Diurnal curves of tropospheric ozone in the Western United States

Diurnal curves of tropospheric ozone are characterized for the areas near coniferous forests in the western U.S. A given day of hourly data can be placed into one of 17 classes of diurnal curves simply by knowing the 24-h mean and coefficient of variation of range, or more precisely, by applying equations derived from our discriminant analysis. The variation among curves is known to be related to theory of ozone formation, scavenging, and transport. Season, latitude, and position relative to source areas affect the form of the diurnal curve.     

洲际传输对我国对流层臭氧影响的数值模拟

采用M0ZART-4模式并引入在线源追踪方法量化分析北美和欧洲对我国对流层臭氧(O3)的贡献,整体来说模拟值能较好地与观测值对应.结果表明,北美和欧洲对流层对我国近地层O3贡献较低,夏季体积分数分别为0.3×10 9和0.6×10-9;冬季略高,均为0.9×10-9.北美对我国自由对流层O3贡献较高,不同季节体积分数峰...     

Influence of power plant emissions and industrial emissions on the leeward ozone levels

In this paper a multibox model is applied to investigate how power plant emissions and industrial emissions affect the O₃ levels in a leeward urban area and a farther downwind rural area. Apart from a detailed consideration of one specific situation, the effect of advection is described and the influence of emission reductions on ozone formation is analyzed. The results prove that the characteristics of upstream emissions is of great significance for the O₃ levels. In particular, a reduction of hydrocarbon emissions was proved to be beneficial in all considered cases, while a reduction of primarily NO_x emissions may lead to an enhanced O₃ formation.     

长江三角洲地区对流层臭氧的数值模拟研究

将NCAR的中尺度天气预报模式MM5和作者开发的化学模式相耦合,建立了一个中尺度区域空气质量模式.利用该模式选取了2个典型个例研究了长江三角洲地区的区域臭氧化学问题.本研究的目的是利用模式再现并描述长江三角洲地区的大气物理化学过程,结合地面观测资料进一步定量分析控制该地区臭氧浓度的物理和化学因子.通过个例模拟和分析表明,模式基本反应了长江三角洲地区的大气物理化学过程,进一步的因子分析解释了模拟区域内1999 06 18(个例2)臭氧浓度普遍比1999 08 07(个例1)的臭氧浓度高的原因.模拟结果表明天气条件决定的大气动力过程对区域空气质量起着至关重要的作用,这也是个例2区域臭氧浓度普遍偏高的最主要因素之一.分析表明,物理因子(平流输送,垂直湍流输送)的作用和化学因子的作用同样重要.同时还做了模式参数的敏感性实验研究,并对中尺度云雨化学模拟及其对臭氧化学的影响做了初步研究.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

Mid-latitude northern hemisphere background sulfate concentration in rainwater

The pH is not sufficient to characterize the acidity of precipitation, but rather its acid-base components must be described. The chemistry of natural emission sources as well as the mechanism of precipitation formation determine the chemistry of precipitation at mid-latitude, Northern Hemisphere locations. With the ocean biota as a source of atmospheric aerosol SO₄²⁻, it is expected that this “background” chemistry will be dominated by SO₄²⁻. For the purpose of this study, background was defined as a remote site generally upwind of urban areas, with the additional requirement that samples with evidence of contamination by anthropogenic sources be excluded. Canadian and U.S. data from long term precipitation monitoring sites along the coasts of British Columbia, Oregon, and Washington were evaluated to estimate a background SO₄²⁻ concentration in rainwater. In addition to screening the data for charge balance, collection efficiency, and anthropogenic influence, the data were corrected for SO₄²⁻ associated with sea salt. The results of this analysis suggest that the mid-latitude, Northern Hemisphere background excess SO₄²⁻ concentration in rainfall occurs most frequently in the range of 2–16 μeqℓ⁻¹ with a mean of 5.5 μeqℓ⁻¹ and an average measured pH of 5.3.     

上海地区对流层低层臭氧及硫酸盐气溶胶时空分布特征研究

基于Aura/OMI卫星资料,分析了上海地区2007—2016年近十年对流层低层O_3浓度(0~3 km)、SO_2柱浓度和硫酸盐气溶胶光学厚度(0~2 km)时空演变特征.结果表明,近十年来上海地区臭氧浓度总体呈现上升的趋势,最低值在2008年,为31.57μg·m~(-3),最高值在2016年,浓度为40.72μg·m~(-3);O_3季节变化明显,夏季高、春秋次之、冬季低.十年来,硫酸盐气溶胶污染先减少后增加,2007年硫酸盐气溶胶(AOD=0.81)污染最为严重,占近十年硫酸盐气溶胶发生频率的16.41%,2010年污染最轻(AOD=0.68),比2007年下降了16.12%,且硫酸盐气溶胶污染频率为7.68%,但在2013年以后,硫酸盐气溶胶污染又出现增长趋势;污染季节特征与O_3相同,这主要是因为夏季阳光充足有利于大气光化学反应的进行,从而使O_3和硫酸盐气溶胶等光化学产物的浓度升高.SO_2浓度在2007—2014年总体呈现下降的变化趋势,且下降趋势明显,最低值(2014年)比最高值(2007年)降低了52.76%,但在2014年后SO_2浓度略有反弹;SO_2污染主要集中在冬季.     

基于卫星观测的青海高原对流层臭氧时空分布特征研究

基于OMI-MLS对流层臭氧总量数据集对2005—2019年青海高原对流层大气臭氧总量进行提取分析,探讨其时空分布格局及气象因子的影响.结果表明：①OMI-MLS对流层臭氧总量数据在青海高原的适用性良好.③海高原的多年平均对流层臭氧总量分布整体呈东北高西南低的态势,受地形和大气环流形势影响较大.海东市的对流层臭氧总量最高,其次是西宁市、格尔木市、德令哈市,玉树市的对流层臭氧总量最低.对流层臭氧总量月变化在一定程度上表现为"倒V"型特点：峰值位于6—7月,谷值位于1月,与气温变化密切相关.对流层臭氧总量季节变化明显,空间异质性强,夏季最高,春季、秋季次之,冬季最低.③近15年青海高原对流层臭氧总量呈显著增加趋势,年平均增加速率为0.22 DU,4个季节的对流层臭氧总量均呈波动上升趋势,冬季的对流层臭氧总量增加速率最快,其次是春季、夏季,秋季增加速率较慢.④影响青海高原对流层大气臭氧总量的主要气象因子是气温和降水,而次要因子表现略有不同.     

航空器场面滑行污染物排放计算研究

分析了航空器发动机排放污染物种类,介绍了标准起飞着陆循环(LTO)与航空器全发滑行方式下油耗与排放计算模型,建立了单发滑行、牵引滑行、APU电力驱动滑行3种滑行方式的油耗与排放计算模型.采用油耗与排放修正模型,对航空器场面滑行阶段因外界温度、气压、湿度等因素造成的油耗系数与排放系数改变进行修正.以上海虹桥机场为例,计算了不同滑行方式下各机型污染物气体排放量.计算结果表明:采用单发滑行与APU电力驱动滑行可降低航空器场面滑行阶段HC、CO和NOx的排放量,牵引滑行对NO_x的排放影响不大,但可明显降低HC、CO的排放量.     

Effect of elevated tropospheric ozone on methane and nitrous oxide emission from rice soil in north India

Physiological changes in crop plants in response to the elevated tropospheric ozone (O₃) may alter N and C cycles in soil. This may also affect the atmosphere-biosphere exchange of radiatively important greenhouse gases (GHGs), e.g. methane (CH₄) and nitrous oxide (N₂O) from soil. A study was carried out during July to November of 2007 and 2008 in the experimental farm of Indian Agricultural Research Institute, New Delhi to assess the effects of elevated tropospheric ozone on methane and nitrous oxide emissions from rice (Oryza sativa L.) soil. Rice crop was grown in open top chambers (OTC) under elevated ozone (EO), non-filtered air (NF), charcoal filtered air (CF) and ambient air (AA). Seasonal mean concentrations of O₃ were 4.3 ± 0.9, 26.2 ± 1.9, 59.1 ± 4.2 and 27.5 ± 2.3 ppb during year 2007 and 5.9 ± 1.1, 37.2 ± 2.5, 69.7 ± 3.9 and 39.2 ± 1.8 ppb during year 2008 for treatments CF, NF, EO and AA, respectively. Cumulative seasonal CH₄ emission reduced by 29.7% and 40.4% under the elevated ozone (EO) compared to the non-filtered air (NF), whereas the emission increased by 21.5% and 16.7% in the charcoal filtered air (CF) in 2007 and 2008, respectively. Cumulative seasonal emission of N₂O ranged from 47.8 mg m⁻² in elevated ozone to 54.6 mg m⁻² in charcoal filtered air in 2007 and from 46.4 to 62.1 mg m⁻² in 2008. Elevated ozone reduced grain yield by 11.3% and 12.4% in 2007 and 2008, respectively. Global warming potential (GWP) per unit of rice yield was the least under elevated ozone levels. Dissolved organic C content of soil was lowest under the elevated ozone treatment. Decrease in availability of substrate i.e., dissolved organic C under elevated ozone resulted in a decline in GHG emissions. Filtration of ozone from ambient air increased grain yield and growth parameters of rice and emission of GHGs.     

Study of tropospheric ozone in the tropical belt (Africa,America) from STRATOZ and TROPOZ campaigns

During three large-scale airborne scientific missions (STRATOZ III: June 1984; STRATOZ III-S: March 1985; TROPOZ I: December 1987), the distributions of ozone and its precursors were measured in the tropical belt over the American and African continents, within an altitude range of 0–12 km. The results reveal an important difference between the northern part of South America, characterized in June by an important O₃ depletion, and West Africa, where high O₃ contents are observed as a result of enhanced formation from bush fires during a large period of the year. O₃ concentrations as high as 160 ppb were observed in the neighborhood of emission areas, corresponding to formation rates on the order of several tens of ppb per hour.     

前体物排放变化对珠江三角洲地区秋季臭氧污染演变的影响研究

自2013年以来,珠三角地区SO₂、NO_x及颗粒物等污染物浓度逐渐下降,但臭氧污染日渐凸显.作为二次污染物,臭氧污染演变受到排放与气象条件共同影响.而评估本地前体物人为排放变化、外部传输和气象变化对臭氧污染演变的影响,并识别臭氧污染长期演变趋势的重要驱动因素,是开展区域臭氧污染防控的关键基础.因此,本文采用WRF-SMOKE-CMAQ模拟平台,以2006—2017年广东省和中国大气污染物排放趋势清单为输入清单,以2014年的气象数据为基准年气象场,通过设置不同案例,结合观测数据,定量评估本地、外部排放变化和气象变化对珠三角秋季O₃污染长期演变趋势的影响.结果表明：在2006—2017年期间,整个珠三角9—10月臭氧日最大8 h(MDA8)浓度上升主要由人为排放变化主导,平均每年贡献0.7μg·m^-3,而气象条件总体上抑制了2006—2017年期间珠三角秋季臭氧MDA8浓度的增长,使得秋季臭氧MDA8浓度上升速率下降为0.2μg·m^-3·a^-1;人为排放变化...     

飞机LTO排放影响评估耦合模型研究与应用

民航飞机在LTO起降阶段的飞行中,发动机污染物排放的源强和空间位置是动态的.为准确定量评估其影响,构建了飞机LTO污染排放影响评估耦合模型.首先利用飞行动力学模型,模拟飞机LTO飞行轨迹,并获得轨迹中每一位置点的性能参数（实时燃油流量）;再通过排放计算模型,确定每一位置点的污染物排放量（源强）;在此基础上,基于拉格朗日烟团模型,针对飞机烟团排气特点进行修正,实现污染扩散模拟.最后采集了一架典型飞机在一个完整LTO飞行过程中的机载数据,结合实时气象参数,进行了实例应用研究.结果显示.在LTO过程中NO_x、SO₂、CO、PM和HC的平均排放速率分别为17.71、2.21、1.05、0.20和0.03g/s;飞机在起飞离地时刻,烟团扩散范围集中于跑道附近及侧向300m、纵向3000m范围内,NO_x地面最大浓度超过100mg/m³;当飞机爬升至混合层顶完成起飞时,地面污染物扩散至侧向1200m范围,NO_x浓度降至298.5μg/m³,依然较为严重,其他污染物地面浓度相对较低_.     

成都市道路移动源减排对空气质量的短期影响

近年来随着经济社会的高速发展,我国的空气污染问题日渐突出.管控污染源以减少污染物排放是改善空气质量的主要手段,且其效率如何会极大地影响空气质量的改善效果.但通常情况下,单一减排手段的实施对空气质量的改善的实际贡献往往在短时间内较难做出客观评价.本研究借助新冠疫情期间以道路移动源为主的各类污染源排放短期内大量下降的机会,通过疫情管控措施实施前后交通条件和空气质量的对比,分析道路移动源减排对空气质量改善的短期影响.结果表明,实施管控措施后,城市范围内道路交通条件明显改善,拥堵路段基本消失.受此影响,各类主要污染物浓度出现不同程度的下降,其中,受道路移动源贡献较大的NO₂浓度下降比例达40%~60%,PM_2.5因受气象条件影响较大而下降幅度较小.结合实时的交通数据估算其相应的尾气排放结果表明,疫情期间道路移动源排放的NO_x、HC、CO分别下降59.7%、59.9%和58.8%.本研究对于分析短时间内急速减排等应急措施对环境改善的效果,以及削减污染物排放对空气质量改善的潜力有重要的实际参考价值.     

河北省中南部对流层CH4时空分布特征的飞机探测研究

为研究河北省中南部对流层内CH₄时空分布特征,2018年6~7月利用空中国王350飞机搭载高精度CH₄分析仪和相关辅助设备,对河北中南部城市上空（600~5500m）CH₄浓度进行飞机探测.探测期间共飞行4架次,取得7组CH₄浓度垂直廓线数据.结果表明：探测期间CH₄浓度最小值为1884×10^-9,最大值为2038×10^-9,多架次垂直方向上平均浓度为（1915±90）×10^-9.不同探测架次CH₄浓度随高度变化趋势有较好的一致性,随高度增加,均出现先增大后减小,后稳定不变的趋势,且在混合层顶以下（约1000m）存在明显分界线.1000m以下,同高度层CH₄浓度变化较大,不同架次间浓度相差最大值达124×10^-9,同一架次CH₄浓度的垂直梯度变化受大气层结影响明显,位温垂直梯度接近零时,CH₄浓度的垂直梯度变化不明显.1000m以上,CH₄浓度垂直随高度增加呈指数减小,同高度层CH₄浓度变化较小,变化偏差在平均值的5%以内,4000m以上,同高度层CH₄浓度振幅最小,差值<15×10^-9,此时浓度可代表该区域背景大气的平均浓度.石家庄上空同高度层CH₄浓度白天整体大于夜间,随高度降低差值变大,说明石家庄白天CH₄排放源强度大于夜间.     

Characterization of aircraft emissions and air quality impacts of an international airport

Beijing Capital International Airport(ZBAA) is the world's second busiest airport. In this study, the emissions of air pollutants from aircraft and other sources at ZBAA in 2015 were estimated using an improved method, which considered the mixing layer height calculated based on aircraft meteorological data relay(AMDAR), instead of using the height(915 m)recommended by ICAO. The yearly emissions of NO_x, CO, VOCs, SO_2, and PM_(2.5) at the airport were 8.76 × 10~3, 4.43 × 10~3, 5.43 × 10~2, 4.80 × 10~2, and 1.49 × 10~2 ton/year, respectively. The spatial–temporal distribution of aircraft emissions was systematically analyzed to understand the emission characteristics of aircraft. The results indicated that NOxwas mainly emitted during the take-off and climb phases, accounting for 20.5% and 55.5% of the total emissions. CO and HC were mainly emitted during the taxi phase, accounting for 91.6%and 92.2% of the total emissions. Because the mixing layer height was high in summer, the emissions of aircraft were at the highest level throughout the year. Based on the detailed emissions inventory, four seasons simulation using WRF-CMAQ model was performed over the domain surrounding the airport. The results indicated that the contribution to PM_(2.5) was relatively high in winter; the average impact was about 1.15 μg/m~3 within a radius of1 km around the airport. Meanwhile, the near surroundings and southwest areas of the airport are the most sensitive to PM_(2.5).     

Carbonyl emissions from heavy-duty diesel vehicle exhaust in China and the contribution to ozone formation potential

Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaidehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasolinepowered vehicles （58.4 Gg）. The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.     

粤北地区一次臭氧污染过程分析及数值模拟

2020年7月1日,粤北地区出现了一次O₃污染过程,其中韶关市录得全省最高值162μg·m^-3.本文利用常规观测资料以及再分析资料对影响此次韶关地区O₃污染过程的主要气象场特征进行分析,结果表明：6月28日—7月2日天气形势总体处于静稳状态,地面受到均压场控制,同时副热带高压较强,脊线位于韶关上空,导致中高层有下沉气流,抑制了垂直方向污染物的扩散.6月28—30日(污染积累阶段),风速较大,韶关在外来输送和污染扩散条件的共同作用下,O₃浓度上升但未超标.7月1日(污染持续阶段),韶关和清远两地风速减小,污染扩散条件不利;同时气温有所上升,光化学反应作用增强,有利于O₃浓度攀升;同时广州和佛山两地的风向从偏南风转为偏北风,韶关市维持偏南风,主导风向的差异是全省只有韶关O₃超标的主要原因.7月2日(污染消散阶段),O₃外来传输及本地生成作用减弱,全省O₃浓度下降.进一步利用HYSPLIT后向轨迹以及WRF-CMAQ空...