珠江三角洲地區(qū)臭氧及其前體物非線性響應(yīng)特征及控制對策研究
發(fā)布時間：2019-03-30 20:47
【摘要】：近年來,隨著城市化、工業(yè)化的快速發(fā)展以高濃度臭氧(O3)為特征的光化學(xué)煙霧污染在珠江三角洲地區(qū)(以下簡稱珠三角)時有發(fā)生,臭氧成為該地區(qū)首要污染物的頻率越來越高。由于臭氧與其前體物揮發(fā)性有機物(VOCs)和氮氧化物(NOx)呈顯著的非線性響應(yīng)關(guān)系,且受氣象條件、排放源分布和土地利用類型等影響,臭氧污染仍然是珠三角地區(qū)大氣污染控制研究的重點和難點之一。本研究在本地化模型物種譜建立與對比的基礎(chǔ)上,利用經(jīng)驗動力學(xué)方法(Empirical Kinetics Modeling Approach,EKMA)建立了珠三角典型地區(qū)臭氧及其前體物的非線性響應(yīng)關(guān)系。通過分析臭氧及其前體物關(guān)系特征,識別各典型地區(qū)臭氧生成機制并評估不同前體物削減比例對臭氧控制效果影響,為該區(qū)域臭氧控制政策的制定提供科學(xué)性建議。本論文的主要工作和結(jié)論如下:首先,在道路移動源、工業(yè)有機溶劑使用和非工業(yè)有機溶劑使用源等典型VOCs化學(xué)成分譜實測研究的基礎(chǔ)上,建立了基于大氣模型化學(xué)機理CB05和SAPRC-07的本地化模型物種譜,并與基于USEPA SPECIATE數(shù)據(jù)庫建立的物種譜進行對比分析。結(jié)果顯示:(1)基于SAPRC-07機制建立的本地物種譜與SPECIATE差異較CB05機制明顯;(2)制鞋、家具制造、輕型汽油車和摩托車等本地物種譜與SPECIATE物種化結(jié)果差異較小;(3)印制電路板、輕型柴油車、LPG出租車及非工業(yè)有機溶劑使用源的物種譜差異較為明顯。再者,通過對比驗證本地與SPECIATE模型物種譜對該區(qū)域臭氧模擬效果影響,建立適用于該地區(qū)臭氧特征綜合分析的模擬平臺。結(jié)果表明:基于CB05機制的臭氧模擬結(jié)果與監(jiān)測值吻合度更高;利用本地模型物種譜的模擬平臺更有利于該地區(qū)臭氧高濃度的捕捉。在此基礎(chǔ)上,基于珠三角地區(qū)污染物濃度監(jiān)測值和城市特點、土地利用類型分布、監(jiān)測站點屬性以及前體物削減比例研究等,建立了典型區(qū)域在臭氧日及非臭氧日的臭氧等濃度曲線,探討不同污染時段各典型區(qū)域臭氧及其前體物非線性響應(yīng)關(guān)系。結(jié)果表明:對于典型臭氧污染時段,(1)以廣州和深圳市區(qū)為代表的典型市區(qū)和以東莞、佛山工業(yè)區(qū)為代表的典型工業(yè)區(qū)夏季臭氧受NOx和VOCs共同影響,秋季臭氧則主要受VOC控制;(2)以萬頃沙為代表的典型城郊區(qū)夏季和秋季臭氧均處于VOC控制區(qū);(3)以江門西南部為代表的典型鄉(xiāng)村夏季臭氧生成機制為明顯的NOx控制,秋季臭氧處于過渡區(qū),NOx作用較VOCs顯著。最后,基于各區(qū)域典型污染時段臭氧等濃度曲線,分析了典型的前體物削減比例對臭氧控制效果影響。結(jié)果表明:由于臭氧生成機制具有區(qū)域性和季節(jié)性特征,最佳的前體物削減比例不可一概而論。在本研究中,從理論上講,對于大部分典型區(qū)域而言,VOCs/NOx=1:2和VOCs/NOx=3:1分別為夏季和秋季臭氧較佳前體物削減比例。但綜合控制方案的效果及可行性,VOCs/NOx=1:1可能更適用于珠三角地區(qū)高濃度臭氧污染的控制。
[Abstract]:In recent years, with the urbanization, the rapid development of industrialization characterized by high concentration of ozone (O3) photochemical smog pollution in the Pearl River Delta region (hereinafter referred to as the Pearl River Delta) from time to time. Ozone is becoming the primary pollutant in the region more and more frequently. Ozone has a significant nonlinear response to volatile organic compounds (VOCs) and nitrogen oxides (NOx), and is affected by meteorological conditions, distribution of emission sources and land use types. Ozone pollution is still one of the key and difficult points in the study of air pollution control in Pearl River Delta. Based on the establishment and comparison of localized model species spectra, the nonlinear response relationship of ozone and its precursors in typical Pearl River Delta region was established by using empirical dynamics method (Empirical Kinetics Modeling Approach,EKMA. Based on the analysis of the relationship between ozone and its precursors, the mechanism of ozone generation in typical areas was identified and the effect of different reduction ratios of precursors on ozone control was evaluated, which provided scientific suggestions for the formulation of ozone control policy in this region. The main work and conclusions of this paper are as follows: firstly, based on the measurement of typical VOCs chemical components, such as road moving source, industrial organic solvent use and non-industrial organic solvent usage source, the main results of this paper are as follows: A localized model species spectrum based on atmospheric model chemistry mechanism CB05 and SAPRC-07 was established and compared with the species spectrum based on USEPA SPECIATE database. The results showed that: (1) the difference of local species spectrum based on SAPRC-07 mechanism and SPECIATE mechanism was more obvious than that of CB05 mechanism, (2) the difference of local species spectrum such as shoe making, furniture manufacture, light gasoline truck and motorcycle was less than that of SPECIATE. (3) the species profiles of printed circuit boards, light diesel vehicles, LPG taxis and non-industrial organic solvents were significantly different. Furthermore, the effects of local and SPECIATE model species spectra on ozone simulation in this region are verified and a simulation platform suitable for comprehensive analysis of ozone characteristics in this region is established. The results show that the ozone simulation results based on the CB05 mechanism have a higher degree of coincidence with the monitoring values, and the simulation platform based on the local model species profile is more conducive to the capture of ozone concentration in this area. On this basis, based on the pollutant concentration monitoring values and urban characteristics in the Pearl River Delta region, the distribution of land use types, the attributes of monitoring stations and the reduction ratio of precursors, and so on, The isoconcentration curves of ozone in typical regions on ozone day and non-ozone day were established, and the nonlinear responses of ozone and its precursors in different pollution periods were discussed. The results show that: (1) for the typical ozone pollution period, (1) the typical urban areas represented by Guangzhou and Shenzhen, and the typical industrial zones represented by Dongguan and Foshan industrial zones are affected by NOx and VOCs in summer. In autumn, ozone was mainly controlled by VOC. (2) the ozone in summer and autumn of typical suburban areas, represented by sand of 10,000 hectares, is in the VOC-controlled area; (3) the typical rural ozone generation mechanism represented by south-west of Jiangmen was obviously controlled by NOx in summer. In autumn, ozone was in the transition zone, and the effect of NOx was more significant than that of VOCs. Finally, based on the ozone isoconcentration curve during typical pollution period in each region, the influence of typical precursor reduction ratio on ozone control effect was analyzed. The results show that due to the regional and seasonal characteristics of ozone generation mechanism, the optimal ratio of precursor reduction cannot be generalized. In this study, in theory, for most typical regions, VOCs/NOx=1:2 and VOCs/NOx=3:1 are the better proportion of ozone reduction in summer and autumn, respectively. However, the effect and feasibility of the integrated control scheme, VOCs/NOx=1:1 may be more suitable for the control of high concentration ozone pollution in Pearl River Delta area.
【學(xué)位授予單位】：華南理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X515
本文編號：2450471
[Abstract]:In recent years, with the urbanization, the rapid development of industrialization characterized by high concentration of ozone (O3) photochemical smog pollution in the Pearl River Delta region (hereinafter referred to as the Pearl River Delta) from time to time. Ozone is becoming the primary pollutant in the region more and more frequently. Ozone has a significant nonlinear response to volatile organic compounds (VOCs) and nitrogen oxides (NOx), and is affected by meteorological conditions, distribution of emission sources and land use types. Ozone pollution is still one of the key and difficult points in the study of air pollution control in Pearl River Delta. Based on the establishment and comparison of localized model species spectra, the nonlinear response relationship of ozone and its precursors in typical Pearl River Delta region was established by using empirical dynamics method (Empirical Kinetics Modeling Approach,EKMA. Based on the analysis of the relationship between ozone and its precursors, the mechanism of ozone generation in typical areas was identified and the effect of different reduction ratios of precursors on ozone control was evaluated, which provided scientific suggestions for the formulation of ozone control policy in this region. The main work and conclusions of this paper are as follows: firstly, based on the measurement of typical VOCs chemical components, such as road moving source, industrial organic solvent use and non-industrial organic solvent usage source, the main results of this paper are as follows: A localized model species spectrum based on atmospheric model chemistry mechanism CB05 and SAPRC-07 was established and compared with the species spectrum based on USEPA SPECIATE database. The results showed that: (1) the difference of local species spectrum based on SAPRC-07 mechanism and SPECIATE mechanism was more obvious than that of CB05 mechanism, (2) the difference of local species spectrum such as shoe making, furniture manufacture, light gasoline truck and motorcycle was less than that of SPECIATE. (3) the species profiles of printed circuit boards, light diesel vehicles, LPG taxis and non-industrial organic solvents were significantly different. Furthermore, the effects of local and SPECIATE model species spectra on ozone simulation in this region are verified and a simulation platform suitable for comprehensive analysis of ozone characteristics in this region is established. The results show that the ozone simulation results based on the CB05 mechanism have a higher degree of coincidence with the monitoring values, and the simulation platform based on the local model species profile is more conducive to the capture of ozone concentration in this area. On this basis, based on the pollutant concentration monitoring values and urban characteristics in the Pearl River Delta region, the distribution of land use types, the attributes of monitoring stations and the reduction ratio of precursors, and so on, The isoconcentration curves of ozone in typical regions on ozone day and non-ozone day were established, and the nonlinear responses of ozone and its precursors in different pollution periods were discussed. The results show that: (1) for the typical ozone pollution period, (1) the typical urban areas represented by Guangzhou and Shenzhen, and the typical industrial zones represented by Dongguan and Foshan industrial zones are affected by NOx and VOCs in summer. In autumn, ozone was mainly controlled by VOC. (2) the ozone in summer and autumn of typical suburban areas, represented by sand of 10,000 hectares, is in the VOC-controlled area; (3) the typical rural ozone generation mechanism represented by south-west of Jiangmen was obviously controlled by NOx in summer. In autumn, ozone was in the transition zone, and the effect of NOx was more significant than that of VOCs. Finally, based on the ozone isoconcentration curve during typical pollution period in each region, the influence of typical precursor reduction ratio on ozone control effect was analyzed. The results show that due to the regional and seasonal characteristics of ozone generation mechanism, the optimal ratio of precursor reduction cannot be generalized. In this study, in theory, for most typical regions, VOCs/NOx=1:2 and VOCs/NOx=3:1 are the better proportion of ozone reduction in summer and autumn, respectively. However, the effect and feasibility of the integrated control scheme, VOCs/NOx=1:1 may be more suitable for the control of high concentration ozone pollution in Pearl River Delta area.
【學(xué)位授予單位】：華南理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X515
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