【摘要】：持久性有機(jī)污染物(POPs)是一類半揮發(fā)、難降解且具有很強(qiáng)親脂憎水性的有機(jī)化合物。這類化合物大多由人類活動(dòng)產(chǎn)生并排放至自然環(huán)境,可在大氣中長(zhǎng)距離遷移導(dǎo)致全球范圍的污染。在主要POPs一次污染源削減和現(xiàn)今全球氣候變化背景下,認(rèn)識(shí)和掌握POPs的二次污染規(guī)律,有助于更客觀理解POPs全球分布現(xiàn)狀和歸趨�！叭蛘麴s模型”一直以來被視為最經(jīng)典的POPs環(huán)境歸趨模型,然而近年來質(zhì)疑該模型的聲音越來越多,季風(fēng)和大氣環(huán)流、降解和生物遷移都是影響POPs環(huán)境命運(yùn)的重要因素。POPs的“森林過濾效應(yīng)”已被廣為接受,但目前相關(guān)研究并不多。全球森林對(duì)于POPs的固定作用及POPs全球傳輸?shù)挠绊懘蠖嘀挥心Ｐ湍M研究,缺乏在林區(qū)的實(shí)測(cè)研究�；赑OPs長(zhǎng)距離傳輸?shù)目赡苄院痛竺娣e森林的可得性,藏東南森林是研究POPs森林過濾效應(yīng)的天然實(shí)驗(yàn)室。因此,本研究工作首先選擇青藏高原東南緣的貢嘎山東坡海螺溝無人區(qū)開展“冷凝捕集效應(yīng)”和“森林過濾效應(yīng)”的對(duì)比研究。通過對(duì)比不同海拔高度、不同環(huán)境介質(zhì)中多氯聯(lián)苯(PCBs)污染水平、組成和空間分布特征,結(jié)合對(duì)環(huán)境參數(shù)(溫度、降雨、土壤有機(jī)碳)的統(tǒng)計(jì)分析,定量獲取兩種效應(yīng)對(duì)PCBs高山富集的貢獻(xiàn)值。結(jié)果表明,貢嘎山東坡土壤中PCBs的組成與分布主要受大氣傳輸和森林土壤有機(jī)碳的影響,土壤有機(jī)碳對(duì)土壤PCBs濃度變化的貢獻(xiàn)率有75%,與由溫度控制的發(fā)生高海拔富集的“全球蒸餾模型”假設(shè)不符,“森林過濾效應(yīng)”在PCBs山地富集中所起的作用較山地“冷凝捕集效應(yīng)”更大,兩種效應(yīng)的平均貢獻(xiàn)率分別為65%和35%。森林過濾效應(yīng)對(duì)不同類別POPs的影響程度可能不同。因此,論文的第二部分,考察了鹵系阻燃劑(HFRs)在貢嘎山東坡土壤的分布情況,利用分子組成比率和氣團(tuán)后向軌跡模型判斷了HFRs的可能來源,并分析了HFRs空間分布的影響因子。結(jié)果表明,貢嘎山東坡森林土壤中可以檢測(cè)出低揮發(fā)性的BDE209和新型溴系阻燃劑(NBFRs)十溴二苯基乙烷(DBDPE)、2-乙基己基-2,3,4,5-四溴苯酸鹽(TBB)、1,2-雙(2,4,6-三溴苯氧基)乙烷(TBE)和氯系阻燃劑德克隆(DP),其中DBDPE在大氣和土壤中的濃度分別達(dá)到171 pg/m3和1450 pg/g干重,是相對(duì)含量最高的單體,NBFRs在HFRs中的比重因此最高。HFRs濃度沿海拔梯度呈整體下降趨勢(shì),BDE47、BDE99和BDE209在山地環(huán)境的遷移能力從高到低依次為BDE47BDE99BDE209,DBDPE濃度沿海拔梯度波動(dòng)較大,推測(cè)其環(huán)境穩(wěn)定性較差。森林土壤的HFRs主要富集在有機(jī)質(zhì)含量高的O層,高山草甸土壤的HFRs在C層的含量最高,可能與高山地表徑流攜帶HFRs從山頂向山腳遷移有關(guān)。HFRs的海拔分布主要受大氣傳輸和人類活動(dòng)遠(yuǎn)近程度影響,與環(huán)境溫度和土壤有機(jī)質(zhì)的相關(guān)性較差。森林過濾效應(yīng)強(qiáng)度與植被覆蓋類型和土壤有機(jī)碳含量密切相關(guān)。然而,在全球氣候變化和人類活動(dòng)雙重壓力下,土地利用/覆蓋類型在時(shí)間和空間尺度發(fā)生快速變化,從而劇烈改變地表覆蓋狀態(tài)和土壤有機(jī)碳儲(chǔ)量。我國(guó)是人工林面積最多的國(guó)家,熱帶地區(qū)天然林向人工林變化情況嚴(yán)峻,其中地力衰退引起的土壤碳流失可能導(dǎo)致“老”POPs的二次遷移。因此,論文的第三部分選取海南島儋州市的蘭洋國(guó)營(yíng)林場(chǎng)開展天然林和人工林土壤富集POPs的比較研究。通過考察不同林型(天然林、橡膠林、桉樹林)和林齡(5齡橡膠、15齡橡膠、25齡橡膠)土壤中POPs的污染水平、組成和空間分布特征,結(jié)合對(duì)土壤理化性質(zhì)(pH、土壤有機(jī)碳、碳氮比)的統(tǒng)計(jì)分析,闡明桉樹和橡膠樹種植對(duì)POPs環(huán)境歸趨的影響。結(jié)果表明,熱帶天然森林對(duì)POPs的持留能力顯著高于熱帶人工林,橡膠林對(duì)POPs的持留能力隨膠林的增加而增加�；谙嚓P(guān)性分析和界面平衡分析,再次強(qiáng)調(diào)土壤有機(jī)碳對(duì)POPs分布的影響,并指出人工林POPs向土壤中的滲濾強(qiáng)度較天然林大。這些新認(rèn)識(shí),有助于更客觀理解POPs全球分布現(xiàn)狀和歸趨。
[Abstract]:Persistent organic pollutants (POPs) are a class of organic compounds that are semi-volatile, difficult to degrade and have very strong lipophilicity. Most of these compounds are produced and discharged to the natural environment by human activities, and long-distance migration in the atmosphere can lead to global pollution. In the context of primary POPs reduction and current global climate change, it is helpful to understand and master the law of secondary pollution of POPs and help to understand the current situation and trend of POPs global distribution more objectively. The "global distillation model" has been regarded as the most classic POPs model, but in recent years it has been questioned that the sound of the model is increasing, and the circulation, degradation and biological migration of the monsoon and the atmosphere are important factors that affect the fate of the POPs. The "forest filtering effect" of POPs has been widely accepted, but the current research is not much relevant. The effect of global forest on the fixed function of POPs and the global transmission of POPs is only a model simulation study, and there is a lack of the actual study in the forest area. Based on the possibility of long-distance transmission of POPs and the availability of large-area forest, the forest in the southeast is the natural laboratory for studying the filtering effect of POPs. Therefore, the research work first selected the comparative study of the "condensation trapping effect" and the "forest filtering effect" in the uninhabited area of the east slope of the Gongga Mountain in the southeast of the Qinghai-Tibet Plateau. By comparing the pollution level, composition and spatial distribution of polychlorinated biphenyls (PCBs) in different environmental media, the contribution of two effects to the high mountain enrichment of PCBs was obtained by statistical analysis of environmental parameters (temperature, rainfall and soil organic carbon). The results show that the composition and distribution of PCBs in the Dongpo soil of Gongga Mountain are mainly influenced by the atmospheric transmission and the organic carbon of the forest, and the contribution rate of soil organic carbon to the change of the concentration of the soil PCBs is 75%, which is not in conformity with the "global distillation model" of the high-altitude enrichment caused by the temperature control. The effect of the "forest filtering effect" on the enrichment of the PCBs in the mountainous region is larger than that of the mountain "condensation trapping effect", and the average contribution rate of the two effects is 65% and 35%, respectively. The effect of forest filtration on different categories of POPs may be different. The second part of the thesis is to study the distribution of the halogen-based flame retardant (HFRs) in the east slope of the Gongga Mountain. The possible sources of the HFRs are determined by the molecular composition ratio and the air mass, and the influence factors of the spatial distribution of the HFRs are also analyzed. The results show that the low-volatility BDE209 and the novel brominated flame retardant (NBFRs) decabromodiphenyl ethane (DBDPE),2-ethylhexyl-2,3,4,5-tetrabromobenzene (TBB), 1,2-bis (2,4,6-tribromophenoxy) ethane (TBE) and chlorine-based flame retardant (DP) can be detected in the forest soil in the east slope of the Gongga Mountain. The concentration of the DBDPE in the atmosphere and the soil reaches 171 pg/ m3 and 1450 pg/ g dry weight, respectively, is the highest relative content, and the specific gravity of the NBFRs in the HFRs is therefore the highest. The concentration of HFRs decreased as a whole along the altitude gradient, and the migration ability of BDE47, BDE99 and BDE209 in the mountain environment was BDE47BDE99BDE209 in order from high to low, and the concentration of DBDPE was large along the altitude gradient, and the environmental stability of BDE47, BDE99 and BDE209 was relatively poor. The HFRs of the forest soil are mainly enriched in the O-layer with high organic matter content. The highest in the C-layer of the high-alpine meadow soil, it is possible to carry the HFRs from the top of the mountain to the mountain-foot migration from the top of the mountain. The altitude distribution of the HFRs is mainly influenced by the atmospheric transmission and the near-far of the human activity, and the correlation between the ambient temperature and the organic matter of the soil is poor. The intensity of the forest filtration effect is closely related to the vegetation cover type and the soil organic carbon content. However, under the dual pressure of global climate change and human activity, the type of land use/ cover changes rapidly in terms of time and space, thus dramatically changing the surface coverage and soil organic carbon reserves. In the country with the largest plantation area, the change of natural forest in the tropics to the plantation is serious, and the loss of soil carbon due to the decline of soil fertility can lead to the secondary migration of the "old" POPs. Therefore, the third part of the thesis is to select the comparative study of the soil-enriched POPs of natural forest and plantation in the Lanyang State-owned Forest Farm in Lanzhou, Hainan, China. The pollution level, composition and spatial distribution of POPs in different forest types (natural forest, rubber forest, eucalyptus forest) and forest age (5-year-old rubber,15-year-old rubber and 25-year-old rubber) were investigated, and the statistical analysis of soil physical and chemical properties (pH, soil organic carbon, carbon-nitrogen ratio) was combined. The effects of the planting of eucalyptus and rubber tree on the environment of the POPs were clarified. The results showed that the retention capacity of the tropical natural forest on the POPs was significantly higher than that of the tropical forest, and the retention capacity of the rubber forest to the POPs was increased with the increase of the rubber forest. Based on the correlation analysis and the analysis of the interface balance, the effect of soil organic carbon on the distribution of POPs is emphasized, and it is pointed out that the percolation intensity of the PPs in the soil is larger than that of the natural forest. These new understandings have contributed to a more objective understanding of the current status and trend of the global distribution of POPs.
【學(xué)位授予單位】：中國(guó)科學(xué)院研究生院(廣州地球化學(xué)研究所)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：X173;X592

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3 梁寶翠;陜西省POPs污染綜合防治對(duì)策研究[D];西北大學(xué);2012年

4 弓俊微;重慶市廢棄殺蟲劑類POPs調(diào)查及前處理方案研究[D];重慶大學(xué);2009年

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7 劉華林;河口持久性有機(jī)污染物（POPs）多介質(zhì)分配特征及影響機(jī)制研究[D];華東師范大學(xué);2005年

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10 吳方國(guó);富營(yíng)養(yǎng)化與POPs協(xié)同關(guān)系的多介質(zhì)環(huán)境化學(xué)模型[D];重慶大學(xué);2004年

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