北京大气臭氧浓度变化特征及其形成机制研究
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摘要
臭氧在全球和区域大气环境变化中扮演着重要角色,它不仅对地-气辐射收支系统产生重要影响,而且作为城市污染大气中的首要污染物,有着显著的环境效应。本研究以北京城区地面观测资料为基础,对大气中臭氧及其相关前体物NOx、CO和VOCs浓度及气象要素的分布特征进行了讨论;分析了臭氧等污染气体的相互关系,就气象要素对污染物浓度影响做了比较;并运用模型对光化学污染过程展开研究,主要研究内容如下:
(1)北京市大气中O_3浓度较高,并呈季节性波动,大气光化学污染以夏季最为严重。受太阳紫外辐射和城市交通的影响,城市大气中O_3和OX(O_3+NO_2)浓度在午后15:00左右出现峰值,NOx呈双峰态日变化,在07:00和23:00左右出现峰值。NO_2的光解速率夏季最大,在正午前后出现目最大值。NOx浓度存在100×10~(-9)(体积分数)的“分界点”,NOx低浓度时以NO_2为主,NOx高浓度时NO占大部分。OX区域贡献和局地贡献存在明显的季节变化,前者主要受区域背景O_3的影响,在春季最大,后者主要受局地NOx光化学反应的制约,在夏季最强,同时OX组分呈现显著的昼夜差异。受城市车流量的变化,周末NOx浓度高于工作日,O_3浓度周末与工作日白天差异较小,而夜晚O_3浓度工作日高于周末。
(2)北京地区大气臭氧总量平均为329DU,并呈冬春季较高,夏秋季较低的季节变化规律,到达地面的紫外辐射呈现相反的变化趋势。受城区大气污染的影响,地面处的紫外辐射量大幅减少(最大50%),且在夏季波动较大。云和污染物对紫外辐射的影响要大于总辐射,紫外辐射衰减约为总辐射衰减的2倍。城市低层大气中O_3和NOx浓度的增加是造成紫外辐射衰减的重要原因,午后O_3浓度与紫外辐射衰减相关系数为0.70。O_3浓度变化与与温度,风速成正相关,与相对湿度成反相关,且存在季节变化,夏季与温度相关性较高,冬季与风速相关性较高。受上游污染源的影响,当北京盛行东南、偏南和偏西气流时,容易造成高O_3浓度。夏季O_3浓度主要受局地光化学反应控制,可以利用常规气象要素对O_3浓度趋势预测。北京大气中CO浓度受排放源和大气扩散能力的影响呈现冬季高,夏季低的季节变化特征。白天8-h(09:00～16:00)CO浓度与风速分布频率存在负的统计相关性,相关系数r=0.93,K值为3.5±0.5。受观测点地理位置和周边道路机动车分布的影响,偏东气流控制时的CO浓度是偏西气流的2.3倍。
(3)北京大气中光化学反应程度夏季最高,平均为0.25。光化学反应程度呈单峰型日变化曲线,在午后15:00出现峰值。在自由基和氮氧化物作用下,O_3超标目光化学反应程度平均增加率为空气优良日的5.3倍。大气中NMHCs浓度中苯乙烯浓度最高(按丙烯等量浓度计),AHC丙烯等量浓度占NMHCs的大部分,而AHC中以R-AROM组分最高。臭氧产生效率平均为4.0,OX产生率随着NOx浓度的增加而递增,平均产生率为(12.5±8.3)×10~(-9)h~(-1)。大气中O_3净产生率在正午12:00最大,并以HO_2+NO和XO_2+NO光化学生成反应为主。北京大气中O_3浓度主要受VOCs浓度的控制,其中以人为源排放的活性芳香烃类化合物和烯烃类对大气中O_3产生的贡献最大。对排放此类化合物的人为活动,如建筑涂料、石油精炼、机动车尾气以及油品挥发性的控制改善,将对降低北京光化学污染程度起到关键作用。此外城市绿化植被品种的科学选择,对减缓城市光化学污染也具有一定程度的帮助。
Atmospheric ozone plays an important role in global and regional environment change.It has a significant impact on the solar radiation budget.As one of primary gaseous contaminant in urban ambient,ozone has an important effect on the urban and suburbant atmospheric environment. Based on the data of air pollutants and meteorological parameter collected in Beijing, Characteristics of ozone precursor are explored.Trace gases NOx and CO,VOCs,temperature and solar radiation are associated with ozone formation.The major contents and conclusions are presented as follows:
Firstly,O_3 pollution is very serious,and O_3 concentrations fluctuate periodically.The photochemical pollution in Beijing is most serious in summer.The peak O_3 and oxidant (OX=O_3+NO_2)concentration in Beijing often appear about 15:00 in the early afternoon;the diurnal variation of NOx concentrations show a very clear cycle with two peaks;one appears about 07:00 in the morning and the other is at 23:00 in the evening.The highest photolysis rate coefficient of NO_2(J_3)appears in summer.The greatest J_3 in daytime appears at noon.The NOx crossover point occurs at about 100×10~(-9)NOx At lower levels,NO_2 is the major component of NOx,whereas NO dominates at higher mixing ratios.It is also shown that the level of OX is made up of two contributions,regional contribution and local contribution.The former is affected by regional background O_3 level,with the maximum in spring,whereas the latter is effectively correlates with the level of primary pollution,with the maximum in summer.Diurnal variation also appears in the concentrations of the components of oxidants.Owing to changes of traffic in urban,NOx concentrations on weekends are higher than weekdays.Variations of O_3 concentrations in daytime in weekend are a little different from weekdays,but O_3 concentrations in night on weekends are lower than weekdays.
Secondly,average total ozone content in Beijing is 329 DU and higher in winter and spring, lower in summer and autumn.The inverse relationship exists between ground level UV radiation and total ozone content.This study also shows that a substantial reduction(up to 50%)in the UV radiation on days with high levels of air pollution.Larger fluctuations are found in UV radiation in the summer.The effects of clouds and air pollution on UV are higher than on total solar radiation, and the reduction in UV is about twice as large as the total solar radiation values.Strong reduction in the UV radiation reaching the ground is associated with the increase of tropospheric ozone and nitrogen oxides in Beijing.The correlation coefficient between ozone concentration and decrease in UV radiation is 0.70 in the early afternoon.Both temperature and wind speed have significant positive correlation with ozone.Relative humidity has a significant negative correlation with ozone.Ozone concentrations have signficant correlation with temperature in summer and with wind speed in winter.The distant transport associated with southeastern,southern and western winds contributes substantially to the ozone because the air mass is polluted.The main relationships we could observe in these analyses are then used to obtain a regression equation linking diurnal ozone concentration in summer with meteorological parameters.The characteristics of CO concentration and wind-speed data distribution show that there is an obviously seasonal cycle of CO concentration,with the maximum in winter and minimum in summer.The seasonal variations are believed to be due to the combination results of emission sources and atmospheric diffusion.Data show an inverse relationship between opposing percentiles of the distribution of CO concentration and mean wind speed,and its correlation coefficient is 0.93.The value of K is 3.5±0.5.CO concentrations when prevailing wind direction is from East sector may be 2.3 times higher as compared from West sector,which are affected by where the sample is located and the advection of pollution air from high traffic density area nearby.
Thirdly,the highest mean extent of reaction appears in summer.Hourly average extent of reaction in summer is 0.25.The diurnal variation of extent of reaction shows a very clear cycle with single peak,the peak often appears at about 15:00 in the early afternoon.With the availability of radicals and oxides of nitrogen,the mean of reaction increase may be 5.3 times higher at high level as compared at low level.The reactivity of NMHCs is dominated by anthropogenic NMHCs and of the anthropogenic NMHCs,reactive aromatics dominate in which eth-benzene is the most important.Ozone production efficiency is 4.0.Oxidant production rate increases with increasing NOx,with the average of(12.5±8.3)×10~(-9)·h~(-1).The highest net ozone production rate appears in the noontime.Generally the formation of ozone throughout of Beijing area is limited by VOCs,in which reactive aromatics and alkene are dominant.
(1)北京市大气中O_3浓度较高,并呈季节性波动,大气光化学污染以夏季最为严重。受太阳紫外辐射和城市交通的影响,城市大气中O_3和OX(O_3+NO_2)浓度在午后15:00左右出现峰值,NOx呈双峰态日变化,在07:00和23:00左右出现峰值。NO_2的光解速率夏季最大,在正午前后出现目最大值。NOx浓度存在100×10~(-9)(体积分数)的“分界点”,NOx低浓度时以NO_2为主,NOx高浓度时NO占大部分。OX区域贡献和局地贡献存在明显的季节变化,前者主要受区域背景O_3的影响,在春季最大,后者主要受局地NOx光化学反应的制约,在夏季最强,同时OX组分呈现显著的昼夜差异。受城市车流量的变化,周末NOx浓度高于工作日,O_3浓度周末与工作日白天差异较小,而夜晚O_3浓度工作日高于周末。
(2)北京地区大气臭氧总量平均为329DU,并呈冬春季较高,夏秋季较低的季节变化规律,到达地面的紫外辐射呈现相反的变化趋势。受城区大气污染的影响,地面处的紫外辐射量大幅减少(最大50%),且在夏季波动较大。云和污染物对紫外辐射的影响要大于总辐射,紫外辐射衰减约为总辐射衰减的2倍。城市低层大气中O_3和NOx浓度的增加是造成紫外辐射衰减的重要原因,午后O_3浓度与紫外辐射衰减相关系数为0.70。O_3浓度变化与与温度,风速成正相关,与相对湿度成反相关,且存在季节变化,夏季与温度相关性较高,冬季与风速相关性较高。受上游污染源的影响,当北京盛行东南、偏南和偏西气流时,容易造成高O_3浓度。夏季O_3浓度主要受局地光化学反应控制,可以利用常规气象要素对O_3浓度趋势预测。北京大气中CO浓度受排放源和大气扩散能力的影响呈现冬季高,夏季低的季节变化特征。白天8-h(09:00～16:00)CO浓度与风速分布频率存在负的统计相关性,相关系数r=0.93,K值为3.5±0.5。受观测点地理位置和周边道路机动车分布的影响,偏东气流控制时的CO浓度是偏西气流的2.3倍。
(3)北京大气中光化学反应程度夏季最高,平均为0.25。光化学反应程度呈单峰型日变化曲线,在午后15:00出现峰值。在自由基和氮氧化物作用下,O_3超标目光化学反应程度平均增加率为空气优良日的5.3倍。大气中NMHCs浓度中苯乙烯浓度最高(按丙烯等量浓度计),AHC丙烯等量浓度占NMHCs的大部分,而AHC中以R-AROM组分最高。臭氧产生效率平均为4.0,OX产生率随着NOx浓度的增加而递增,平均产生率为(12.5±8.3)×10~(-9)h~(-1)。大气中O_3净产生率在正午12:00最大,并以HO_2+NO和XO_2+NO光化学生成反应为主。北京大气中O_3浓度主要受VOCs浓度的控制,其中以人为源排放的活性芳香烃类化合物和烯烃类对大气中O_3产生的贡献最大。对排放此类化合物的人为活动,如建筑涂料、石油精炼、机动车尾气以及油品挥发性的控制改善,将对降低北京光化学污染程度起到关键作用。此外城市绿化植被品种的科学选择,对减缓城市光化学污染也具有一定程度的帮助。
Atmospheric ozone plays an important role in global and regional environment change.It has a significant impact on the solar radiation budget.As one of primary gaseous contaminant in urban ambient,ozone has an important effect on the urban and suburbant atmospheric environment. Based on the data of air pollutants and meteorological parameter collected in Beijing, Characteristics of ozone precursor are explored.Trace gases NOx and CO,VOCs,temperature and solar radiation are associated with ozone formation.The major contents and conclusions are presented as follows:
Firstly,O_3 pollution is very serious,and O_3 concentrations fluctuate periodically.The photochemical pollution in Beijing is most serious in summer.The peak O_3 and oxidant (OX=O_3+NO_2)concentration in Beijing often appear about 15:00 in the early afternoon;the diurnal variation of NOx concentrations show a very clear cycle with two peaks;one appears about 07:00 in the morning and the other is at 23:00 in the evening.The highest photolysis rate coefficient of NO_2(J_3)appears in summer.The greatest J_3 in daytime appears at noon.The NOx crossover point occurs at about 100×10~(-9)NOx At lower levels,NO_2 is the major component of NOx,whereas NO dominates at higher mixing ratios.It is also shown that the level of OX is made up of two contributions,regional contribution and local contribution.The former is affected by regional background O_3 level,with the maximum in spring,whereas the latter is effectively correlates with the level of primary pollution,with the maximum in summer.Diurnal variation also appears in the concentrations of the components of oxidants.Owing to changes of traffic in urban,NOx concentrations on weekends are higher than weekdays.Variations of O_3 concentrations in daytime in weekend are a little different from weekdays,but O_3 concentrations in night on weekends are lower than weekdays.
Secondly,average total ozone content in Beijing is 329 DU and higher in winter and spring, lower in summer and autumn.The inverse relationship exists between ground level UV radiation and total ozone content.This study also shows that a substantial reduction(up to 50%)in the UV radiation on days with high levels of air pollution.Larger fluctuations are found in UV radiation in the summer.The effects of clouds and air pollution on UV are higher than on total solar radiation, and the reduction in UV is about twice as large as the total solar radiation values.Strong reduction in the UV radiation reaching the ground is associated with the increase of tropospheric ozone and nitrogen oxides in Beijing.The correlation coefficient between ozone concentration and decrease in UV radiation is 0.70 in the early afternoon.Both temperature and wind speed have significant positive correlation with ozone.Relative humidity has a significant negative correlation with ozone.Ozone concentrations have signficant correlation with temperature in summer and with wind speed in winter.The distant transport associated with southeastern,southern and western winds contributes substantially to the ozone because the air mass is polluted.The main relationships we could observe in these analyses are then used to obtain a regression equation linking diurnal ozone concentration in summer with meteorological parameters.The characteristics of CO concentration and wind-speed data distribution show that there is an obviously seasonal cycle of CO concentration,with the maximum in winter and minimum in summer.The seasonal variations are believed to be due to the combination results of emission sources and atmospheric diffusion.Data show an inverse relationship between opposing percentiles of the distribution of CO concentration and mean wind speed,and its correlation coefficient is 0.93.The value of K is 3.5±0.5.CO concentrations when prevailing wind direction is from East sector may be 2.3 times higher as compared from West sector,which are affected by where the sample is located and the advection of pollution air from high traffic density area nearby.
Thirdly,the highest mean extent of reaction appears in summer.Hourly average extent of reaction in summer is 0.25.The diurnal variation of extent of reaction shows a very clear cycle with single peak,the peak often appears at about 15:00 in the early afternoon.With the availability of radicals and oxides of nitrogen,the mean of reaction increase may be 5.3 times higher at high level as compared at low level.The reactivity of NMHCs is dominated by anthropogenic NMHCs and of the anthropogenic NMHCs,reactive aromatics dominate in which eth-benzene is the most important.Ozone production efficiency is 4.0.Oxidant production rate increases with increasing NOx,with the average of(12.5±8.3)×10~(-9)·h~(-1).The highest net ozone production rate appears in the noontime.Generally the formation of ozone throughout of Beijing area is limited by VOCs,in which reactive aromatics and alkene are dominant.
引文
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