北京地区大气有机物对臭氧生成的影响研究
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摘要
根据北京地区主要大气环流形式和大气污染源分布状况，沿北京地区污染物主要输送路径布置监测站点，于2007年6～9月开展了一次相对系统的北京地区臭氧光化学外场强化观测试验。以该试验的观测资料为基础，通过数据分析、光化学箱模式模拟、三维气象化学模式模拟以及排放清单估算等方法，采用递进式的研究方式（总VOCs—分类VOCs—物种化VOCs）逐步细致的开展了北京地区大气VOCs反应活性及其对O_3生成的影响研究，建立了北京地区物种化VOCs排放清单并初步应用。得到主要结论如下：①通过对地面实测资料的分析揭示了北京城、郊O_3及其前体物浓度的分布状况，结果显示：烷烃在北京城、郊大气总VOCs中占有绝大部分浓度比例，其余物种依次为芳香烃、烯烃及生物VOCs；城郊对比结果表明，城区站各类VOCs物种环境浓度均高于本底站，但本底地区生物VOCs物种在总VOCs中的比例较城市地区偏高；②利用光化学箱模式，模拟采用输入实测资料的约束计算方式，估算了O_3化学生成过程的关键参量O_3生成速率G(O_3)和O_3生成效率OPE，并研究了OPE与NOx浓度变化的关系，分析结果表明：北京城市地区O_3生成受VOCs控制，区域本底地区O_3生成受VOCs及NOx的交替控制；③在箱模式定性研究结果的基础上，进一步利用三维区域化学输送模式WRF-Chem，对北京地区典型区域光化学污染过程进行了模拟研究，模拟结果进一步验证了O_3生成受VOCs控制的结论，显示北京地区地面O_3的生成主要受烯烃类VOCs排放的影响；④估算环境浓度VOCs物种的OH自由基消耗速率(LiOH)及O_3生成潜势(OFP)，结果显示对北京地区OH自由基消耗的主要环境VOCs组分是烯烃类物质，对O_3生成潜势贡献最高的环境VOCs组分是芳香烃类物质；综合LiOH及OFP值评价，识别影响北京地区O_3生成的关键环境VOCs反应活性物种为二甲苯、甲苯、三甲基苯、丙烯、异戊二烯以及丁烯类物质；⑤进一步利用VOCs物种排放量估算各物种的O_3生成潜势，研究结果显示：烯烃类VOCs物种对北京地区总OFP的贡献率最高；对北京地区O_3生成潜势贡献最大的前10个VOCs物种依次为乙烯、间/对-二甲苯、甲苯、1-丁烯、异戊烷、反-2-丁烯、丙烯、顺-2-丁烯、邻-二甲苯和乙炔，这10个物种的累计排放量占VOCs排放总量的60%左右，但对总OFP值的贡献率接近80%；北京城区是VOCs排放的重点区域，同时也是O_3生成潜势最大的区域；降低交通排放、溶剂挥发及油品挥发排放是降低北京地区VOCs排放、控制O_3生成的有效途径；⑥针对北京城、郊O_3形成过程的对比研究表明，城市地区O_3的形成主要源于人为源排放引发的局地光化学生成过程，而生物源排放及污染物的远距离传输在本底地区OH自由基消耗及O_3形成过程中起到十分重要的作用。
Sea-land and mount-valley circulations are the dominant mesoscale synoptic systemsaffecting the Beijing area. Under the influence of these two circulations, the prevailing windis southwesterly from afternoon to midnight, and then changes to northeasterly till forenoon.This prevailing wind pattern can affect the pollutants’ regional distribution significantly.According to the survey on the above meteorological background and regional pollutantsource distribution character, a relatively systematic and intensive field experiment on ozonephotochemical pollution in Beijing area was carried out from June to September2007.Surface ozone and its precursors’ concentrations were measured at four stations, which arelocated along the route of prevalent wind. Based on the observed data from field experiment,as well as photochemical box model and3-D regional chemical and transport modelsimulations, the effect of VOCs on the formation of ozone in Beijing area was investigated byclassifying the VOCs progressively (from total VOCs to classified VOCs, and to speciatedVOC). An emission inventory of speciated VOCs emitted from main anthropogenic sources ofBeijing was developed and applied. Main conclusions of this thesis include：①Due to thehigh traffic density and local emissions, the average levels of reactive VOCs at the urban siteswere much higher than those at the SDZ regional background site. Alkanes were the primarycomponents of VOCs in Beijuing area, followed by aromatics, alkenes and biogenic VOCs.Alkanes, alkenes, aromatics and biogenic VOCs all had much higher ambient concentrationsat the urban site than those at the rural site, while the percentage of biogenic VOCs to totalVOCs was higher at the rural site than that at the urban site.②The gross ozone productionrate G(O_3) and ozone production efficiency (OPE) have been calculated with a photochemicalbox model constrained by observed data, and the relationship between OPE and NOxconcentration was also analyzed. Results showed that photochemical ozone productionprocess is mainly sensitive to VOCs at urban area. In the background area, the productionprocess is sensitive to VOCs and NOxalternatively.③A3-D regional chemical and transportmodel WRF-Chem was used to simulate the typical regional photochemical pollutionprocesses in Beijing area. Simulated results showed that the ozone formation is controlled bythe alkenes emissions in the urban area. Reducing the emissions of alkenes can decrease O_3concentration efficiently in urban area, and this also affects the concentration level of ozone inbackground area.④Alkenes make a major contribution to the LOH, aromatics dominate OFP atboth urban and rural sites. According to the OH loss rate coefficient (LiOH) and the ozoneformation potential (OFP) estimated from the observed ambient mixing ratios of speciatedVOCs, key reactivie species for the ozone formation in Beijing area were recognized. They are m,p-xylene, toluene, trimethyl benzene, propylene, isoprene and butenes. Compared to thethe urban area, biogenic emission and the regional transport have a large influence on OHradicals and the ozone formation in the regional background area.⑤An emission inventoryof speciated VOCs emitted from main anthropogenic sources of Beijing in2003and2006wasdeveloped, and the ozone formation potential (OFP) of VOCs was estimated. Alkenes make amajor contribution to OFP. The top10species, in terms of OFP, consist of ethylene,m,p-xylene, toluene,1-butene, i-pentane, trans-2-butene, propene, cis-2-butene, o-xylene, andacetylene. These species contribute about60%to the total VOC emissions but account for80%of the OFPs in the region. Both high VOC emissions and OFP values appear in the urbanarea of Beijing. Decreasing the traffic exhaust, solvent volatilization and gasoline evaporationwill be the most effective way to reduce VOC emissions and control ozone formation inBeijing area.⑥Local photochemistry played adominant role in ozone formation at urbansite, while biogenic VOCs emissions and long range transportation by urban plume made agreater percentage contribution to OH radical consumption and ozone creation at the ruralsite.
Sea-land and mount-valley circulations are the dominant mesoscale synoptic systemsaffecting the Beijing area. Under the influence of these two circulations, the prevailing windis southwesterly from afternoon to midnight, and then changes to northeasterly till forenoon.This prevailing wind pattern can affect the pollutants’ regional distribution significantly.According to the survey on the above meteorological background and regional pollutantsource distribution character, a relatively systematic and intensive field experiment on ozonephotochemical pollution in Beijing area was carried out from June to September2007.Surface ozone and its precursors’ concentrations were measured at four stations, which arelocated along the route of prevalent wind. Based on the observed data from field experiment,as well as photochemical box model and3-D regional chemical and transport modelsimulations, the effect of VOCs on the formation of ozone in Beijing area was investigated byclassifying the VOCs progressively (from total VOCs to classified VOCs, and to speciatedVOC). An emission inventory of speciated VOCs emitted from main anthropogenic sources ofBeijing was developed and applied. Main conclusions of this thesis include：①Due to thehigh traffic density and local emissions, the average levels of reactive VOCs at the urban siteswere much higher than those at the SDZ regional background site. Alkanes were the primarycomponents of VOCs in Beijuing area, followed by aromatics, alkenes and biogenic VOCs.Alkanes, alkenes, aromatics and biogenic VOCs all had much higher ambient concentrationsat the urban site than those at the rural site, while the percentage of biogenic VOCs to totalVOCs was higher at the rural site than that at the urban site.②The gross ozone productionrate G(O_3) and ozone production efficiency (OPE) have been calculated with a photochemicalbox model constrained by observed data, and the relationship between OPE and NOxconcentration was also analyzed. Results showed that photochemical ozone productionprocess is mainly sensitive to VOCs at urban area. In the background area, the productionprocess is sensitive to VOCs and NOxalternatively.③A3-D regional chemical and transportmodel WRF-Chem was used to simulate the typical regional photochemical pollutionprocesses in Beijing area. Simulated results showed that the ozone formation is controlled bythe alkenes emissions in the urban area. Reducing the emissions of alkenes can decrease O_3concentration efficiently in urban area, and this also affects the concentration level of ozone inbackground area.④Alkenes make a major contribution to the LOH, aromatics dominate OFP atboth urban and rural sites. According to the OH loss rate coefficient (LiOH) and the ozoneformation potential (OFP) estimated from the observed ambient mixing ratios of speciatedVOCs, key reactivie species for the ozone formation in Beijing area were recognized. They are m,p-xylene, toluene, trimethyl benzene, propylene, isoprene and butenes. Compared to thethe urban area, biogenic emission and the regional transport have a large influence on OHradicals and the ozone formation in the regional background area.⑤An emission inventoryof speciated VOCs emitted from main anthropogenic sources of Beijing in2003and2006wasdeveloped, and the ozone formation potential (OFP) of VOCs was estimated. Alkenes make amajor contribution to OFP. The top10species, in terms of OFP, consist of ethylene,m,p-xylene, toluene,1-butene, i-pentane, trans-2-butene, propene, cis-2-butene, o-xylene, andacetylene. These species contribute about60%to the total VOC emissions but account for80%of the OFPs in the region. Both high VOC emissions and OFP values appear in the urbanarea of Beijing. Decreasing the traffic exhaust, solvent volatilization and gasoline evaporationwill be the most effective way to reduce VOC emissions and control ozone formation inBeijing area.⑥Local photochemistry played adominant role in ozone formation at urbansite, while biogenic VOCs emissions and long range transportation by urban plume made agreater percentage contribution to OH radical consumption and ozone creation at the ruralsite.
引文
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