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基于激光吸收光譜的主要人為氨排放源在線檢測技術與應用研究

發(fā)布時間:2018-08-15 15:25
【摘要】:氨氣對環(huán)境大氣、土壤、水體中的氮循環(huán)起關鍵作用,研究農(nóng)業(yè)面源、工業(yè)點源、機動車移動源這幾類排放權重高、有規(guī)律的人為氨排放源的在線檢測方法并掌握其排放規(guī)律,對研究全球氮循環(huán)和環(huán)境保護具有重要意義。論文針對氨排放在線檢測的技術需求,研究了氨氣高溫特征光譜檢測方法及濃度精確反演算法,并開展區(qū)域型氨排放通量在線檢測技術和應用研究。研究了氨氣在近紅外波段的振轉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量實驗平臺,開展了高溫氨氣特征光譜及線強檢測實驗,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際測量環(huán)境下的光譜相關性分析算法,對多吸收線交疊的線型擬合殘差優(yōu)于±2%,當測量光譜與標準光譜的相關系數(shù)優(yōu)于85%時檢測相對誤差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系統(tǒng)控制和濃度反演軟件,開展了高溫氨逃逸現(xiàn)場在線檢測實驗,測量結果表明:脫硝催化還原反應氨逃逸與NOx濃度呈現(xiàn)負相關特征。采用高溫伴熱尾氣取樣系統(tǒng)開展了機動車尾氣氨氣排放在線檢測實驗,怠速約為800r/min時,氨排放平均濃度約1.64ppm,轉速提高到1500r/min時,氨排放平均濃度約為2.24ppm,結果表明:隨著轉速升高,氨氣排放的濃度呈現(xiàn)上升趨勢。研究了 OP-TDLAS技術結合bLS模型進行通量監(jiān)測的有效性和數(shù)據(jù)融合方法,包括細化儀器架設光程、高度、數(shù)據(jù)平均周期等實驗條件;優(yōu)化區(qū)域型開放式監(jiān)測方式并進行一致性分析。通過開展農(nóng)田、養(yǎng)殖場氨排放監(jiān)測應用研究,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,結果表明施肥對氨排放的增勢效應更快并且持續(xù)時間更短,而秸稈還田的增勢效果更明顯、持續(xù)時間更長久。在黃淮海平原開展農(nóng)田施肥氨排放監(jiān)測,在施肥后的10天氨揮發(fā)通量較大,峰值達到5.34 kg N/(hm~2d);開展不同季節(jié)典型城市奶牛場氨排放監(jiān)測,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,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.
【學位授予單位】:中國科學技術大學
【學位級別】:博士
【學位授予年份】:2017
【分類號】:X831;O433

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