筑大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X132
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