腐植酸作用下γ-HCH在冰和雪中的光轉(zhuǎn)化
發(fā)布時(shí)間：2018-07-25 11:05
【摘要】：光化學(xué)反應(yīng)是有機(jī)污染物在環(huán)境中遷移轉(zhuǎn)化的重要途徑之一。腐植酸作為天然光敏劑能夠促進(jìn)有機(jī)污染物發(fā)生間接光轉(zhuǎn)化反應(yīng),對(duì)于有機(jī)污染物的遷移、轉(zhuǎn)化和歸宿都有著非常重要的影響。同時(shí)在全球氣候作用下,冰雪已經(jīng)成為持續(xù)性有機(jī)污染物的重要積累場(chǎng)所,冰雪中的持久性有機(jī)污染物及其降解產(chǎn)生的二次污染物已對(duì)冰雪覆蓋地區(qū)環(huán)境產(chǎn)生了重要影響。因此,對(duì)于腐植酸存在下冰雪中有機(jī)污染物光化學(xué)反應(yīng)的研究至關(guān)重要。本文擬通過添加腐植酸(Humic Acid,簡(jiǎn)稱HA),選取典型有機(jī)氯農(nóng)藥γ-Hexachlorocyclohexane(簡(jiǎn)稱γ-HCH)為目標(biāo)污染物,選用80 W高壓汞燈作為光源(λ(?)280 nm),研究HA存在情況下冰雪體系中有機(jī)污染物的光轉(zhuǎn)化規(guī)律,進(jìn)一步揭示環(huán)境中有機(jī)污染物在自然冰雪環(huán)境中的遷移轉(zhuǎn)化機(jī)制,為溫帶及寒帶地區(qū)污染控制對(duì)策的制定提供理論依據(jù)。研究結(jié)果表明： (1)水、冰以及雪中γ-HCH的光轉(zhuǎn)化率：雪冰相水相。這是由于在冰相中存在冷凍濃縮效應(yīng)及在結(jié)冰過程中溶解氧對(duì)γ-HCH的抑制作用減緩,使得冰中γ-HCH的光轉(zhuǎn)化率大于水中；雪中γ-HCH的光轉(zhuǎn)化率大于冰中是由于雪擁有更大的比表面積以及類似液體層(LLL層)。 (2)研究了冰相中γ-HCH初始濃度、HA濃度、鹽離子濃度、pH、Fe3+、NO2及N03-、比表面積對(duì)γ-HCH的光轉(zhuǎn)化率的影響。γ-HCH初始濃度、HA濃度對(duì)γ-HCH的光轉(zhuǎn)化率呈現(xiàn)低濃度促進(jìn)、高濃度抑制的現(xiàn)象；鹽離子濃度、pH、Fe3+、NO2及N03-、比表面積對(duì)γ-HCH的光轉(zhuǎn)化率均有促進(jìn)作用。(3)研究了雪中鹽離子濃度、pH、Fe3+對(duì)γ-HCH的光轉(zhuǎn)化率的影響。與冰相中鹽離子濃度對(duì)γ-HCH光轉(zhuǎn)化率的影響相比,雪中鹽離子濃度對(duì)γ-HCH光轉(zhuǎn)化率影響較小,這主要是由于雪中的LLL層要比冰中的LLL層厚,已經(jīng)有足夠的γ-HCH進(jìn)入到LLL層中,不會(huì)帶來γ-HCH光轉(zhuǎn)化率發(fā)生更大的變化；pH對(duì)γ-HCH光轉(zhuǎn)化率的影響結(jié)果與冰中所得的結(jié)果相似；Fe3+低濃度時(shí)就出現(xiàn)了抑制現(xiàn)象,這可能是由于γ-HCH在雪中的光轉(zhuǎn)化反應(yīng)比冰中的反應(yīng)要快,對(duì)于Fe3+抑制性的響應(yīng)也要更加靈敏。(4)冰相中HA通過產(chǎn)生單線態(tài)氧(1O2)、羥基自由基(·OH)及三重激發(fā)態(tài)(HA*)加速γ-HCH的光轉(zhuǎn)化。 (5)自然光照下,冰樣中γ-HCH的光轉(zhuǎn)化率和實(shí)驗(yàn)室模擬光照下γ-HCH的光轉(zhuǎn)化率基本保持一致,然而,雪樣中γ-HCH的光轉(zhuǎn)化率要比實(shí)驗(yàn)室模擬光照下γ-HCH的光轉(zhuǎn)化率低。 (6)HA存在下γ-HCH的光轉(zhuǎn)化產(chǎn)物主要是五氯環(huán)己烯、鄰二氯苯和間二氯苯、一氯苯,光轉(zhuǎn)化過程中1O2通過消耗中間產(chǎn)物間接加速了γ-HCH的光轉(zhuǎn)化過程。
[Abstract]:Photochemical reaction is one of the important ways to transfer and transform organic pollutants in the environment. Humic acid, as a natural Guang Min agent, can promote the indirect photoconversion of organic pollutants and play an important role in the migration, transformation and fate of organic pollutants. At the same time, under the action of global climate, ice and snow has become an important accumulation of persistent organic pollutants, the persistent organic pollutants in snow and ice and the secondary pollutants produced by their degradation have had an important impact on the environment of snow and ice covered areas. Therefore, it is very important to study the photochemical reaction of organic pollutants in ice and snow in the presence of humic acid. In this paper, a typical organochlorine pesticide 緯 -Hexachlorocyclohexane (緯 -HCH) was selected as the target pollutant by adding humic acid (Humic Acid, for short, and 80 W high pressure mercury lamp was chosen as the light source (位 280 nm),) to study the phototransformation of organic pollutants in ice and snow system in the presence of HA. The migration and transformation mechanism of organic pollutants in the natural ice and snow environment is further revealed, which provides a theoretical basis for the formulation of pollution control measures in temperate and cold regions. The results show that: (1) the light conversion of 緯 -HCH in water, ice and snow: the water phase of snow ice. This is due to the freezing concentration effect in ice phase and the inhibition of dissolved oxygen on 緯 -HCH in ice, which makes the light conversion rate of 緯 -HCH in ice larger than that in water. The light conversion of 緯 -HCH in snow is higher than that in ice because the snow has a larger specific surface area and similar liquid layer (LLL layer). (2) the effects of the initial concentration of 緯 -HCH in ice phase, the concentration of HA, the concentration of salt ion, the pH of Fe _ 3O _ 2 and N _ 03-and the specific surface area on the photoconversion rate of 緯 -HCH were studied. The initial concentration of 緯 -HCH and HA concentration increased the photoconversion rate of 緯 -HCH at low concentration and inhibited it at high concentration; The effect of salt ion concentration (pH = Fe _ 3O _ 2 and N _ 03-H _ 2O _ 3) and specific surface area on the photoconversion of 緯 -HCH was studied. (3) the effect of salt ion concentration (pH = Fe _ 3) on the photoconversion of 緯 -HCH was studied. Compared with the effect of salt ion concentration in ice phase on the light conversion of 緯 -HCH, the effect of salt ion concentration in snow on the light conversion of 緯 -HCH is less, which is mainly due to the fact that the LLL layer in snow is thicker than the LLL layer in ice, and enough 緯 -HCH has already entered the LLL layer. The effect of pH on the light conversion rate of 緯 -HCH is similar to that obtained in ice. This may be due to the fact that the photoconversion of 緯 -HCH in snow is faster than that in ice, and the response to the inhibition of Fe3 is more sensitive. (4) HA in ice phase accelerates the photoconversion of 緯 -HCH by producing monolinear oxygen (1O2), hydroxyl radical (OH) and triple excited state (HA*). (5) the light conversion rate of 緯 -HCH in ice samples was basically the same as that of 緯 -HCH under simulated light. However, the light conversion rate of 緯 -HCH in snow samples was lower than that in simulated illumination in laboratory. (6) in the presence of HA, the photoconversion products of 緯 -HCH were mainly pentachlorocyclohexene, o-dichlorobenzene and m-dichlorobenzene, and monochlorobenzene. 1O2 indirectly accelerated the photoconversion process of 緯 -HCH by consuming intermediate products.
【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X131
本文編號(hào)：2143633
[Abstract]:Photochemical reaction is one of the important ways to transfer and transform organic pollutants in the environment. Humic acid, as a natural Guang Min agent, can promote the indirect photoconversion of organic pollutants and play an important role in the migration, transformation and fate of organic pollutants. At the same time, under the action of global climate, ice and snow has become an important accumulation of persistent organic pollutants, the persistent organic pollutants in snow and ice and the secondary pollutants produced by their degradation have had an important impact on the environment of snow and ice covered areas. Therefore, it is very important to study the photochemical reaction of organic pollutants in ice and snow in the presence of humic acid. In this paper, a typical organochlorine pesticide 緯 -Hexachlorocyclohexane (緯 -HCH) was selected as the target pollutant by adding humic acid (Humic Acid, for short, and 80 W high pressure mercury lamp was chosen as the light source (位 280 nm),) to study the phototransformation of organic pollutants in ice and snow system in the presence of HA. The migration and transformation mechanism of organic pollutants in the natural ice and snow environment is further revealed, which provides a theoretical basis for the formulation of pollution control measures in temperate and cold regions. The results show that: (1) the light conversion of 緯 -HCH in water, ice and snow: the water phase of snow ice. This is due to the freezing concentration effect in ice phase and the inhibition of dissolved oxygen on 緯 -HCH in ice, which makes the light conversion rate of 緯 -HCH in ice larger than that in water. The light conversion of 緯 -HCH in snow is higher than that in ice because the snow has a larger specific surface area and similar liquid layer (LLL layer). (2) the effects of the initial concentration of 緯 -HCH in ice phase, the concentration of HA, the concentration of salt ion, the pH of Fe _ 3O _ 2 and N _ 03-and the specific surface area on the photoconversion rate of 緯 -HCH were studied. The initial concentration of 緯 -HCH and HA concentration increased the photoconversion rate of 緯 -HCH at low concentration and inhibited it at high concentration; The effect of salt ion concentration (pH = Fe _ 3O _ 2 and N _ 03-H _ 2O _ 3) and specific surface area on the photoconversion of 緯 -HCH was studied. (3) the effect of salt ion concentration (pH = Fe _ 3) on the photoconversion of 緯 -HCH was studied. Compared with the effect of salt ion concentration in ice phase on the light conversion of 緯 -HCH, the effect of salt ion concentration in snow on the light conversion of 緯 -HCH is less, which is mainly due to the fact that the LLL layer in snow is thicker than the LLL layer in ice, and enough 緯 -HCH has already entered the LLL layer. The effect of pH on the light conversion rate of 緯 -HCH is similar to that obtained in ice. This may be due to the fact that the photoconversion of 緯 -HCH in snow is faster than that in ice, and the response to the inhibition of Fe3 is more sensitive. (4) HA in ice phase accelerates the photoconversion of 緯 -HCH by producing monolinear oxygen (1O2), hydroxyl radical (OH) and triple excited state (HA*). (5) the light conversion rate of 緯 -HCH in ice samples was basically the same as that of 緯 -HCH under simulated light. However, the light conversion rate of 緯 -HCH in snow samples was lower than that in simulated illumination in laboratory. (6) in the presence of HA, the photoconversion products of 緯 -HCH were mainly pentachlorocyclohexene, o-dichlorobenzene and m-dichlorobenzene, and monochlorobenzene. 1O2 indirectly accelerated the photoconversion process of 緯 -HCH by consuming intermediate products.
【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X131
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