京津冀區(qū)域民用散煤燃燒對(duì)環(huán)境空氣影響的光化學(xué)煙霧箱模擬研究
本文選題:民用散煤 切入點(diǎn):小型室外光化學(xué)煙霧箱 出處:《吉林大學(xué)》2017年碩士論文
【摘要】:我國富煤、貧油、少氣的資源賦存條件決定了煤炭在能源結(jié)構(gòu)中的主導(dǎo)地位,民用散煤燃燒排放的PM_(2.5)是造成當(dāng)前環(huán)境空氣質(zhì)量問題的主要因素之一。本文選用市場上常見的民用爐具和蜂窩煤模擬民用散煤污染源,通過直接測量和統(tǒng)計(jì)平均的方法考察了實(shí)驗(yàn)所采用的充分燃燒狀態(tài)下的NO_x和PM_(2.5)一次排放因子,分別為0.17 kg/t和3×10-3 kg/t。結(jié)合民用型煤使用量的調(diào)研數(shù)據(jù),在本文所模擬的充分燃燒狀態(tài)下,京津冀區(qū)域采暖季民用燃煤源向大氣中直接排放的NO_x和PM_(2.5)分別約為243.29 t和4.29 t。本文使用自主設(shè)計(jì)加工的兩個(gè)平行放置的小型室外光化學(xué)煙霧箱測試了一次污染物在大氣中轉(zhuǎn)化生成二次顆粒物的反應(yīng)特性。其中一個(gè)煙霧箱通入環(huán)境空氣作為背景箱,另一個(gè)引入模擬民用散煤污染源排放的煙氣作為實(shí)驗(yàn)箱,實(shí)驗(yàn)在接近真實(shí)的自然氣象條件下(溫度、相對(duì)濕度、太陽輻射、紫外輻射)進(jìn)行。首先對(duì)所使用的光化學(xué)煙霧箱模擬實(shí)驗(yàn)系統(tǒng)的可靠性進(jìn)行表征,內(nèi)容包括遮光性、密閉性、混合性和壁效應(yīng)性能。表征結(jié)果顯示,遮光狀態(tài)可完全避免環(huán)境紫外線影響,確保實(shí)驗(yàn)初始狀態(tài)的穩(wěn)定性;煙霧箱有效混合時(shí)間3 min,NO_2在實(shí)驗(yàn)箱和背景箱中的半衰期分別是231 h和173.25 h;O_3的半衰期分別是51.31 h和46.20 h,實(shí)驗(yàn)系統(tǒng)滿足二次顆粒物生成模擬實(shí)驗(yàn)的需求。二次顆粒物生成的模擬實(shí)驗(yàn)結(jié)果顯示,即使在冬季北方地區(qū)太陽紫外輻射較弱的情況下,依然可以觀測到明顯的大氣光化學(xué)過程。實(shí)驗(yàn)中測得的最大二次顆粒物生成速率可達(dá)到0.02μg/(m3·s);初始NO_x/VOCs比對(duì)一次污染物的大氣光化學(xué)行為有明顯影響:反應(yīng)處于NO_x控制區(qū)時(shí),NO_x濃度的升高可顯著促進(jìn)光化學(xué)反應(yīng)的進(jìn)行,并觀測到大量二次顆粒物生成和粒徑的增長;反應(yīng)處于VOCs控制區(qū)時(shí),過量的NO_x對(duì)二次污染物(二次顆粒物和臭氧)的生成起到顯著的抑制效果。對(duì)不同實(shí)驗(yàn)過程中顆粒物進(jìn)行分析,結(jié)果表明:顆粒物有機(jī)碳/無機(jī)碳(OC/EC)分析結(jié)果均大于2,并且隨著反應(yīng)的進(jìn)行,OC/EC呈現(xiàn)出持續(xù)增加趨勢;指示氣溶膠老化的鄰苯二甲酸所占比例隨實(shí)驗(yàn)進(jìn)程有增加的趨勢;單顆粒物的粒徑不斷增長,其中的元素也不斷豐富,但即使元素種類不斷增多,C所占的質(zhì)量分?jǐn)?shù)仍然增加,以上實(shí)驗(yàn)結(jié)果均說明實(shí)驗(yàn)箱中的揮發(fā)性有機(jī)物(VOCs)經(jīng)光化學(xué)反應(yīng)生成二次有機(jī)氣溶膠。最后,基于本文得到的二次顆粒物生成速率估算了京津冀區(qū)域民用散煤燃燒排放污染物在大氣中光氧化生成二次顆粒物的環(huán)境影響。實(shí)驗(yàn)所得的二次顆粒物最大生成速率約為0.02μg/(m3·s),計(jì)算得出在實(shí)驗(yàn)燃燒狀態(tài)(充分燃燒)和理想的氣象條件下民用散煤燃燒排放污染物轉(zhuǎn)化生成二次顆粒物的生成因子約為4×10-3 kg/t,京津冀區(qū)域民用散燒煤排放生成的二次顆粒物質(zhì)量約為5.72 t,稍高于本文測量得到一次顆粒物排放量,表明既有的冬季民用散煤排放對(duì)區(qū)域環(huán)境空氣PM_(2.5)污染的貢獻(xiàn)率研究結(jié)果可能嚴(yán)重低估,應(yīng)綜合考慮一次和二次顆粒物的復(fù)合影響。
[Abstract]:The rich coal, oil, and gas resources conditions determine the dominant position of coal in the energy structure, coal combustion emissions of civilian PM_ (2.5) is one of the main factors causing the current ambient air quality problems. This paper selects the common market of domestic stove and honeycomb coal civilian bulk coal pollution source simulation, combustion under the condition of NO_x and PM_ fully employed in the study were investigated by the method of direct measurement and statistical average (2.5) an emission factor, respectively 0.17 kg/t and 3 * 10-3 kg/t. with the survey data of civil coal consumption, full combustion state simulation in this paper, the Beijing Tianjin Hebei region civilian coal-fired heating season the source to the atmospheric emissions of NO_x and PM_ directly (2.5) were approximately two parallel small outdoor smog chamber of 243.29 T and 4.29 T. using self design and processing of a pollutant in atmospheric test The transfer of two generation particle responses. One of the smoke box pass into the air as a background box, another civilian bulk coal into gas simulation pollution as the experimental box, experiments in the natural weather conditions close to the real conditions (temperature, relative humidity, solar radiation, ultraviolet radiation) first. To characterize the photochemical smog box used in the simulation of the reliability of the system, including shading, airtight, mixed and wall effect performance. The results show that shading condition can completely avoid the effects of environmental ultraviolet radiation, to ensure stability of the experimental initial state; effective mixing time 3 min smoke box, the half-life of NO_2 in experiment box and background box are respectively 231 h and 173.25 h respectively; the half-life of O_3 is 51.31 h and 46.20 h, two times to meet the experimental system of particle formation simulation needs. Two particles generated The simulation results show that even in the northern winter solar UV radiation is weak, can still be observed obviously. The maximum photochemical process of two particle formation rate measured in experiments can reach 0.02 g/ (M3 - s); have obvious effects of atmospheric photochemical behavior of initial NO_x/VOCs ratio of primary pollutants the reaction in the NO_x control region, the increase of NO_x concentration can significantly promote the photochemical reaction, and observed a large number of two particle formation and growth of grain size; VOCs reaction in control area, the excess NO_x two times (two times of pollutant particles and ozone generation) plays a significant inhibitory effect for particles of different experimental process were analyzed, the results show that the particulate organic carbon and inorganic carbon (OC/EC) analysis results are greater than 2, and with the reaction, OC/EC showed increasing trend indicating gas; Ortho benzoic acid sol aging two proportion with experimental process had an increasing trend; the single particle size increasing, the elements were enriched, but even if the element type is increasing, C accounts for the mass fraction still increases, above results are that the volatile organic compounds in the experimental box (VOCs the photochemical reaction of two times) organic aerosol. Finally, the two particle formation rate estimated by the Beijing Tianjin Hebei region civilian bulk coal combustion emissions of pollutants in the atmosphere light oxidation two particles. The experimental results based on the environmental impact of the two particle of the maximum production rate is about 0.02 g/ (M3 - s), calculated in the combustion state (combustion) and meteorological conditions under the ideal civilian bulk coal combustion emissions of pollutants into the two particle formation factor is about 4 * 10-3 kg/t, Beijing, Tianjin and Hebei areas With the two particulate mass scattered coal emissions generated is about 5.72 T, slightly higher than the measured primary particulate matter emissions, that the existing civil winter scattered coal emissions on regional air PM_ (2.5) results may seriously underestimate the contribution rate of pollution, should consider the impact of a composite and two secondary particles.
【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】:2017
【分類號(hào)】:X515
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