本文選題：霧霾 + 顆粒物��； 參考：《中國(guó)科學(xué)院研究生院(地球環(huán)境研究所)》2015年碩士論文

【摘要】：本研究于2013年3月9~12日春季沙塵期間和2013年12月24日~2014年1月27日冬季霧霾期間,在西安市區(qū)分別進(jìn)行TSP離線采集以及PM2.5化學(xué)組分、NH3濃度、CCN分檔活化率的在線觀測(cè),時(shí)間分辨率均為1小時(shí),并檢測(cè)離線樣品的無(wú)機(jī)離子組成、含碳組分及水溶性組分吸濕性。目的在于分析春季沙塵暴和冬季霧霾期間西安大氣顆粒物化學(xué)演化特征,探討硫酸鹽、硝酸鹽、銨鹽及鈉鹽等主要無(wú)機(jī)鹽的來(lái)源、形成機(jī)制及其對(duì)顆粒物吸濕性能的影響。冬季霧霾觀測(cè)期間,PM2.5是影響能見(jiàn)度的主要因素;其中出現(xiàn)重霾天主要是由于除夕凌晨煙花爆竹的大量燃放以及不利于污染物擴(kuò)散的氣象條件造成的,并且還導(dǎo)致重霾天期間Cl 、K+、Mg2+濃度突然增加。而PM2.5中的NO3 、SO42 、NH4+主要是通過(guò)二次轉(zhuǎn)化形成,并呈現(xiàn)出濃度逐漸上升的趨勢(shì)。Na+主要是人為燃燒秸稈等燃料供暖所產(chǎn)生,僅在0.64~1.63μg·m 3范圍內(nèi)上下波動(dòng),無(wú)增加趨勢(shì)。由于NO2 是中間產(chǎn)物不容易積累成高濃度,且氣相中的HNO2非常不穩(wěn)定,所以檢測(cè)到的NO2 濃度非常低。而觀測(cè)期間風(fēng)速很低,無(wú)地面揚(yáng)塵,且Ca2+主要存在于粗顆粒中,因此PM2.5中Ca2+濃度也非常低。NH3濃度在10.7~47.8μg·m 3范圍內(nèi)上下波動(dòng),并且由于NH3主要受人為活動(dòng)影響,而白天人為活動(dòng)頻繁,晚上人為活動(dòng)減少,所以NH3呈現(xiàn)出明顯的晝夜變化特征,即白天上午濃度達(dá)到最高,凌晨左右降到最低。使用ZSR規(guī)則以及簡(jiǎn)化模型分別計(jì)算冬季霧霾期PM2.5吸濕參數(shù)κ的結(jié)果顯示:重霾天PM2.5吸濕參數(shù)(κ=0.36)比輕霾天(κ=0.26)的略高。此外,由于邊界層的晝夜變化以及白天的光化學(xué)反應(yīng),造成吸濕參數(shù)κ呈現(xiàn)出比較明顯的晝夜變化趨勢(shì)。冬季SMPS與CCN聯(lián)用的觀測(cè)結(jié)果,表明顆粒物的粒徑相較于化學(xué)組分對(duì)于其活化成為CCN更重要,以及細(xì)顆粒的吸濕性比粗顆粒較強(qiáng)。春季沙塵期間有兩次沙塵峰值過(guò)境西安,TSP小時(shí)濃度最高分別達(dá)到7527μg·m 3和3200μg·m 3,同期SO42 分別為180μg·m 3和38μg·m 3。沙塵暴初入西安時(shí)NO3 與NH4+濃度較低,其后,二者以1:1的摩爾比同步漸增,至沙塵過(guò)后第48小時(shí)達(dá)最大值(分別為34μg·m 3和8.7μg·m 3)。沙塵期Na+與SO42 、Cl 的相關(guān)系數(shù)為.95,NH4+與NO3 的相關(guān)系數(shù)為0.78,由此推測(cè)他們的來(lái)源相同,是來(lái)源于戈壁上干旱湖泊中的巖鹽、芒硝、石膏和鈣芒硝等礦物;但NH4+和NO3 主要來(lái)源于沙塵顆粒表面的非均相反應(yīng),并以NH4NO3的形式存在。由于TSP樣品水溶性組分中大部分是無(wú)機(jī)離子,因此樣品水溶性組分顯示出一定的吸濕性,整個(gè)觀測(cè)期其吸濕增長(zhǎng)因子變化范圍為1.27~1.44。
[Abstract]:During the spring dust period from March 9 to 12, 2013 and the winter haze from December 24, 2013 to January 27, 2014, the off-line collection of TSP and the on-line observation of the NH _ 3 concentration of the chemical component of PM2.5 and the activation rate of PM2.5 were carried out in Xi'an urban area, respectively.The time resolution was 1 hour, and the moisture absorption of inorganic ions, carbon and water soluble components were detected.The aim of this paper is to analyze the chemical evolution characteristics of atmospheric particulate matter in Xi'an during spring sandstorm and winter haze, and to discuss the source, formation mechanism and effect of sulfate, nitrate, ammonium salt and sodium salt on the moisture absorption of particles.During the winter haze observation, PM2.5 is the main factor affecting visibility. The heavy haze is mainly caused by the massive discharge of fireworks and firecrackers in the early hours of New Year's Eve's morning and the weather conditions that are not conducive to the diffusion of pollutants.It also leads to the sudden increase of Cl ~ (2 +) K ~ (2 +) mg _ (2) concentration during heavy haze days.However, the NH4 in PM2.5 was mainly formed by secondary transformation, and the concentration increased gradually. Na was mainly produced by heating fuel such as burning straw, and only fluctuated in the range of 0.64 ~ 1.63 渭 g / m ~ (3), with no increasing trend.As the intermediate product of NO2 is not easy to accumulate into high concentration, and the HNO2 in gas phase is very unstable, the detected NO2 concentration is very low.However, during the observation period, the wind speed is very low, there is no surface dust, and Ca2 mainly exists in coarse particles. Therefore, the concentration of Ca2 in PM2.5 is very low. NH3 concentration fluctuates in the range of 10.7 ~ 47.8 渭 g / m ~ (3), and NH3 is mainly affected by human activities.But during the day the human activities are frequent and the night human activities decrease so the NH3 shows obvious diurnal variation characteristics namely the highest concentration in the morning and the lowest in the early morning.Using the ZSR rule and the simplified model to calculate the PM2.5 hygroscopicity parameter 魏 in the haze phase in winter, the results showed that the hygroscopic parameters of PM2.5 in heavy haze days (魏 ~ 0.36) were slightly higher than those in light haze days (魏 ~ (26)).In addition, due to the diurnal variation of the boundary layer and the photochemical reaction during the day, the hygroscopic parameter 魏 shows an obvious diurnal variation trend.The observation results of SMPS and CCN in winter show that the particle size is more important than the chemical component in the activation to CCN, and the moisture absorption of fine particles is stronger than that of coarse particles.During spring, the peak concentration of tsp in Xi'an is 7527 渭 g / m ~ (-3) and 3200 渭 g / m ~ (-3), respectively, and SO42 ~ (3) is 180 渭 g / m ~ (-3) and 38 渭 g / m ~ (-3), respectively.The concentrations of NO3 and NH4 were lower at the beginning of dust storm in Xi'an, and then increased at 1:1 molar ratio, and reached their maximum values at 48h after dust dust (34 渭 g / m ~ 3 and 8.7 渭 g / m ~ (3)), respectively.The correlation coefficient between Na and SO42 + Cl ~ (2 +) in sand dust stage is 0.78. The correlation coefficient between Na and NO3 ~ (2 +) is 0.78, which is derived from rock salt, mirabilite, gypsum and glauberite from arid lakes on the Gobi.However, NH4 and NO3 mainly originate from heterogeneous reactions on the surface of dust particles and exist in the form of NH4NO3.Because most of the water-soluble components of TSP samples are inorganic ions, the water-soluble components of TSP samples show a certain moisture absorption, and the range of moisture absorption growth factor is 1.27 ~ 1.44 in the whole observation period.
【學(xué)位授予單位】：中國(guó)科學(xué)院研究生院(地球環(huán)境研究所)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X513

【共引文獻(xiàn)】

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