本文關(guān)鍵詞：住宅室內(nèi)降塵中多環(huán)芳烴污染研究與預(yù)警系統(tǒng)構(gòu)建　出處：《重慶大學(xué)》2015年博士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 室內(nèi)環(huán)境 多環(huán)芳烴 風(fēng)險(xiǎn)評價(jià) 特征圖譜 風(fēng)險(xiǎn)預(yù)警

【摘要】：多環(huán)芳烴(Polycyclic aromatic hydrocarbons,簡稱PAHs),是一類典型持久性有機(jī)污染物,是環(huán)境中的重要致癌物質(zhì)之一。PAHs對環(huán)境的污染無處不在,人類已經(jīng)在大氣、水體、土壤、農(nóng)作物、食品等樣品中檢測到了不同種類的PAHs污染物。PAHs污染具有“三大特性”,即:明顯毒性(致癌、致畸、致突變)、長期殘留性和生物蓄積性,因此,PAHs的研究受到了國內(nèi)外政府組織與專家學(xué)者的廣泛關(guān)注。降塵是指在自身重力作用下可以沉降到地面上的顆粒物,它對生態(tài)系統(tǒng)的破壞具有隱蔽性、潛在性和長期性。室內(nèi)降塵作為多種污染物的載體,能直接或間接被人體吸入或攝入,誘發(fā)多種疾病。隨著社會(huì)經(jīng)濟(jì)的不斷發(fā)展,人們對環(huán)境污染的關(guān)注度越來越高,由于人類超過80%的時(shí)間暴露于室內(nèi),室內(nèi)環(huán)境污染方面的研究正日益受到重視,室內(nèi)降塵污染研究也不例外。但是,迄今為止,國內(nèi)外關(guān)于室內(nèi)降塵中PAHs污染方面的研究較少,我國西部地區(qū)由于經(jīng)濟(jì)發(fā)展水平相對落后,對室內(nèi)降塵中PAHs污染研究就更少,甚至處于空白狀態(tài)。自國家確立“西部大開發(fā)”戰(zhàn)略以來,西部地區(qū)的社會(huì)經(jīng)濟(jì)得到了極大的發(fā)展和提升,但隨之而來的環(huán)境污染問題也日益突出。尋找合適的研究載體為突破口,掌握環(huán)境污染的第一手資料和信息,探討其分布規(guī)律與影響因素,構(gòu)建科學(xué)合理的污染預(yù)警系統(tǒng),對協(xié)調(diào)我國西部地區(qū)發(fā)展經(jīng)濟(jì)與環(huán)境保護(hù)之間的關(guān)系,促進(jìn)地方經(jīng)濟(jì)以環(huán)境友好為前提的可持續(xù)發(fā)展和再快速提升發(fā)展具有重要意義。因此,本文針對我國西部地區(qū)室內(nèi)降塵中PAHs研究匱乏的現(xiàn)狀,以西部代表性區(qū)域貴州省為研究示范,開展了室內(nèi)降塵中PAHs的污染現(xiàn)狀、季節(jié)變化、區(qū)域分布規(guī)律、風(fēng)險(xiǎn)特征等研究,并在此基礎(chǔ)上構(gòu)建了基于指紋識別理論的PAHs預(yù)警系統(tǒng),為西部地區(qū)室內(nèi)環(huán)境保護(hù)提供理論依據(jù)和技術(shù)支撐。主要內(nèi)容如下:第一部分,室內(nèi)降塵PAHs污染預(yù)警系統(tǒng)構(gòu)建方法和理論研究。PAHs污染組成復(fù)雜,種類繁多,且目前缺乏能同時(shí)對上百種PAHs污染進(jìn)行監(jiān)控和預(yù)警的方法。為此,本文借鑒指紋識別理論,結(jié)合現(xiàn)代色譜分析技術(shù)和模式識別統(tǒng)計(jì)方法,構(gòu)建基于指紋圖譜技術(shù)的PAHs污染預(yù)警系統(tǒng)的理論框架,以實(shí)現(xiàn)對上百種PAHs污染物的整體監(jiān)控。第二部分,室內(nèi)降塵中代表性PAHs污染物現(xiàn)狀及分布規(guī)律研究。為實(shí)現(xiàn)預(yù)警系統(tǒng)的構(gòu)建,優(yōu)先對當(dāng)前國際上要求嚴(yán)控的18種PAHs進(jìn)行研究,摸清其污染現(xiàn)狀,分析其分布規(guī)律,探討其影響因素,為預(yù)警系統(tǒng)的構(gòu)建提供重要依據(jù)。主要工作如下:首先,完成了18種pahs的高效液相色譜定量分析方法構(gòu)建。18種pahs污染物在0.2-2.0μg范圍內(nèi)線性關(guān)系良好,相關(guān)系數(shù)γ均大于0.9992,檢出限和定量限分別為6.18-12.58ng和20.6-41.93ng;各pahs組分的平均回收率在91.61%-102.81%之間,相對平均標(biāo)準(zhǔn)偏差rsd值為1.06%-3.24%。同時(shí),利用所建立的pahs定量分析方法,對2012-2013年采集的貴州省全部9個(gè)地級行政區(qū)(涉及13個(gè)市縣、22個(gè)鄉(xiāng)鎮(zhèn)和52個(gè)村)的住宅室內(nèi)降塵樣品進(jìn)行測試分析。結(jié)果顯示,貴州室內(nèi)降塵中的Σ18pahs平均含量為1.61μg·g-1,不同行政區(qū)Σ18pahs含量有較大差異;整個(gè)研究區(qū)域pahs污染物種類以高環(huán)(4-6環(huán))pahs為主,尤以phe、flt和pyr為最優(yōu)勢物種。在室內(nèi)降塵中18種pahs污染物特征及現(xiàn)狀分析基礎(chǔ)上,進(jìn)一步對pahs污染的季節(jié)變化和區(qū)域分布特征進(jìn)行研究,為后續(xù)建立pahs污染預(yù)警系統(tǒng)提供基礎(chǔ)數(shù)據(jù)。研究結(jié)果表明:冬季Σ18pahs水平比夏季高,大量燃用煤和生物質(zhì)的季節(jié)性排放是導(dǎo)致室內(nèi)降塵Σ18pahs冬夏濃度出現(xiàn)差異的主要因素;Σ18pahs的行政區(qū)域分布與人口密度的線性相關(guān)系數(shù)為0.91,顯示出人為活動(dòng)帶來的排放是室內(nèi)降塵pahs分布的重要驅(qū)動(dòng)因子。Σ18pahs含量存在顯著的城鄉(xiāng)趨勢,市縣Σ18pahs平均濃度分別是鄉(xiāng)鎮(zhèn)和農(nóng)村的1.6倍和2.7倍,但農(nóng)村地區(qū)面臨發(fā)展經(jīng)濟(jì)和保護(hù)環(huán)境的雙重壓力比城鎮(zhèn)更為嚴(yán)峻。最優(yōu)尺度回歸模型表明:行政區(qū)、城鄉(xiāng)區(qū)域、季節(jié)、采樣樓層、距主干道距離均是影響室內(nèi)降塵Σ18pahs濃度水平的重要因素,且行政區(qū)和城鄉(xiāng)區(qū)域?qū)κ覂?nèi)降塵Σ18pahs濃度的影響最大。第三部分,pahs污染的來源解析及暴露風(fēng)險(xiǎn)評價(jià)。源解析和暴露風(fēng)險(xiǎn)評價(jià)是pahs污染研究的重要組成部分,研究成果可為環(huán)境污染相關(guān)標(biāo)準(zhǔn)的制訂提供理論基礎(chǔ),也為pahs污染預(yù)警系統(tǒng)的構(gòu)建提供重要依據(jù)。本文采用特征化合物法和主成分分析/多元線性回歸法對室內(nèi)降塵中Σ18pahs的來源進(jìn)行解析,結(jié)果表明:室內(nèi)降塵Σ18pahs濃度受室外和室內(nèi)環(huán)境因素的共同影響,其中交通排放和燃煤排放對室內(nèi)降塵Σ18pahs的影響較大;市縣住宅燃煤排放源主要來自室外,而農(nóng)村住宅室內(nèi)環(huán)境中存在直接的煤炭燃燒源,直接向室內(nèi)環(huán)境釋放一定含量的pahs。對住宅室內(nèi)降塵Σ18pahs的健康風(fēng)險(xiǎn)評價(jià)結(jié)果表明:對皮膚接觸和吞食降塵而引起的終生致癌風(fēng)險(xiǎn)(ilcrs),兒童和成人的平均ilcrs均超過了10-7,遠(yuǎn)大于因呼吸攝入引起的致癌風(fēng)險(xiǎn)(平均ilcrs小于10-10)�？偟膩碚f,兒童對室內(nèi)降塵pahs引發(fā)的總致癌風(fēng)險(xiǎn)率要高于成人,且蒙特卡羅不確定性分析結(jié)果表明,兒童對室內(nèi)降塵Σ18pahs污染物的暴露時(shí)間更為敏感。第四部分,室內(nèi)降塵pahs污染預(yù)警系統(tǒng)構(gòu)建及運(yùn)行示范。在前述室內(nèi)降塵pahs污染預(yù)警系統(tǒng)構(gòu)建方法和理論研究基礎(chǔ)上,結(jié)合對18種代表性pahs污染物研究獲得的基礎(chǔ)性數(shù)據(jù)與結(jié)論,以貴州省為示范地點(diǎn),將所建立的pahs預(yù)警理論和方法進(jìn)行了實(shí)踐應(yīng)用。建立了室內(nèi)降塵中PAHs指紋圖譜采集方法;構(gòu)建了貴州地區(qū)特征圖譜庫,獲得了市縣、鄉(xiāng)鎮(zhèn)和農(nóng)村住宅室內(nèi)降塵PAHs污染特征圖譜27幅;成功構(gòu)建了貴州地區(qū)基于指紋識別技術(shù)的室內(nèi)降塵PAHs污染預(yù)警系統(tǒng),該預(yù)警系統(tǒng)由指紋圖譜采集、特征圖譜提取、特征圖譜庫、圖譜匹配處理以及結(jié)果輸出等核心模塊組成。并以貴陽地區(qū)為例,對所建立的PAHs污染預(yù)警系統(tǒng)進(jìn)行運(yùn)行示范研究,通過采集實(shí)時(shí)樣品,分析貴陽地區(qū)室內(nèi)降塵中PAHs的實(shí)時(shí)污染狀況,預(yù)測了其污染趨勢,驗(yàn)證了本文所建立的預(yù)警系統(tǒng)能夠?qū)崿F(xiàn)對室內(nèi)降塵中上百種PAHs的整體監(jiān)控和預(yù)警。
[Abstract]:Polycyclic aromatic hydrocarbons (Polycyclic aromatic hydrocarbons, referred to as PAHs), is a kind of typical persistent organic pollutants, is an important one of the carcinogens in the environment of.PAHs pollution everywhere on the environment, human beings have in the atmosphere, water, soil, crops and food samples were detected in different types of PAHs.PAHs with "three pollution pollutants namely: characteristics, toxicity (carcinogenic, teratogenic, mutagenic), environmental persistence, bioaccumulation, therefore, the research of PAHs has attracted extensive attention of the government organization and domestic experts and scholars. The dust is under its own gravity can settle to particles on the ground, its damage to the ecological the system has a hidden, potential and long-term indoor dust. As a carrier of various pollutants, which can directly or indirectly be inhaled or ingested, cause a variety of diseases. With the continuous development of social economy, The environmental pollution has been paid more and more attention, because more than 80% of human exposure to indoor environmental pollution, indoor research is more and more attention, research on reducing indoor dust pollution is no exception. However, so far, the domestic and foreign research on indoor PAHs pollution in reducing dust less, because the level of economic development the relatively backward western region of our country, dust pollution of PAHs is less on the interior, even in a blank state. Since the establishment of the "western development" strategy, the western region's social economy has been greatly developed and improved, but the attendant environmental problems have become increasingly prominent. Research on finding suitable vector as a breakthrough environmental pollution, master first-hand data and information, the distribution regularity and influence factors, construction of pollution warning system is scientific and reasonable coordination of western region development in China The relationship between the economy and environmental protection, promote the sustainable development of the local economy in the premise of environmental friendly and has important significance to enhance the rapid development. Therefore, according to the interior in the western area of China reduced the current status of the dust in PAHs research is scarce, in the western representative areas of Guizhou Province as the research model, the pollution situation, carry out indoor drop the dust PAHs seasonal changes, regional distribution of risk characteristics, and on the basis of constructing the PAHs warning system based on fingerprint identification theory, provide theoretical basis and technical support for the protection of the indoor environment in the western region. The main contents are as follows: the first part, the indoor dust pollution warning system PAHs construction method and theory research.PAHs the pollution of complex composition, variety, and the current lack of methods for simultaneous monitoring and early warning of hundreds of PAHs pollution. Therefore, based on fingerprint recognition theory, Combined with the analysis of technology and statistical pattern recognition method of modern chromatography, constructs the theoretical framework of PAHs pollution warning system based on fingerprint technology, based on hundreds of PAHs pollutants overall monitoring. The second part of the status and distribution of PAHs indoor pollutants reduction law research on behalf of dust. For construction of early warning system, research the priority of 18 PAHs on the current international strict control, to find out the pollution situation, analyze the distribution, to explore its influencing factors, provide an important basis for the construction of the early warning system. The main work is as follows: first, finished 18 PAHs quantitative high performance liquid chromatography analysis method to construct the.18 PAHs pollutants in 0.2-2.0 g good linear range, correlation coefficient r was greater than 0.9992, and quantification limit of detection were 6.18-12.58ng and 20.6-41.93ng; the PAHs component of the average recovery rate was 91.61% -102.81% The relative standard deviation, average RSD value of 1.06%-3.24%. at the same time, by using the PAHs analysis method based on quantitative, 2012-2013 years collected in Guizhou province all 9 prefecture level administrative region (involving 13 counties, 22 towns and 52 villages) were tested and analyzed the indoor dust samples. The results showed that the average content of sigma 18pahs in Dustfall of Guizhou chamber of 1.61 G - g-1, there is great difference in different administrative region 18pahs content; the entire study area of PAHs pollutants with high ring (4-6 rings) PAHs, especially Phe, FLT and Pyr were the most dominant species. In the indoor 18 characteristics and the current situation of PAHs pollutants analysis in the dust, the further research of PAHs pollution seasonal changes and regional distribution, to provide the basic data for the subsequent establishment of PAHs pollution warning system. The results show that: Sigma 18pahs level was higher than that in summer winter, seasonal discharge burning a lot of coal and biomass Let is the cause of dust concentration in winter 18pahs sigma factors difference; linear correlation coefficient of the administrative area of distribution and population density of sigma 18pahs was 0.91, showing human activities bring dust emission is an important driving factor of PAHs distribution. There is a significant trend in urban and rural areas the total 18pahs content, and the average concentration of 18pahs sigma are 1.6 times and 2.7 times of the towns and rural areas, but rural areas face the dual pressures of economic development and protect the environment than in cities is more severe. The optimal scale regression model showed that the administrative region, urban and rural areas, seasons, sampling floors, the main road distance is an important factor affecting the dust concentration level of 18pahs the influence and the administrative region and urban and rural areas of dust total 18pahs concentration maximum. In the third part, the source apportionment of PAHs pollution and risk assessment. Source apportionment and exposure risk assessment is PAHs. An important part of the dye, provide theoretical basis for the research results of environmental pollution related standards, but also provide an important basis for the construction of PAHs pollution warning system. This paper uses the analysis / characteristic compound method and principal component analysis, the source of dust on the indoor 18pahs multivariate linear regression method. The results showed that the influence of dust total 18pahs concentration by outdoor and indoor environmental factors, which affect the traffic emissions and emissions of coal dust 18pahs; and residential coal emissions are mainly sourced from the outside, while the rural living existence of coal combustion source directly home indoor environment, health risk assessment of the release of certain content directly to the indoor environment pahs. of residential indoor dust Sigma 18pahs results indicated that the skin contact and ingestion of dust caused by cancer risk (ilcrs), the average ilcrs of children and adults are More than 10-7, far greater than the intake of carcinogenic risk caused by breathing (average ilcrs less than 10-10). In general, children of dust caused by PAHs the total cancer risk rate is higher than that of adults, and Monte Carlo uncertainty analysis results show that the exposure time of children's indoor dust pollution is more sensitive to 18pahs fourth. Part of indoor construction dust reduction PAHs pollution early warning system and operation demonstration. In the indoor drop foundation method and theoretical research on the construction of PAHs dust pollution warning system, combined with the basic number of research on 18 typical PAHs pollutants and according to the conclusion, taking Guizhou Province as demonstration sites, the PAHs early warning theory and method of application. Established PAHs fingerprint collecting dust reduction method for indoor; construction of Guizhou area characteristic map database, obtained the counties, towns and rural residential indoor dust pollution characteristics of PAHs 27 patterns; the successful construction of the Guizhou area of fingerprint recognition technology based on PAHs indoor dust pollution warning system, the warning system consists of fingerprint acquisition, fingerprint feature extraction, map database, map matching processing and result output module. The core and takes Guiyang as an example, to run the demonstration research on PAHs pollution warning this system, by collecting samples in real time, real-time analysis of pollution condition of Guiyang area dust in PAHs, predicts the trend of the pollution, the overall monitoring and early warning warning system to verify the proposed in this paper can realize the reduction of hundreds of PAHs dust on the indoor.

【學(xué)位授予單位】：重慶大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2015
【分類號】：X51;TU834.6

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