【摘要】：氨氣對(duì)環(huán)境大氣、土壤、水體中的氮循環(huán)起關(guān)鍵作用,研究農(nóng)業(yè)面源、工業(yè)點(diǎn)源、機(jī)動(dòng)車(chē)移動(dòng)源這幾類(lèi)排放權(quán)重高、有規(guī)律的人為氨排放源的在線檢測(cè)方法并掌握其排放規(guī)律,對(duì)研究全球氮循環(huán)和環(huán)境保護(hù)具有重要意義。論文針對(duì)氨排放在線檢測(cè)的技術(shù)需求,研究了氨氣高溫特征光譜檢測(cè)方法及濃度精確反演算法,并開(kāi)展區(qū)域型氨排放通量在線檢測(cè)技術(shù)和應(yīng)用研究。研究了氨氣在近紅外波段的振轉(zhuǎn)吸收譜帶和氨的配分函數(shù),分析了6528.8cm-1附近的吸收光譜特性;建立了高溫氨氣近紅外波段激光吸收光譜測(cè)量實(shí)驗(yàn)平臺(tái),開(kāi)展了高溫氨氣特征光譜及線強(qiáng)檢測(cè)實(shí)驗(yàn),獲得了室溫和500～700K不同溫度、不同壓力下氨氣的特征吸收光譜,并分析得到了常溫及高溫環(huán)境的線型和線強(qiáng)參數(shù)。研究了基于高分辨近紅外吸收光譜高溫氨氣濃度反演算法,建立了基于特征光譜解析、多線Voigt線型擬合、溫度參數(shù)修正的高溫氨氣濃度反演算法模型和實(shí)際測(cè)量環(huán)境下的光譜相關(guān)性分析算法,對(duì)多吸收線交疊的線型擬合殘差優(yōu)于±2%,當(dāng)測(cè)量光譜與標(biāo)準(zhǔn)光譜的相關(guān)系數(shù)優(yōu)于85%時(shí)檢測(cè)相對(duì)誤差5%,高溫氨濃度反演的精度約4%。研發(fā)了高溫氨氣在線檢測(cè)系統(tǒng)控制和濃度反演軟件,開(kāi)展了高溫氨逃逸現(xiàn)場(chǎng)在線檢測(cè)實(shí)驗(yàn),測(cè)量結(jié)果表明:脫硝催化還原反應(yīng)氨逃逸與NOx濃度呈現(xiàn)負(fù)相關(guān)特征。采用高溫伴熱尾氣取樣系統(tǒng)開(kāi)展了機(jī)動(dòng)車(chē)尾氣氨氣排放在線檢測(cè)實(shí)驗(yàn),怠速約為800r/min時(shí),氨排放平均濃度約1.64ppm,轉(zhuǎn)速提高到1500r/min時(shí),氨排放平均濃度約為2.24ppm,結(jié)果表明:隨著轉(zhuǎn)速升高,氨氣排放的濃度呈現(xiàn)上升趨勢(shì)。研究了 OP-TDLAS技術(shù)結(jié)合bLS模型進(jìn)行通量監(jiān)測(cè)的有效性和數(shù)據(jù)融合方法,包括細(xì)化儀器架設(shè)光程、高度、數(shù)據(jù)平均周期等實(shí)驗(yàn)條件;優(yōu)化區(qū)域型開(kāi)放式監(jiān)測(cè)方式并進(jìn)行一致性分析。通過(guò)開(kāi)展農(nóng)田、養(yǎng)殖場(chǎng)氨排放監(jiān)測(cè)應(yīng)用研究,獲得安徽皖北地區(qū)秸稈還田和農(nóng)田施肥共同作用下的土壤氨排放規(guī)律,結(jié)果表明施肥對(duì)氨排放的增勢(shì)效應(yīng)更快并且持續(xù)時(shí)間更短,而秸稈還田的增勢(shì)效果更明顯、持續(xù)時(shí)間更長(zhǎng)久。在黃淮海平原開(kāi)展農(nóng)田施肥氨排放監(jiān)測(cè),在施肥后的10天氨揮發(fā)通量較大,峰值達(dá)到5.34 kg N/(hm~2d);開(kāi)展不同季節(jié)典型城市奶牛場(chǎng)氨排放監(jiān)測(cè),秋季氨排放速率為1.48～130.6(kg/head/hr),冬季氨排放速率約為0.0045～43.32(kg/head/hr),排放與溫度、氣象條件有關(guān),體現(xiàn)出季節(jié)性差異。
[Abstract]:Ammonia gas plays a key role in nitrogen cycling in environmental atmosphere, soil and water body. This paper studies the on-line detection methods and the emission rules of agricultural non-point source, industrial point source and motor vehicle moving source, which have high weight and regular artificial ammonia emission source. It is of great significance to study the global nitrogen cycle and environmental protection. In order to meet the technical requirements of on-line detection of ammonia emissions, this paper studies the method of high temperature characteristic spectrum detection of ammonia gas and the accurate inversion algorithm of ammonia concentration, and carries out on-line detection technology and application research of regional ammonia emission flux. The vibrational absorption band of ammonia in near infrared band and the partition function of ammonia are studied, the absorption spectrum characteristics near 6528.8cm-1 are analyzed, and the experimental platform for measuring laser absorption spectrum of high temperature ammonia in near infrared band is established. The characteristic absorption spectra of ammonia at room temperature and 500K at different temperatures and pressures were obtained, and the line shape and line strength parameters of normal temperature and high temperature environment were analyzed. Based on the high resolution near infrared absorption spectrum, the inversion algorithm of ammonia concentration at high temperature is studied. Based on the characteristic spectrum analysis, the multi-line Voigt line fitting is established. The inversion algorithm model of high temperature ammonia concentration modified by temperature parameters and the spectral correlation analysis algorithm under the actual measurement environment, When the correlation coefficient between the measured spectrum and the standard spectrum is better than that of 85, the relative error is 5 and the inversion accuracy of ammonia concentration at high temperature is about 4. The software of high temperature ammonia on-line detection system control and concentration inversion was developed, and the field on-line detection experiment of high temperature ammonia escape was carried out. The results showed that ammonia escape from denitrification catalytic reduction reaction showed a negative correlation with NOx concentration. The on-line detection experiment of ammonia emission from motor vehicle tail gas was carried out by using the high temperature heat tracing tail gas sampling system. When the idle speed was about 800r/min, the average concentration of ammonia emission was about 1.64 ppm, and the average concentration of ammonia emission was about 2.24 ppm when the rotational speed increased to 1500r/min. The results showed that the average concentration of ammonia emission was about 2.24 ppm with the increase of rotational speed. The concentration of ammonia gas emission showed an increasing trend. The effectiveness and data fusion method of OP-TDLAS technology combined with bLS model for flux monitoring are studied, including thinning the experimental conditions of optical path, height and data mean period, optimizing the open monitoring mode and analyzing the consistency. Through the application research of ammonia emission monitoring in farmland and aquaculture farm, the soil ammonia emission law under the joint action of straw returning to field and farmland fertilization in northern Anhui Province was obtained. The results showed that the increasing effect of fertilization on ammonia emission was faster and the duration was shorter. The effect of straw returning to the field is more obvious, and the duration is longer. The ammonia emission monitoring of farmland fertilization was carried out in Huang-Huai-Hai Plain. The ammonia volatilization flux reached 5.34kg / (hm~2d) in 10 days after fertilization, and the ammonia emission monitoring was carried out in typical urban dairy farms in different seasons. The ammonia emission rate in autumn is 1.48 ~ 130.6 (kg/head/hr) and that in winter is about 0.0045 ~ 43.32 (kg/head/hr). The discharge rate is related to temperature and meteorological conditions, showing seasonal difference.
【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：X831;O433

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