夹卷对郊外大气边界层内臭氧影响的数值模拟研究

夹卷是大气边界层与自由大气进行能量和物质交换的重要途径,对边界层动力结构及边界层内温度、水汽和各种污染物浓度有重要影响。利用化学-地表-大气-土壤(CLASS)模式定量评估了夹卷过程对远郊地区大气边界层内臭氧（O₃）浓度的影响并与大气化学反应贡献进行了对比,结合地面O₃、NO_x及边界层高度、位温和比湿等观测资料和再分析资料对CLASS模拟结果进行了定量评估。结果表明:CLASS模式能较为真实地模拟夹卷和大气光化学反应对远郊地区大气边界层臭氧浓度的影响,且当自由大气层内臭氧浓度达到一定值时,两者对边界层内臭氧峰值影响相当。数值试验结果进一步揭示,夹卷对控制氮氧化物（NO_X）和可挥发性有机物(VOC_S)排放源控制效果有重要影响,且当夹卷区内O₃跳跃值增大到一定时,可完全抵消源排放减排控制的效果。本研究旨在表明,为有效控制近地层臭氧浓度,在制定人为污染源减排措施时必须考虑自由大气层臭氧的夹卷贡献。      

京津冀典型工业城市沙河市大气污染特征及来源分析

近些年京津冀地区秋、冬季大气重污染事件频发,工业生产与居民燃煤是大气灰霾污染的重要原因。河北省沙河市是京津冀地区以玻璃制造和加工为主的典型工业城市,本研究选取该城市为研究对象,主要利用2017年1月至12月国控站点的大气环境监测和气象数据,采用扩散模型、潜在源分析等手段,分析了沙河市主要污染物的时空分布特征和污染来源。主要结论有:（1）沙河市首要污染物具有明显季节特征,春季、夏季、秋冬季分别以PM₁₀、O₃、PM_2.5污染为主,季节贡献率分别为43.3%、72.3%、61.5%。（2）受城市大气边界层和排放的共同影响,PM₁₀、PM_2.5、SO₂、NO₂和CO浓度均有剧烈的季节—日变化特征。（3）冬季东北风时PM_2.5、NO₂、SO₂均展现出高浓度和高相关性特征,表明站点可能受东北方向玻璃企业排放影响。同时,站点可能也受城中村散煤燃烧影响。（4）沙河市冬季PM_2.5浓度为143 μg m-3。冬季的一次重污染中硫氧化率SOR、氮氧化率NOR的最高值分别达0.67、0.39,气态污染物的二次转化剧烈,高湿度利于二次粒子的生成。重污染中C(NO₃-)/C(SO₄2-)均值为1.89,推测沙河市NO₂主要来自大型运输车辆和企业的共同排放。（5）本地源是沙河市PM_2.5的主要潜在源区,周边几个重工业城市也有一定贡献。因此本研究建议沙河市PM_2.5的治理除需加强本地污染源的削减和控制外,区域联防联控也十分重要。     

彭州市大气污染物浓度变化特征研究

本文利用2017年彭州市大气污染物(SO₂、NO₂、O₃、CO、PM₁₀、PM_2.5)小时浓度数据并结合地面气象观测资料,统计分析了该地区大气污染物浓度的演变规律及影响因素。结果表明:该地区细粒子(PM₁₀和PM_2.5)污染较为严重,O₃次之,其它污染物浓度水平则低于国家新二级标准限值。观测期间,各污染物浓度表现出明显的日变化与季节变化,其中SO₂、O₃呈单峰型日变化,NO₂、CO和细粒子则呈双峰型日变化;污染物浓度的季节变化基本表现为冬高夏低、春秋次之的变化特征(O₃为夏高冬低),并且固态污染物(PM₁₀、PM_2.5)与气态污染物(NO₂、CO)之间有显著的相关性。在污染物浓度与气象要素相关性分析中表明,湿度对于污染物浓度的影响整体上要弱于温度和风速,除了O₃与温度、风速呈正相关外,其它污染物与两者均呈负相关。除此以外,风向对于当地各种大气污染物的积累与清除也有直接的影响。      

闪电产生氮氧化物对青藏高原臭氧低谷形成的影响

为了进一步了解青藏高原闪电的产生氮氧化物（LNO_x）经由光化学反应对O₃浓度变化及夏季O₃低谷形成的可能影响,本文利用2005~2013年由OMI卫星得到的对流层NO₂垂直浓度柱（NO₂ VCD）、O₃总浓度柱（TOC）和O₃廓线以及星载光学瞬变探测器OTD和闪电成像仪LIS获取的总闪电数资料,对青藏高原和同纬度长江中下游地区的TOC和NO₂ VCD月均值时空分布特征、闪电与NO₂ VCD的相关性和O₃的垂直分布特征及其与LNO_x的关系进行了对比分析。结果表明,青藏高原的O₃低谷主要出现在夏季和秋季,其TOC值比同纬度长江中下游地区低约10~15 DU（Dobson unit）。青藏高原NO₂VCD总体较小,表现为夏高冬低的分布特征。青藏高原夏季O₃浓度受南亚高压的影响总体呈减小趋势,但因强雷暴天气导致对流层中上部LNO_x浓度升高,并随强上升气流向对流层顶输送,同时通过光化学反应使O₃浓度增加,缩小了青藏高原和同纬度地区的O₃浓度差,减缓了O₃总浓度的下降,抑制了夏季O₃低谷的进一步深化。     

2016—2021年呼和浩特市大气臭氧浓度变化特征分析

随着城市的发展,大气O₃的污染不容忽视。文章以呼和浩特市2016—2021年大气O₃浓度为研究对象,结合同期气象数据,采用相关分析等数理统计方法,分析了呼和浩特市大气O₃浓度年际、季节以及月份动态特征规律,探讨大气O₃浓度与关键影响气象要素之间的关系。结果表明：呼和浩特市大气O₃作为空气首要污染物的天数在逐年增加;6年间O₃浓度年际变化呈下降趋势,以-0.02μg·m^-3的年均速率变化;O₃浓度季节变化明显,夏季最高,其次是春季、秋季、冬季;O₃月平均浓度呈倒“V”形单峰变化,主要在6—8月浓度较高,12月浓度最低,O₃浓度超标日主要集中在6、7月;O₃浓度与气象要素呈密切关系,在非采暖期,O₃-8 h浓度与日平均气温和日照时数具有正相关趋势,与日平均气压、日平均相对湿度以及平均风速具有负相关趋势,降水对大气O₃     

陕西初夏臭氧污染事件及其成因

关中平原至陕北黄土高原海拔渐次升高,大气污染物分布、排放源和下垫面特征均有较大变化。利用陕西省由南至北西安、延安、榆林三市环境空气质量监测数据和气象观测数据及NCEP再分析产品,对2018年春末夏初(5月下旬至6月初)连续两次臭氧(O₃)污染过程开展研究。结果表明：三市O₃质量浓度(用C(O₃)表示)皆呈昼高夜低的日变化特征;三市日均C(O₃)表现出随海拔高度升高而增加的现象,即榆林最高,延安次之,西安最低,较高海拔的黄土高原高背景O₃可能是榆林、延安C(O₃)较高的重要原因。两次O₃污染发生在大气环流由春季型向夏季型过渡阶段,陕西处于500 hPa暖性高脊、850 hPa偏南风主导、地面静稳晴热的天气形势下,有利于光化学O₃生成以及大气低层O₃区域输送,其中西安的光化学生成对其日间C(O₃)升高作用最明显。三市温度和C(O₃)呈正相关,相同温度下...     

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。     

2020年1—3月四川地区大气污染物变化特征分析

利用2018-2020年中国环境监测总站全国城市空气质量实时发布平台公布的监测点数据以及中国气象局气象站点的同期地面观测资料,采用相关性分析的方法对2020年1-3月四川地区大气污染物的变化特征进行分析。结果表明：由于2020年1-3月人为排放源管控政策的实施,成都、绵阳、宜宾和攀枝花的NO₂和PM₁₀浓度相比2018-2019年同期平均下降幅度达到30%,而O₃质量浓度在四座城市的日均值却分别上升了15.21%、10.32%、5.03%和0.42%。同时,O₃与相对湿度成负相关关系,与温度、风速和降水成正相关关系且相关系数都超过了0.7。O₃的反常增长不仅是受到气象要素的影响,较低的氮氧化物和PM₁₀浓度也间接维持了O₃的存在。严格的污染物排放控制措施对主要污染物排放影响较大,但对臭氧等次生污染物的影响较小,次生污染物污染的防治依旧面临严峻挑战。     

华南区域大气成分数值模式GRACEs预报性能评估

利用2016-2019年广东省国控站实况监测数据对华南区域大气成分数值模式系统(GRACEs)预报性能进行了综合评估。除空气质量指数AQI外,重点对PM_2.5、O₃及NO₂进行了分析评估。(1) 模式预报性能存在年际差异,对各要素的预报值总体偏低。(2) 模式预报能较好地反映空气质量的空间分布,PM_2.5中心在珠三角西北部,而O₃-8 h高值区在珠三角核心区和粤东沿海,但模式对O₃-8 h高值区存在显著预报低估现象。(3)模式可较好地模拟出PM_2.5月变化的单峰型特征和O₃-8 h月变化双峰型特征,但模式对AQI的秋冬季主峰值和春季次峰值的预报存在低估,分别与模式对O₃-8 h、PM_2.5的低估有关。(4) 模式能较好体现O₃的午后峰值和NO₂双峰值的日变化规律;模式对O₃前体物NO₂的预报偏差,有可能是导致随后几小时对O₃浓度预报偏差的重要原因。(5) 日平均浓度预报效果检验显示模式可较好预测AQI和3种污染物的变化趋势,但对夏秋季高O₃-8 h浓度预报显著偏低;模式对轻度污染及以上等级预报能力偏低,亟需提升模式对污染天气的预报能力。      

南京北郊 O3、NO2和 SO2变化特征分析

利用 2008年1-12月南京北郊O₃、NO₂及SO₂质量浓度连续观测资料,分析了南京北郊气体污染物(O₃、NO₂、SO₂) 的质量浓度变化规律。结果表明：南京北郊O₃浓度夏季较高,日变化曲线呈单峰型,NO₂和SO₂浓度夏季较低,日变化曲线呈双峰型,NO₂与O₃的日变化呈现负相关关系,该地区SO₂浓度整体较高,夏季周末效应NO₂和SO₂较O₃更明显。     

Impact of precursor levels and global warming on peak ozone concentration in the Pearl River Delta Region of China

The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.     

On the Spatial Distribution and Seasonal Variation of Lower-Troposphere Ozone over Europe

Surface ozone data from 25 Europeanlow-altitude sites and mountain sites located between79°N and 28°N were studied. The analysiscovered the time period March 1989–February 1993.Average summer and winter O₃ concentrations inthe boundary layer over the continent gave rise togradients that were strongest in the north-west tosouth-east direction and west-east direction, respectively. WintertimeO₃ ranged from 19 to 27 ppbover the continent, compared to about 32 ppb at thewestern border, while for summer the continentalO₃ values ranged between 39 and 56 ppb and theoceanic mixing ratios were around 37 ppb. In the lowerfree troposphere average wintertime O₃ mixingratios were around 38 ppb, with only an 8 ppbdifference between 28°N and 79°N. For summerthe average O₃ levels decreased from about 55 ppbover Central Europe to 32 ppb at 79°N. Inaddition, O₃ and O_x(= O₃ + NO₂)in polluted and clean air were compared. Theamplitudes of the seasonal ozone variations increasedin the north-west to south-east direction, while thetime of the annual maximum was shifted from spring (atthe northerly sites) to late summer (at sites inAustria and Hungary), which reflected the contributionof photochemical ozone production in the lower partsof the troposphere.     

华南地区春季平流层入侵对对流层低层臭氧影响的模拟研究

利用中尺度大气化学模式WRF/Chem对2013年3月6日华南地区一次平流层入侵事件及其对对流层低层臭氧的影响进行模拟研究。通过加入UBC（Upper Boundary Condition）上边界处理方案,弥补WRF/Chem模式未考虑平流层臭氧化学反应的不足。结合臭氧探空廓线资料、地面O₃、CO、NO_x、相对湿度、温度和风速等观测资料以及再分析资料对模拟结果进行定量评估,结果表明模式能较为真实地模拟本次平流层入侵过程。模拟分析进一步揭示:（1）副热带高空急流是本次平流层入侵的主要原因。当华南地区处在副热带急流入口区左侧下沉区域时,平流层入侵将富含臭氧的干燥空气输送到对流层中低层。（2）本次平流层入侵对对流层低层臭氧收支有重要影响,导致香港地区近地层臭氧体积混合比浓度明显上升,如塔门站夜间臭氧浓度升高21.3 ppb（1 ppb=1×10-9）。地面气象场和化学物种的分析进一步确认了平流层入侵的贡献。（3）采用动力学对流层顶高度时零维箱式模型和Wei公式计算得到的平流层入侵通量相当,分别为-1.42×10-3 kg m-2 s-1和-1.59×10-3 kg m-2 s-1,这一结果与前人研究相吻合,且与采用热力学对流层顶高度计算所得到的结果具有可比性。     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.     

Subsonic aircraft and ozone trends

Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO _x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO _x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO _x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.     

Ozone Production Efficiency in Savanna and Forested Areas during the EXPRESSO Experiment

NO, NO_x, NO_y and O₃ have been measuredduring the airborne EXPRESSO experiment, November 96,which took place near Bangui (Central Africa) at thebeginning of the dry season. This period correspondsto an intense burning activity. Chemical andphotochemical characteristics of the planetaryboundary layer, which corresponds most of the time tothe monsoon layer, and the Harmattan layer, which issituated above the latter, have been studied forsavanna as well as rain forest areas. These two layersare very different when considering the chemicalcomposition (especially for ozone and NO_z) andthe photochemical age.The relationship of photochemical ozone productionversus photochemical NO_x oxidation products hasbeen investigated. Results indicate an ozoneproduction efficiency (OPE) ranging from 6.3 to 14.8in the planetary boundary layer. Thus, this layer ischaracteristic of a photochemically young and activeair mass. In this layer, the ozone potentialproduction increases with the air mass photochemicalage. On the other hand, the Harmattan layer shows anOPE ranging from 4.6 to 7.4. These values arecharacteristic of photochemically well-aged airmasses. In this layer, the ozone potential productionseems to be exhausted with values around 4.0 (i.e., 4ozone molecules produced for each NO_x moleculeemitted).     

Measurement of PAN in the Polluted Boundary Layer and Free Troposphere Using a Luminol-NO2 Detector Combined with a Thermal Converter

Peroxyacetyl nitrate (PAN,CH³C(O)O₂NO₂) has been measured inthe polluted boundary layer and free troposphere by thermal conversion tonitrogen dioxide (NO₂) followed by detection of thedecomposition product with a Scintrex LMA-3 NO₂-luminolinstrument. Following laboratory tests of the efficiency of PAN conversionand investigations of possible interferences, the technique was evaluated atthe West Beckham TOR (Tropospheric Ozone Research) Station near the northNorfolk coast in Eastern England between September 1989 and August 1990. PANmeasured by the new technique was reasonably well correlated with PANrecorded using electron capture gas chromatography (EC/GC). PAN was alsowell correlated with ozone (O³) in the summer months. Springand autumn episodes of simultaneously high concentrations of PAN andO³ were examined in conjunction with air parcelback-trajectories and synoptic- and local-scale meteorology in a study ofthe sources of photooxidants on the east coast of England. Spring-timemeasurements of PAN made in the free troposphere in a light aircraft ataltitudes up to 3.1 km showed the presence of 0.54 and 0.26 ppbv PAN inpolar maritime and mid-latitude oceanic air masses, respectively. Thetechnique is particularly suited to airborne applications because potentialinterferences are minimised and the frequency of measurements is higher thangenerally achieved with EC/GC methods.     

What Causes the Springtime Tropospheric Ozone Maximum over Northeast Asia？

Scientists have long debated the relative importance of tropospheric photochemical production versus stratospheric influx as causes of the springtime tropospheric ozone maximum over northern mid-latitudes. This paper investigates whether or not stratospheric intrusion and photochemistry play a significant role in the springtime ozone maximum over Northeast Asia,where ozone measurements are sparse.We examine how tropospheric ozone seasonalities over Naha(26°N,128°E),Kagoshima(31°N,131°E),and Pohang(36°N,129°E),which are located on the same meridional line,are related to the timing and location of the jet stream.The ozone seasonality shows a gradual increase from January to the maximum ozone month,which corresponds to April at Naha,May at Kagoshima,and June at Pohang.In order to examine the occurrence of stratospheric intrusion,we analyze a correlation between jet stream activity and tropospheric ozone seasonality.From these analyses,we did not find any favorable evidence supporting the hypothesis that the springtime enhancement may result from stratospheric intrusion.According to trajectory analysis for vertical and horizontal origins of the airmass,a gradual increasing tendency in ozone amounts from January until the onset of monsoon was similar to the increasing ozone formation tendency from winter to spring over mainland China,which has been observed during the build-up of tropospheric ozone over Central Europe in the winter-spring transition period due to photochemistry.Overall,the analyses suggest that photochemistry is the most important contributor to observed ozone seasonality over Northeast Asia.     

Responses of the tropospheric ozone and odd hydrogen radicals to column ozone change

The response of tropospheric ozone to a change in solar UV penetration due to perturbation on column ozone depends critically on the tropospheric NO _x (NO+NO₂) concentration. At high NO _x or a polluted area where there is net ozone production, a decrease in column ozone will increase the solar UV penetration to the troposphere and thus increase the tropospheric ozone concentration. However, the opposite will occur, for example, at a remote oceanic area where NO _x is so low that there is net ozone destruction. This finding may have important implication on the interpretation of the long term trend of tropospheric ozone. A change in column ozone will also induce change in tropospheric OH, HO₂, and H₂O₂ concentrations which are major oxidants in the troposphere. Thus, the oxidation capacity and, in turn, the abundances of many reduced gases will be perturbed. Our model calculations show that the change in OH, HO₂, and H₂O₂ concentrations are essentially independent of the NO _x concentration.