2021年南京市新冠疫情期间大气污染物变化特征及来源解析

为了解2021年南京市新冠疫情期间城市大气污染物浓度的变化和成因,利用南京大学SORPES站点2021年7月1日—2021年8月30日大气污染物在线监测数据,分析疫情前、中、后颗粒物及气态污染物的浓度变化,针对臭氧(O₃)的关键前体物,挥发性有机物(Volatile Organic Compounds,VOCs)采用正定矩阵因子分解法模型(Positive Matrix Factorization,PMF)、拉格朗日粒子输送与扩散模型(Lagrangian Particle Distribution M odel,LPDM)分析其污染来源。结果表明:疫情封闭期间,南京市PM_2.5质量浓度较疫情前降低了40%～50%,组分中硝酸盐、有机物质量浓度降幅最为显著,分别下降了34.0%和16.5%。臭氧体积浓度不降反升,城中区域增幅最显著站点可达50%左右。其气态前体物氮氧化物(NO_x)及VOCs浓度变化呈相反态势,分别较疫情前降低28%、升高49.6%。模型及卫星遥感结果表明,疫情期间南京市臭氧属于协同偏VOCs控制区。气团溯...     

武汉市2018年4—9月臭氧及其前体物非线性关系研究

近年来武汉市臭氧污染日益严峻,成为影响空气质量达标的瓶颈,弄清臭氧及其前体物非线性关系是臭氧防控的关键和基础.本研究基于武汉中心城区2018年4—9月臭氧及其前体物在线观测数据,分析出武汉市臭氧浓度受前体物和气象条件等因素的共同影响,呈较为明显的季节变化和日变化特征.观测期间武汉市大气挥发性有机物（VOCs）平均体积分数为32.5×10^-9,烷烃是武汉市VOCs的主要组分,其次是含氧VOCs （OVOCs）和卤代烃.利用基于观测的模型定量分析臭氧与前体物之间的关系,发现削减VOCs会引起臭氧生成潜势的显著下降,而削减氮氧化物则会使臭氧生成潜势升高,说明武汉市臭氧生成处于VOCs控制区.在人为源VOCs中,间/对二甲苯和邻二甲苯的相对增量反应活性（RIR）最高,是影响臭氧生成的关键组分.     

东亚区域对流层臭氧及其前体物的季节性关联

利用2010—2012年对流层臭氧（O₃）及其多种前体物的卫星遥感资料和全球水汽再分析资料,研究东亚区域O₃及其前体物的时空分布,以及在中国东部（分为南、北两部分）相关性的季节变化。结果表明:东亚区域NO₂与CO的对流层柱含量均表现为冬季高、夏季低的时空变化形式。O₃对流层柱含量夏季达到峰值,冬季为谷值。中国东部的北部与南部地区O₃与NO₂均在夏秋季呈正相关,冬春季呈负相关。夏季大部分地区NO_x的光化学循环反应对O₃生成有积极的促进作用,冬季大部分地区O₃的光化学循环生成受到抑制。O₃与CO在北部地区夏秋季和南部地区夏季正相关性最大,无论是在北部还是南部地区,O₃与CO的相关性在轻污染情况下最大,而在重污染和背景情况下较小,表明重污染气团向下风方的输送更有利于O₃的光化学生成。O₃与水汽在北部和南部地区的多数时间均呈较显著的正相关性,而在南部地区夏季和北部地区冬季具有较大的负相关性,反映出不同的环流形式、气团来源及伴随的天气条件变化对O₃分布的影响。     

解析北京郊区一次典型臭氧污染的物理化学过程

臭氧污染是我国当前面临的重要大气环境问题,其不仅取决于大气化学反应过程,而且会受大气物理过程和各气象要素的影响,因此需要从化学和物理两个方向来研究近地面臭氧污染问题。本研究结合外场观测和欧拉光化学模式,解析了2022年秋季北京怀柔城区的一次光化学污染周期内的物理和化学过程。给出了温度、湿度和风速等气象因子,以及臭氧及其前体物挥发性有机物(VOCs)和氮氧化物(NO_x,x=1、2)在此期间的日变化特征。通过源解析得到VOCs主要来源为交通排放(46%)、植物源(25%)、溶剂挥发(23%)和燃烧源(9%)。通过欧拉光化学模式确定了区域传输和本地VOCs对臭氧的贡献,结果显示强北风天气条件下,怀柔区臭氧以外来水平输送为主(贡献超过70%);当以弱的南风或东南风为主时,天气处于稳定状态,臭氧主要来自VOCs和NO_x的二次转化。根据VOCs的臭氧潜势,在所有VOCs中对臭氧贡献最大的物质为烯烃,其贡献为67%,其次为芳香烃(16%)。通过敏感度分析,发现臭氧生成对物理因子中的光强、温度和边界层高度最敏感;在臭氧前体物中,活性较强的烯烃类物质的敏感度最...     

典型区域传输过程关键源区减排对天津无机气溶胶及PM2.5的影响研究

利用嵌套网格空气质量数值预报模式NAQPMS探究一次典型区域传输过程关键源区气态前体物减排对天津无机气溶胶(IA)及PM2.5的影响。大尺度区域高精度的IA模拟数据显示,华北平原地区生成了高浓度的IA,向华东地区传输后,按顺时针方向又返回华北平原地区。这一往返式区域传输过程导致天津出现两次污染时段。利用耦合在NAQPMS中的在线污染物来源追踪方法量化了不同源区对天津IA的贡献,识别出华北平原地区是关键源区,日均贡献为57.6%～100%。在天津污染前1天和污染天对华北平原地区SO₂、NH₃和NO_x减排30%分别开展敏感性试验,研究表明NH₃减排导致天津IA和PM2.5最大下降率分别为30.8%和13.3%,是SO₂减排对IA和PM2.5最大下降率的16倍和26.6倍,是NO_x减排情景对IA和PM2.5最大下降率的7倍和6.4倍,成为降低天津污染水平最显著的前体物。SO₂减排造成天津硝酸盐浓度上升,最大增长率为3.5%,根据热动力学平衡...     

武汉地区疫情管控期间空气质量变化及改善措施研究

2020年1月23日起,武汉地区施行了严格的交通管控措施,对当地的人为活动产生了重大影响。本文基于地面监测站网和卫星遥感分析了管控期间武汉地区的主要大气成分的变化,并研究了人为排放下降对O₃和细颗粒物（PM2.5）污染的影响。研究发现,由于管控期间施行机动车禁行政策,武汉地区的NO₂浓度与2019年同期相比下降53.2%,挥发性有机物（VOCs）下降了25.1%;与NO₂和VOCs的显著下降不同,O₃日最大8小时滑动平均第90百分位浓度平均值与去年同期相比上升16.5%,尤其是2月温度同比增高超过5°C,紫外辐射增长超过100%,O₃浓度显著高于去年同期,说明应基于O₃前体物NO_x和VOCs 活性种类的非线性定量关系加强协同减排;同时,管控期间PM2.5浓度与去年同期相比下降了35.6%,但是PM2.5浓度低值主要集中在风速较大、扩散较好的2月,其他时段PM2.5浓度下降并不明显;值得注意的是,与2月的显著下降不同,3月硝酸盐的浓度同比变化不大,说明导致NO_x转化为硝酸盐的大气氧化能力并未受到较大削减,武汉地区颗粒物减排应基于颗粒物不同组分的形成机理,加强颗粒物一次排放源和关键前体物控制。     

新冠疫情影响下全球对流层臭氧变化特征研究进展

自2020年新冠疫情(COVID-19)爆发以来,各地进行了不同程度的人员流动限制或封控,致使全球范围内氮氧化物(NO_x)、二氧化硫(SO₂)、一氧化氮(CO)、细颗粒物(PM2.5)等大气污染物浓度均大幅度降低,而作为二次污染物的臭氧(O₃)在各地区却表现出复杂的变化特征,成为研究热点。本研究总结了近两年该方向的研究成果,阐明了COVID-19期间对流层O₃及其前体物的变化特征、变化机制及其可能存在的潜在环境效应。COVID-19严控期,全球人为NO_x排放下量降了至少15%,特别是高人为活动影响区,下降了18%～25%,部分高污染地区(挥发性有机物敏感区)近地层NO_x的减少量达50%以上。NO_x的减少导致NO对O₃的滴定作用减弱,使得该类高污染地区O₃增加(10%～50%)。而偏远地区及自由对流层O₃主要受NO_x控制,NO_x...     

2017年8—9月湖州市臭氧污染特征及其生成机制研究

近年来近地面臭氧问题日益凸显,成为影响空气质量持续改善的瓶颈.本研究基于2017年8—9月在湖州市城区开展的为期1个月的臭氧及其前体物挥发性有机物（VOCs）和氮氧化物（NO_x）在线观测数据,分析了臭氧及其前体物污染特征,利用正矩阵因子分析（PMF）解析了VOCs来源,并采用基于观测的模型（OBM）对臭氧生成机制进行研究.研究结果表明：1）观测期间湖州市VOCs平均体积分数为（24.78±9.10）×10^-9,其中占比最高的组成为烷烃、含氧VOCs （OVOCs）和卤代烃;2）在臭氧非超标时段,湖州市臭氧生成处于VOCs控制区,而在臭氧重污染期间湖州市处于以VOCs控制为主的过渡区;3）在臭氧超标时段,对臭氧生成潜势（OFP）贡献最大的是芳香烃（39.6%）,其次是烯烃（21.5%）和OVOCs （19.4%）,排名前三的关键组分为甲苯、乙烯和间/对二甲苯;4）源解析结果显示观测期间湖州市VOCs的主要来源是溶剂使用（27.0%）、交通排放（22.7%）、背景+传输（19.3%）、工业排放（16.9%）、汽油挥发（7.7%）和植物排放（6.4%）,重污染过程期间对OFP贡献最大的两类源是交通排放源和溶剂使用源,贡献百分比分别为35.1%和30.5%.因此,对交通排放和溶剂使用方面进行控制管理对湖州市大气臭氧污染防控有重要意义.     

污染源反演对重点城市群夏季O3模拟的改进效果评估

在嵌套网格空气质量预报模式系统(NAQPMS)的基础上,采用污染源反演方法优化以中国多尺度排放清单(MEIC)为主的先验排放清单中臭氧(O₃)前体物排放量估计。分析时段为2019年6～8月,重点评估了污染源反演对我国“2+26”城市、长三角、珠三角、成渝4个重点城市群O₃模拟的改进效果。评估结果表明,污染源反演获得的“2+26”城市、长三角、珠三角的氮氧化物(NO_x)排放速率整体低于先验清单的排放速率约0.6μg m_-2 s_-1,但反演的挥发性有机物(VOCs)排放速率在“2+26”城市整体上高于先验清单的排放速率约0.5μg m_-2 s_-1。利用反演的NO_x和VOCs排放量和NAQPMS模式对4个城市群O₃进行模拟,发现反演排放数据可以显著改进夏季O₃模拟性能,使得O₃日最大8小时平均值(MDA8-O₃)模拟的均方根误差(R...     

银川都市圈夏季臭氧来源数值模拟分析

在我国当前臭氧和颗粒物复合污染的局面下，位于西北地区的宁夏回族自治区近年来夏季臭氧区域性污染突出，浓度高值区主要分布在银川都市圈(银川市、石嘴山市和吴忠市)。因此利用区域空气质量模式系统RAMS-CMAQ对2019年夏季6月银川都市圈臭氧污染问题开展数值模拟，定量探讨区域传输及垂直输送对O₃浓度的贡献，为有效控制当地臭氧污染提供科学依据。结果表明：2019年6月银川都市圈O₃浓度北高、中部低，与前体物的分布特征并不完全一致，表明O₃的非线性效应以及背景O₃传输潜在的贡献。水平方向上，银川都市圈本地排放源对近地面O₃的贡献大都在20%～30%，仅灵武达40%以上，外界传输贡献均在30%以上。其中银川本地贡献较弱，相邻区域间存在输送影响，一定程度上减弱了该地区的本地贡献。此外，在夏季整体偏南风的影响下O₃有较为明显的由南向北的输送作用。垂直方向上，郊区、城市和工业代表性站点O₃浓度的变化趋势基本一致，各过程量贡献有所差异。夜晚O_...     

A study of ozone in the Colorado mountains

The seasonal and diurnal variations of ozone mixing ratios have been observed at Niwot Ridge. Colorado. The ozone mixing ratios have been correlated with the NO _x (NO+NO₂) mixing ratios measured concurrently at the site. The seasonal and diurnal variations in O₃ can be reasonably well understood by considering photochemistry and transport. In the winter there is no apparent systematic diurnal variation in the O₃ mixing ratio because there is little diurnal change of transport and a slow photochemistry. In the summer, the O₃ levels at the site are suppressed at night due to the presence of a nocturnal inversion layer that isolated ozone near the surface, where it is destroyed. Ozone is observed to increase in the summer during the day. The increases in ozone correlate with increasing NO _x levels, as well as with the levels of other compounds of anthropogenic origin. We interpret this correlation as in-situ or in-transit photochemical production of ozone from these precursors that are transported to our site. The levels of ozone recorded approach 100 ppbv at NO _x mixing ratios of approximately 3 ppbv. Calculations made using a simple clean tropospheric chemical model are consistent with the NO _x -related trend observed for the daytime ozone mixing ratio. However, the chemistry, which does not include nonmethane hydrocarbon photochemistry, underestimates the observed O₃ production.     

Surface ozone measurements in the Venezuelan tropical savannah

A one-year set of surface ozone measurements in a four-station network located in the Venezuelan savannah is reported. The diurnal ozone variation is typical of continental stations with a maximum in the afternoon, when vertical turbulent mixing is strongest. The annual O₃ average concentration, based on the monthly averages of daily maxima, was 17±2 ppb, which is in good agreement with values reported for similar latitudes. The boundary-layer ozone levels did not fall below 8 ppb, in contrast with previous sporadic measurements made in tropical latitudes. No evidence was found that mesoscale O₃ downdrafts in the ITCZ in the South American continent are an important source of surface ozone. Finally, it is suggested that the relatively high ozone levels observed at the end of the dry season are probably of photochemical origin.     

Role of Ozone Deposition in the Occurrence of the Spring Maximum

Abstract

A hypothesis has been formulated on the basis of experimental data presented in this article. According to the hypothesis, occurrence of the spring surface ozone maximum at mid-latitudes results from a delay in snow-cover melt. The data were collected at ozone stations in Minsk (Belarus) and Preila (Lithuania). Because the measurements of surface ozone concentration are quite different, despite the close proximity of the stations, a conclusion can be drawn about the significant influence of meteorological parameters on measurements. In addition to a rather subjective and poorly defined parameter—time of snow melt—the difference between the average March temperature and a climatological mean may be treated as a criterion for the presence or absence of the spring ozone maximum.     

1993年春季南极中山站上空大气臭氧的观测分析

利用球载电化学O3探空仪于1993年南半球春季在南极中山站测量了O3和温度垂直廓线，三次观测到O3 柱总量＜ 220 Du的低值，O3浓度减少从9月开始，9月中旬～10月中旬达到最大。典型O3垂直廓线表明，O3量损失最大区域在高度13～23 km之间，此高度与PSCs和火山气溶胶的存在高度有很好的对应关系。本文给出观测结果及初步分析。     

北京秋季地面O3的一维模式模拟研究

用一维光化学模式,基本模拟出静稳天气条件下2001年9月9日北京几个主要大气污染物种:O3、NO、NO2、CO以及SO2的日变化特点,并解释了影响O3及NO、NO2、CO和SO2日变化的控制因子作用。初步分析认为,地面O3对非甲烷碳氢化合物(NMHC)的变化很敏感。NMHC的增加或减少,将会造成O3的明显改变。造成9月9日夜间20:00~23:00一次污染物NO、CO和SO2浓度急剧升高的原因是由于夜间大气层结稳定情况下,大气的垂直扩散减弱,污染物在底层积累造成的。由于实际大气中,影响O3生成和损耗的机制很复杂,同时大气的平流输送是影响O3及其他污染物分布的重要因素,用一维模式虽然能够揭示出影响O3变化的几个因子的作用,但要深入分析O3产生和消耗机制,还需要用三维模式。     

Seasonal and Diurnal Ozone Variations: Observations and Modeling

Ozone mixing ratios observed by the Bordeaux microwave radiometer between 1995 and 2002 in an altitude range 25–75 km show diurnal variations in the mesosphere and seasonal variations in terms of annual and semi-annual oscillations (SAO) in the stratosphere and in the mesosphere. The observations with 10–15 km altitude resolution are presented and compared to photochemical and transport model results.Diurnal ozone variations are analyzed by averaging the years 1995–1997 for four representative months and six altitude levels. The photochemical models show a good agreement with the observations for altitudes higher than 50 km. Seasonal ozone variations mainly appear as an annual cycle in the middle and upper stratosphere and a semi-annual cycle in the mesosphere with amplitude and phase depending on altitude. Higher resolution (2 km) HALOE (halogen occultation experiment) ozone observations show a phase reversal of the SAO between 44 and 64 km. In HALOE data, a tendancy for an opposite water vapour cycle can be identified in the altitude range 40–60 km.Generally, the relative variations at all altitudes are well explained by the transport model (up to 54 km) and the photochemical models. Only a newly developed photochemical model (1-D) with improved time-dependent treatment of water vapour profiles and solar flux manages to reproduce fairly well the absolute values.     

A Possible Photochemical Link Between Stratospheric and Near-Surface Ozone on Swiss Mountain Sites in Late Winter

Record high near-surface ozone concentrations at two elevated sites (Chaumont, 1140 m asl, and Rigi, 1030 m asl) in Switzerland were observed simultaneously with extremely low total ozone during a fair weather period in mid-February 1993. An analysis of ozone, temperature, humidity, and wind profiles suggests that the surface ozone peaks were most possibly generated within the region in a layer between about 1000 and 1500 m asl. Mean diurnal cycles of ozone concentration during the period shows a strong increase from late morning to late afternoon at Chaumont and at the same time a decrease at the high alpine site Jungfraujoch (3580 m asl). The different diurnal ozone cycles can both be explained photochemically by taking into account the large difference in NOx concentrations (about two orders of magnitude) between the sites. Photochemical processes are also indicated by the diurnal cycles of NO2 and NO concentration. As a strong photochemical activity is not expected in mid-February at 47°N, we hypothesize that the extremely low total ozone played a role. Total ozone controls the amount of UV-B radiation reaching the troposphere and thus influences photochemical processes. Using a radiation model, we calculated an increase in ozone photolysis at Chaumont and Jungfraujoch of 73% and 83%, respectively, on the day with the lowest total ozone (243 DU) compared to average February conditions (335 DU). It is suggested that total ozone changes have the potential to stimulate photochemistry sufficiently to produce the observed surface ozone peaks at Chaumont and Rigi of 61 and 64 ppbv, respectively. A fog layer just below Chaumont during these days probably also influenced photochemistry, but on a smaller spatial scale. Our empirical results on the influence of changing UV radiation on tropospheric photochemistry are in close agreement with model studies of other groups. Although this case study represents unique conditions, a distinct anticorrelation between near-surface ozone at Chaumont and total ozone also appears in other years (1992–1997) when selecting fair weather days in mid-February. However, other influences cannot be excluded. The selected days provide evidence of a significant photochemical source of ozone in the mid-latitude lower troposphere in late winter.     

NUMERICAL SIMULATION OF OZONE DISTRIBUTIONS AND ITS VARIATION MECHANISM*

A 2-D global chemistry-transport model is set up in this paper.The model simulates the atmospheric ozone distributions well with specified dynamical conditions.The analysis of ozone variation mechanism shows that ozone is chemically in quasi-equilibrium except for the polar night region where the variation of ozone concentration is under the control of dynamical processes,that the oxygen atoms which produce ozone are mainly provided by the photolysis of O₂ in the upper stratosphere and by the photolysis of NO₂ in the lower stratosphere and the troposphere.and that the ozone is destroyed mainly by NO_x:the reactions between NO_x and O₃ and the odd oxygen cycle contribute 80% to more than 90% of the ozone destruction.     

NUMERICAL SIMULATION OF OZONE DISTRIBUTIONS AND ITS VARIATION MECHANISM

A 2-D global chemistry-transport model is set up in this paper.The model simulates theatmospheric ozone distributions well with specified dynamical conditions.The analysis of ozonevariation mechanism shows that ozone is chemically in quasi-equilibrium except for the polar nightregion where the variation of ozone concentration is under the control of dynamical processes,thatthe oxygen atoms which produce ozone are mainly provided by the photolysis of O_2 in the upperstratosphere and by the photolysis of NO_2 in the lower stratosphere and the troposphere.and thatthe ozone is destroyed mainly by NO_x:the reactions between NO_x and O_3 and the odd oxygen cyclecontribute 80% to more than 90% of the ozone destruction.     

青藏高原春季不同地区臭氧和大气温度变化趋势的差异性

利用1979—2018年太阳后向散射紫外辐射计SBUV(/2)星下点臭氧遥感资料,结合ERA-Interim和MERRA-2大气温度再分析资料,考察青藏高原区域内拉萨和共和两地春季臭氧和大气温度变化趋势的差异性。结果表明拉萨和共和两个地区的臭氧和大气温度逆转趋势均发生于1999年。对比2008年以来青藏高原整体臭氧总量变化速率（4.5 DU/(10 a)),拉萨臭氧总量变化更快,为5.9 DU/(10 a),共和相对较慢,仅为3.7 DU/(10 a);同时,1999年以来拉萨和共和春季下平流层（100~30 hPa）大气温度分别以0.5~1.4℃/(10 a)和0.01~0.9℃/(10 a)速率增加,上对流层(250~175 hPa)大气温度分别以0.2~1.5℃/(10 a)和0.2~1.2℃/(10 a)速率降低。与2008年以来高原整体大气温度变化相比较,均慢于高原下平流层（125~70 hPa) 1~2℃/(10 a)的增温速率,快于高原上对流层（225~175 hPa）0.4~1.1℃/(10 a)的降温速率。两地臭氧与大气温度的相关系数和回归系数计算结果表明,拉萨和共和两个地区1999年以来春季臭氧恢复速率的不同是导致两地同期下平流层-上对流层温度逆转速率差异的重要因子之一。