光腔衰蕩光譜方法探測大氣中氮氧化物
本文選題:光腔衰蕩光譜 + 二氧化氮; 參考:《中國科學(xué)技術(shù)大學(xué)》2017年博士論文
【摘要】:氮氧化物 NO_y,包括 NO_x(NO+NO_2),NO_3,HONO,HNO_3,N2O5,PNs(total peroxy nitrates, RO_2NO_2),ANs (total alkyl nitrates, RONO_2),和 aerosol nitrates等,作為大氣中重要的污染物,對于O_3、OH和HO_2等自由基含量、光化學(xué)煙霧以及二次有機(jī)氣溶膠的形成具有重要的影響。因此,實(shí)現(xiàn)氮氧化物的準(zhǔn)確快速監(jiān)測以及排放監(jiān)管,是目前環(huán)境科學(xué)和大氣化學(xué)重點(diǎn)關(guān)注的課題之一。本論文主要工作為發(fā)展光腔衰蕩光譜(CRDS)方法探測大氣中NO、NO_2、RNO_2(PNs+ANs)、NO_3。第一章主要介紹了相關(guān)大氣化學(xué)的研究背景,NO、NO_2、RNO_2、NO_3參與的大氣化學(xué)過程。簡單分析了這些物質(zhì)在大氣中如何影響大氣組分,改變空氣質(zhì)量的機(jī)制。還介紹了 NO_2的主要測量技術(shù),并分析了各自優(yōu)勢以及局限性。最后,重點(diǎn)介紹了光腔衰蕩光譜技術(shù)的發(fā)展歷程及其測量原理。第二章介紹了基于405 nm半導(dǎo)體激光的雙腔光腔衰蕩光譜系統(tǒng)用于探測NO_2、RNO_2和NO,包括系統(tǒng)的結(jié)構(gòu)、標(biāo)定與檢驗(yàn)。其NO_2的探測靈敏度度可以達(dá)到 0.09 ppbv(1 s)。第三章介紹了基于662 nm半導(dǎo)體激光的NO_3光腔衰蕩光譜系統(tǒng)。其NO_3探測靈敏度達(dá)到了 1 pptv(1 s)。第四章中,我們利用405 nm雙腔光腔衰蕩光譜系統(tǒng)實(shí)現(xiàn)了 NO_2、RNO_2的監(jiān)測,分析了監(jiān)測過程中兩次霧霾事件的可能原因,闡述了 NO_2、RNO_2對二次有機(jī)氣溶膠的產(chǎn)生的影響。我們利用405 nm雙腔光腔衰蕩光譜系統(tǒng),與商用的鉬催化NO_x分析儀對比監(jiān)測大氣中了大氣中的NO_2;評定了鉬催化NO_x分析儀測定大氣中NO_2的偏差大小以及來源。此外,我們分別利用405 nm和662 nm光腔衰蕩光譜系統(tǒng)實(shí)現(xiàn)了對大氣中NO和NO_3的連續(xù)監(jiān)測。第五章對現(xiàn)有實(shí)驗(yàn)的進(jìn)行了總結(jié),并對未來后續(xù)的拓展研究做了分析。
[Abstract]:As important pollutants in the atmosphere, no _ y, including NO_x(NO no _ 2 / no _ 3, HNOS _ 3N _ 2O _ 5 / PNs total peroxy nitrates, RO2NO _ 2 / ANs total alkyl nitrates, etc., have important effects on the free radical contents such as O3OH and HO_2, photochemical smog and the formation of secondary organic aerosols. Therefore, accurate and rapid monitoring of nitrogen oxides and emission regulation is one of the most important issues in environmental science and atmospheric chemistry. The main work of this thesis is to develop the optical cavity ring-down spectroscopy (CRDSs) method for the detection of NONNO2 / RNO2 / PNNs and NO3 in the atmosphere. In the first chapter, the background of atmospheric chemistry is introduced. The mechanism of how these substances affect atmospheric components and change air quality in the atmosphere is briefly analyzed. The main measurement techniques of NO_2 are also introduced, and their advantages and limitations are analyzed. Finally, the development history and measurement principle of cavity ring-down spectroscopy are introduced. In chapter 2, a double-cavity cavity ring-down spectroscopy system based on 405nm semiconductor laser is introduced to detect NO2 / RNO2 and NO2, including the structure, calibration and verification of the system. The detection sensitivity of NO_2 can reach 0.09 ppbv(1 / s. In chapter 3, the NO_3 cavity ring-down spectrum system based on 662nm semiconductor laser is introduced. The sensitivity of NO_3 detection is up to 1 pptv(1 sm. In chapter 4, we use 405nm double-cavity ring-down spectrum system to realize the monitoring of no _ 2O _ 2 / RNO2. The possible causes of two haze events in the monitoring process are analyzed, and the influence of no _ 2O _ 2 RNO2 on the production of secondary organic aerosol is discussed. Using 405nm double-cavity ring-down spectrum system, compared with the commercial molybdenum catalytic NO_x analyzer, the NO2 in the atmosphere was monitored, and the deviation and source of the NO_2 in the atmosphere were evaluated by using the molybdenum catalytic NO_x analyzer. In addition, we have realized the continuous monitoring of no and NO_3 in the atmosphere by using 405nm and 662nm optical cavity ring-down spectroscopy system, respectively. The fifth chapter summarizes the existing experiments and analyzes the future development research.
【學(xué)位授予單位】:中國科學(xué)技術(shù)大學(xué)
【學(xué)位級別】:博士
【學(xué)位授予年份】:2017
【分類號】:O657.3;X831
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