1994-2006年长江三角洲和东北平原酸性气体浓度变化

 利用长江三角洲和东北平原地区大气本底站的二氧化硫（SO2）和氮氧化物（NOx）历史资料和近期取得的观测数据,探讨两个地区人为排放对这些气候相关酸性气体的不同贡献。从两种酸性气体过去和现在的浓度水平,估算了它们在两个地区的增长率,比较了NOx与SO2比值的不同变化趋势。结果表明,早在20世纪90年代中期,长江三角洲酸性气体污染水平已经较高,其后主要是NOx浓度显著升高,从而使该地区成为硫和氮污染并重的地区;东北平原酸性气体过去浓度很低,但这些气体以很高的速率增长,虽然目前浓度水平仍然比较低,但未来形势不容乐观。     

1994-2006年长江三角洲和东北平原酸性气体浓度变化

利用长江三角洲和东北平原地区大气本底站的二氧化硫（SO2）和氮氧化物（NOx）历史资料和近期取得的观测数据,探讨两个地区人为排放对这些气候相关酸性气体的不同贡献。从两种酸性气体过去和现在的浓度水平,估算了它们在两个地区的增长率,比较了NOx与SO2比值的不同变化趋势。结果表明,早在20世纪90年代中期,长江三角洲酸性气体污染水平已经较高,其后主要是NOx浓度显著升高,从而使该地区成为硫和氮污染并重的地区;东北平原酸性气体过去浓度很低,但这些气体以很高的速率增长,虽然目前浓度水平仍然比较低,但未来形势不容乐观。     

Characterization of Organic Aerosol at a Rural Site in the North China Plain Region: Sources,Volatility and Organonitrates

The North China Plain(NCP) is a region that experiences serious aerosol pollution. A number of studies have focused on aerosol pollution in urban areas in the NCP region; however, research on characterizing aerosols in rural NCP areas is comparatively limited. In this study, we deployed a TD-HR-AMS(thermodenuder high-resolution aerosol mass spectrometer) system at a rural site in the NCP region in summer 2013 to characterize the chemical compositions and volatility of submicron aerosols(PM_1). The average PM_1 mass concentration was 51.2 ± 48.0 μg m~(-3) and organic aerosol(OA) contributed most(35.4%) to PM_1. Positive matrix factorization(PMF) analysis of OA measurements identified four OA factors, including hydrocarbon-like OA(HOA, accounting for 18.4%), biomass burning OA(BBOA, 29.4%), lessoxidized oxygenated OA(LO-OOA, 30.8%) and more-oxidized oxygenated OA(MO-OOA, 21.4%). The volatility sequence of the OA factors was HOA BBOA LO-OOA MO-OOA, consistent with their oxygen-to-carbon(O:C)ratios. Additionally, the mean concentration of organonitrates(ON) was 1.48-3.39 μg m~(-3), contributing 8.1%–19% of OA based on cross validation of two estimation methods with the high-resolution time-of-flight aerosol mass spectrometer(HRToF-AMS) measurement. Correlation analysis shows that ON were more correlated with BBOA and black carbon emitted from biomass burning but poorly correlated with LO-OOA. Also, volatility analysis for ON further confirmed that particulate ON formation might be closely associated with primary emissions in rural NCP areas.     

北京地区严重大气污染的气象和化学因子

利用北京３２５ ｍ 气象塔进行了大气污染物臭氧、氮氧化物、一氧化碳和气象要素的同步观测, 对影响大气污染的气象和化学因子进行了分析,探讨大气污染物变化的规律, 为城市空气污染预报提供理论基础。     

Value-Added Products Derived from 15 Years of High-Quality Surface Solar Radiation Measurements at Xianghe,a Suburban Site in the North China Plain

Surface solar radiation(SSR) is a key component of the energy budget of the Earth’s surface, and it varies at different spatial and temporal scales. Considerable knowledge of how and why SSR varies is crucial to a better understanding of climate change, which surely requires long-term measurements of high quality. The objective of this study is to introduce a value-added SSR dataset from Oct 2004 to Oct 2019 based on measurements taken at Xianghe, a suburban site in the North China Plain; two va...     

华北平原夜间对流性天气对地面O3混合比的抬升效应

2013年6—9月在河北省固城站观测到多次夜间对流性天气伴随地面O₃混合比快速抬升的过程,并引起次日清晨到中午O₃混合比升高。大多数对流过程中,O₃混合比在半小时内升高至60×10-9～80×10-9,同时NO_x等反应性气体混合比下降,θ_se值降低,说明下沉气流将高空气团带到地面,造成了O₃混合比的升高。通过再分析资料得到下沉气团基本来源于对流层中下层,这一结论与当地进行的一次飞机观测结果吻合。多数对流过程中固城站和北京城区地面O₃混合比和θ_se值有相同的变化趋势和程度。根据观测结果,推测华北地区在夏季和初秋时,对流层中下层存在O₃高值区,混合比约为60×10-9～80×10-9。对流性天气对地面O₃抬升的影响区域与对流系统的影响范围有关,可达到中尺度范围。华北地区光化学污染严重,对流性天气引起的地面O₃混合比抬升程度比较强,对环境的影响值得关注。     

2013年夏季华北乡村站点固城大气氨变化特征

利用2013年6—8月河北省定兴县固城站的NH3连续高时间分辨率观测数据,分析了NH3体积分数水平、变化特征和影响因素。结果表明：2013年夏季固城站NH3小时平均体积分数变化范围为0.9×10-9~862.9×10-9,平均体积分数为43.9×10-9±65.9×10-9。观测期间PM2.5中NH4+平均质量浓度为 (19.77±33.24) μg·m-3。2013年夏季固城站NH3和NH4+质量浓度有较好的相关性,且浓度明显高于华北地区城市站点,说明由于农业施肥等活动导致固城站大气NH3和NH4+质量浓度水平显著提高。夏季NH3体积分数有明显日变化且呈单峰特征。2013年夏季固城站硫氧化率和氨转化率较高,说明SO2和NH3转化为SO42-和NH4+的速率较大。华北地区应加大对由农业活动造成的NH3排放的控制力度,以降低区域二次气溶胶污染。     

冷锋天气大气边界层内臭氧及 氮氧化物的观测研究

利用北京325 m气象塔作为高空平台,于1997年10月观测到一次冷锋过程大气边界层内O3及NOx体积分数的变化,研究了O3及NOx体积分数与气象要素之间的关系,着重讨论了冷锋过境前后O3及NOx的体积分数变化及其与输送过程的关系。研究表明:北京大气边界层中下层存在明显的O3体积分数垂直梯度,O3的垂直输送与风速及温度梯度密切相关。冷锋过程有利于高层O3向低层输送,使O3体积分数垂直梯度明显减小,并使NOx体积分数显著降低。     

Background ozone and anthropogenic ozone enhancement at niwot ridge,Colorado

The mixing ratios for ozone and NO_x (NO+NO₂) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NO_x levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NO_x from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NO_x mixing ratio. For NO_x mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NO_x]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NO_x]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O₃ in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NO_x levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NO_x]0.2 ppbv, 0.3 ppbv[NO_x]0.7 ppbv and 1 ppbv[NO_x]. These monthly ozone averages reflect the seasonal ozone dependence on the NO_x level.     

Particulate sulfate levels at a rural site in Israel

Ambient particulate sulfate measurements have been intermittently performed at a rural site in Israel over a period of more than two years. Concurrent measurements of ambient pollutants (SO₂, NO–NO_x, and O₃), as well as meteorological data, were also carried out. The daily data included four particulate sulfate samples representing four successive 6 h accumulating periods. The measured concentrations of sulfate ions ranged from a low 2 g m^-3 observed during the winter season to a high of >50 g m^-3 obtained during the summer. Little correlation was obtained between the sulfate concentration and either O₃ or SO₂, although sulfate and O₃ showed a similar diurnal and annual trend. Based on the data distribution and on a photochemical model, it was concluded that a large part of the particulate sulfate observed at the eastern coast of the Mediterranean Sea must be related to long-range transport from distant sources.     

近地面臭氧研究进展

近地面臭氧是空气中氮氧化物和挥发性有机物发生光化学反应的产物,其浓度与气象条件密切相关。晴天少云、紫外辐射较强、温度较高、相对湿度较低以及风速较小的天气,均有利于臭氧的生成,其中紫外辐射是产生臭氧最关键的因素。臭氧前体物（氮氧化物和挥发性有机物）的浓度及其比值是影响近地面臭氧浓度的另外三个重要因素。我国大多数城市的O3处于VOC控制区,即NOx浓度的增加会引起O3浓度的降低,而VOCs浓度的增加则会使其浓度升高。因而VOC源解析问题成为近年来O3研究的一个热点问题。同时,由于气溶胶可以直接吸收、散射太阳紫外辐射、短波辐射以及大气长波辐射,因此气溶胶的存在会影响大气中光化学反应的进程,从而影响臭氧的光化学生成,气溶胶对近地面臭氧的影响已成为目前大气环境的前沿课题。     

北京奥运会期间CBM-Z化学机制的模拟应用

利用CBM-Z化学机制模拟了中国科学院大气物理研究所气象塔站在北京奥运会期间高臭氧时段O3浓度的日变化,评估了气象条件、北京奥运会加强控制措施以及O3前体物浓度对近地面O3生成的影响。结果表明:(1)CBM-Z化学机制较好地模拟了北京奥运会期间典型时段气象塔站O3、NO、NO2日变化特征。(2)有利于局地高臭氧事件发生的气象条件非常相似;北京奥运会加强控制措施的实施显著减少了NOx及VOCs的排放量,导致近地面O3浓度的明显下降。(3)奥运会期间VOCs和CO是影响气象塔站O3生成量的关键因素。     

Estimates of the Chemical Budget for Ozone at Waliguan Observatory

Waliguan Observatory (WO) is an in-land Global Atmosphere Watch (GAW) baseline station on the Tibetan plateau. In addition to the routine GAW measurement program at WO, measurements of trace gases, especially ozone precursors, were made for some periods from 1994 to 1996. The ozone chemical budget at WO was estimated using a box model constrained by these measured trace gas concentrations and meteorological variables. Air masses at WO are usually affected by the boundary layer (BL) in the daytime associated with an upslope flow, while it is affected by the free troposphere (FT) at night associated with a downslope flow. An anti-relationship between ozone and water vapor concentrations at WO is found by investigating the average diurnal cycle pattern of ozone and water vapor under clear sky conditions. This relationship implies that air masses at WO have both the FT and BL characteristics. Model simulations were carried out for clear sky conditions in January and July of 1996, respectively. The chemical characteristics of mixed air masses (MC) and of free tropospheric air masses (FT) at WO were investigated. The effects of the variation in NO_x and water vapor concentrations on the chemical budget of ozone at WO were evaluated for the considered periods of time. It was shown that ozone was net produced in January and net destroyed in July for both FT and MC conditions at WO. The estimated net ozone production rate at WO was –0.1 to 0.4 ppbv day^–1 in FT air of January, 0.0 to 1.0 ppbv day^–1 in MC air of January, –4.9 to –0.2 ppbv day^–1 in FT air of July, and –5.1 to 2.1 ppbv day^–1 in MC air of July.     

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.     

北京上甸子本底站2003年秋冬季痕量气体浓度变化特征

2003年9月至2004年2月在北京上甸子区域大气污染本底监测站(117°07′E,40°39′N,海拔293.9 m)开展了对大气中痕量气体的连续在线监测,获得了NO、NO2、SO2、CO和O3等气体组分的变化特征、变化规律和浓度水平。初步分析表明,NO、NO2、SO2、CO和O3有明显的日变化和月变化特征。O3浓度在秋季较高,冬季较低;NO、NO2和SO2冬季出现浓度高值。探讨了O3和痕量气体与气象因子的关系。O3与NO、NO2、NOx、CO和SO2皆为负相关,CO与NOx和SO2具有较好的相关性。本底站痕量气体浓度与同期观测的城区污染物浓度相比其变化趋势基本呈同位相。     

北京秋季城区和近郊近地层O3特征

北京十三陵地区出现O3高值,一直是人们所关心的环境问题,秋季是北京地区高O3浓度季节,为此2001年9月7～17日在北京城区舞蹈学院楼顶和十三陵地区昭陵进行了一次以O3为主,并结合其前体物的综合比对实验.对北京城区和郊区地面O3特征进行了比对分析,目的是了解北京秋季近地面城乡O3差异的原因.结果表明郊区O3浓度日均值普遍大于城区O3日均值,城区和郊区白天O3浓度接近,城乡O3平均浓度的差异是由于不同天气条件下城区夜间地面O3浓度很低,有时甚至接近于零,而郊区夜间O3依然维持一定浓度.其主要原因在于城区有较多的污染排放源,致使夜间NO浓度维持相对高值,其通过滴定过程大量消耗O3所致.观测中发现无论城区或郊区当小时平均NO浓度大于10×10-9(体积混合比)时,相应小时平均O3浓度接近于零.NO2/NO低值区对应于地面O3低浓度,城区夜间NO2/NO值低于郊区.由此可见城区O3日平均值较低和城区空气污染重于郊区有密切关系.     

地面臭氧光化学过程规律的初步研究

给出了1996年夏季在广东肇庆鼎湖山对光化辐射、地面O3、NO、NO2浓度的观测结果,对影响地面O3、NO、NO2的主要因子进行了分析。晴天,地面O3、NO、NO2浓度有明显的日变化;阴天,它们的日变化比较复杂。晴天和阴天,在lnQUVB/m和lnQvis/m(其中QUVB为紫外B辐射,Qvis为可见光辐射,m为大气质量)与地面O3、NO,NO2浓度、整层大气水汽含量(q1、q2、q3、q4)之间存在着很好的相关关系。利用得到的关系式计算了地面O3浓度,在紫外和可见光波段,计算值与观测值符合得都比较好。     

华北平原对流风暴的个例分析

应用较详细的卫星云图,多普勒雷达和探空资料对一次强对流风暴进行了综合分析研究,得出了具有一定特色的对流单体组合与垂直结构图象。     

2013年1月华北地区重雾霾过程及其成因的模拟分析

2013年1月11~14日,华北地区经历重雾霾过程。为了探讨其形成原因,利用大气化学模式系统Weather Research and Forecasting(WRF)-Chem模拟2013年1月华北地区气溶胶的时空变化。模拟的能见度、气象要素(温度、湿度、降水、风速和风向)以及细颗粒物(PM2.5,大气中直径≤2.5μm的颗粒物)地表浓度的时间变化与近地面观测值都较为吻合。模拟结果表明,1月11~14日,细颗粒物高值分布于河北省南部和东部、天津地区以及北京地区,其日均值约为400~500μg m–3。通过与历史气候数据比较发现,2013年1月10~15日华北地区的气象条件表现为较大的相对湿度正距平(20%~40%)以及风速的负距平(-1 m s–1)。北京站点的探空数据还表明,在1月11~13日期间,垂直方向上,1 km以下的大气中存在明显的逆温层,并且湿度保持较高的值(80%~90%)。模拟结果表明,1月11~14日,近地面南向风和东向风将水汽输送到华北地区,上层大气(850hPa)的西北风则将沙尘输送到华北地区。以上气象条件有利于气溶胶的吸湿增长和浓度的聚集。硝酸盐的收支分析表明,在北京地区,与1~9日相比,10~14日夜间化学生成和传输的显著增加都贡献于硝酸盐浓度,是重雾霾形成的主要原因。     

Comparison of column-integrated aerosol optical and physical properties in an urban and suburban site on the North China Plain

The column-integrated optical properties of aerosol in Beijing and Xianghe, two AErosol RObotic NETwork(AERONET)sites situated on the North China Plain(NCP), are investigated based on Cimel sunphotometer measurements from October2004 to June 2012. The outstanding feature found is that the seasonal medians of aerosol optical depth(AOD) at the two stations are in good agreement. The correlation coefficients and the absolute differences between AOD at the two stations are larger than 0.84 and less than 0.05, respectively. Good agreement in AOD at these two sites(one urban and the other suburban; 70 km apart) indicates that aerosol pollution in the Greater Beijing area is regional in nature. However, we find significant differences in the absorption ?Angstr ¨om Exponent(AAE), the real and imaginary part of the refractive index, and thereby the single scattering albedo(SSA), and the difference is seasonally dependent. The feature is found to be more prominent in fall when the fine-mode fraction(FMF) and fine-mode effective radius are significantly different at the two stations,besides the parameters mentioned above. The SSA in Beijing at four wavelengths shows lower values as compared to those in Xianghe, although the difference is not significant in some cases. Significant differences in AAE and fine-mode effective radius indicate that there are differences in aerosol physical and chemical properties in urban and suburban regions on the NCP.