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1.
重度灰霾(或重霾)条件下,大气气溶胶颗粒物显著衰减到达地表的太阳紫外辐射,对臭氧O3光化学过程形成产生重要影响。通过对2013年12月1-10日发生在长三角地区的一次重霾过程进行详尽分析,结合对流层紫外和可见光模型(TUV)及NCAR箱式模型(MM),探讨气溶胶辐射效应对地面臭氧形成和浓度峰值的影响。研究表明,区域输送、稳定边界层累积和二次气溶胶过程等是导致本次重霾发生的主要原因;重霾条件下,臭氧光化学反应明显减弱,臭氧日峰值明显降低,但光化学反应仍缓慢进行;受各种因素如区域输送、边界层累积效应及二次气溶胶等过程影响,臭氧浓度随细颗粒物PM10浓度升高而缓慢上升。TUV和MM模拟结果与观测吻合较好,模拟结果进一步显示,当气溶胶光学厚度AOD由0.8增加到2.0时,到达地表的紫外辐射衰减63%,地面臭氧峰值浓度降低近83%,表明随着灰霾污染加重,近地层臭氧浓度有所降低。  相似文献   

2.
地面臭氧的变化规律和计算方法的初步研究Ⅰ.紫外波段   总被引：5，自引：1，他引：4  
通过对广州鼎湖山近地面O3、NOx、太阳辐射、气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳辐射的变化规律,详细讨论了紫外波段、不同天气条件地面O3与NOx,光化学反应、气溶胶、光化辐射等之间复杂的关系.用光能量传输与守恒的观点来考虑大气中与紫外辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明,不同情况下计算值与观测值均吻合较好.  相似文献   

3.
本文探讨了百万吨级大气核爆炸对臭氧天然浓度局地短期变化的影响,其中考虑到了核爆炸火球紫外线和γ射线辐射,核爆炸蘑菇云中的光化学反应以及在其上升过程中和稳定之后的漫射扩散等对大气中臭氧生成的影响。本文对北半球平流层臭氧含量在核爆炸尘埃和氮氧化物注入情况下的变化进行了估算,其中考虑到了爆炸尘埃对平流层大气的加热因素和大气天然的自洁作用。  相似文献   

4.
城市化已引起大量痕量气态污染物、气溶胶以及臭氧前体物的人为排放,从而引起区域大气化学循环的扰动变化。在分析国内外研究现状与观测实例的基础上,进一步用辐射模式与化学模式研究了气溶胶对到达地面的光化辐射通量以及臭氧形成的影响,表明气溶胶可显著减小到达地面的光化学辐射通量,减缓光化学反应进程,并进一步抑制臭氧的形成;在目前广州等大城市的污染过程中,高浓度的气溶胶可造成光化学辐射通量衰减高达70%~80%,紫外线的衰减比可见光更明显,在可见光波段随波长增大衰减幅度减小,气溶胶层的存在对短波长激发的光化学过程的影响更加显著。分析说明城市污染大气中光化学反应的生成物与反应物之间存在自抑制过程,在目前的城市群复合污染情况下,气溶胶与臭氧之间的非线性相互作用值得关注。  相似文献   

5.
鼎湖山森林地区臭氧及其前体物的变化特征和分析   总被引：18，自引：2，他引：16  
通过对鼎湖山森林地区近地面O3和NOx浓度、太阳辐射、气象参数等为期一年的观测和资料分析,给出了地面O3和NOx浓度、太阳辐射的变化规律及其相互之间的关系.地面O3、NOx、CO、SO2浓度以及紫外辐射、太阳总辐射等有明显的日变化和季节变化.不同因子对O3的敏感性试验结果表明,晴天和实际天气,O3浓度对NO、NO2浓度的变化最为敏感,其次是水汽、气溶胶,最后是紫外辐射.所有因子的变化均引起O3在湿季比干季更大的变化率,因此在研究臭氧化学和光化学时,应该考虑水汽以及OH自由基的重要作用.对于晴天和实际天气的逐时值和日平均值而言,O3浓度与NO2/NO之间存在很好的正相关关系,比值NO2/NO可以作为判断O3峰值出现的一个指标.O3极值的出现既受NO和NOx影响,也受气象因素(温湿度、云、风、雾、降雨)和辐射的影响.周末O3、NOx浓度及NO2/NO有规律的增大,表明实验地点的大气受到人为污染源的影响.  相似文献   

6.
通过对广州鼎湖山近地面O3、NOx、太阳辐射,气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳可见光辐射的变化规律,详细讨论了可见光波段、不同天气条件地面O3与NOx、光化学反应、气溶胶、可见光辐射等之间复杂的关系.提出以光能量传输与守恒的观点来考虑大气中与可见光辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明:不同情况下,计算值与观测值吻合得均比较一致.  相似文献   

7.
基于2014-2017年西安市环保局臭氧观测资料、泾河气象站总辐射和气象资料以及长安气象站紫外辐射和气象资料,对西安市臭氧污染特征及其与气象条件的关系进行了研究。结果表明:西安市臭氧质量浓度的日变化和月变化均呈明显的单峰形态;日最小值22.2μg/m^3和最大值100.7μg/m^3分别出现在07时和16时;臭氧日最大8 h平均质量浓度(用C8h(O3)表示)月均值最大为148.5μg/m^3,最小为30.0μg/m^3,分别出现在7月和11月。总辐射日最大辐照度、日总辐射曝辐量和日紫外辐射曝辐量与C8h(O3)之间具有显著的正相关关系,并且以日紫外辐射曝辐量与C8h(O3)的相关性最高,表明紫外辐射对近地面臭氧质量浓度的影响更为强烈。日最高气温、平均气温、日照时数和C8h(O3)正相关,风速、相对湿度与C8h(O3)负相关,表明晴空时高温、低湿、小风更有利于近地面臭氧的形成。统计关系显示,在5-8月,当日最高气温大于35℃或日最低相对湿度小于40%时,需要警惕臭氧超标污染的发生。  相似文献   

8.
夹卷对郊外大气边界层内臭氧影响的数值模拟研究   总被引：3，自引：2，他引：3  
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、NOx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（NOX）和可挥发性有机物(VOCS)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。   相似文献   

9.
《高原气象》2021,40(4):954-964
汾渭平原作为中国大气环境治理的第三大重点区域,由挥发性有机物和氮氧化物等前体物排放增加导致光化学反应加剧进而引发的近地面臭氧(O_3)污染已成为迫切需要面对的关键问题。本文基于汾渭平原11个重点城市2015-2019年近地面大气O_3及前体物观测数据结合同期气象监测资料,总结归纳其时空变化特征,利用Global Moran's I和Getis-Ord Gi*指数方法分析空间集聚效应和冷热点区域,运用KZ(Kolmogorov-Zurbenko)滤波方法揭示了不同时间尺度的排放和气象环境对O_3浓度变化的影响。结果表明:近5年汾渭平原O_3污染以轻度为主,超标率逐年增加且夏季最高春季次之,其中6月超标37%以上,前体物中NO_2年际差异不大CO浓度逐年减少。空间分布上,O_3空间集聚特征逐年增强,高浓度聚集区分布在临汾、运城、三门峡和洛阳的三角区域。从气象环境的影响看,O_3浓度主要受到前体物排放及气象条件的季节分量和短期分量影响,贡献率分别达到40%和24%。原始序列及各分量除与气压成负相关外,与气温和日照均呈显著正相关且对不同区域影响较为一致,而相对湿度和风速对各分量的影响具有显著的区域性差异。  相似文献   

10.
人们为什么对大气中大量的臭氧感兴趣呢?其原因在于臭氧对大气的结构、特性,以致于地球上有生命物体有着巨大影响。大气中臭氧的存在使得波长小于290nm的太阳强紫外辐射不能透过大气。另外,臭氧还大量吸收了波长在290-320nm之间的中紫外辐射,波长在320-240nm的近紫外辐射才能通过臭氧层到达地面,但它对生物没有危害。今天无疑可以认为:由于大气中“臭氧盖”的存在,才能使人类免遭紫外辐射的有害影响,人类才能得以生存和发展。大气中臭氧总量的变化(臭氧含量平衡的破坏)影响了平流层中不同高度太阳紫外辐散流入量的分布,这就导致了平流层温度和高层大气  相似文献   

11.
Understanding the chemical links between ozone (O3) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O3/NOy and O3/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.  相似文献   

12.
Abstract

The dependence of ozone formation on the mixing ratios of volatile organic compounds (VOCs) and nitrogen oxides (NOx) has been widely studied. In addition to the atmospheric levels of VOCs and NOx, the extent of photochemical processing of VOCs has a strong impact on ozone levels. Although methods for measuring atmospheric mixing ratios of VOCs and NOx are well established and results of those measurements are widely available, determination of the extent of photochemical processing of VOCs, known as photochemical age (PCA), is difficult. In this article a recently developed methodology for the determination of PCA for individual compounds based on the change in their stable carbon isotope composition is used to investigate the dependence between ozone and VOC or NOx mixing ratios at a rural site in Ontario, Canada, during fall and winter. The results show that under these conditions the variability in VOC mixing ratios is predominantly a result of the varying impact of local emissions and not a result of changes in the extent of atmospheric processing. This explains why the mixing ratio of ozone shows no systematic dependence on the mixing ratios of VOCs or NOx in this environment and at this time of the year.  相似文献   

13.
Photochemical smog characterized by high concentrations of ozone (O3) is a serious air pollution issue in the North China Plain (NCP) region, especially in summer and autumn. For this study, measurements of O3, nitrogen oxides (NOx), volatile organic compounds (VOCs), carbon monoxide (CO), nitrous acid (HONO), and a number of key physical parameters were taken at a suburban site, Xianghe, in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O3 formation and find an optimal way to control O3 pollution. Here, the radical chemistry and O3 photochemical budget based on measurement data from 1-23 July using a chemical box model is investigated. The daytime (0600-1800 LST) average production rate of the primary radicals referred to as ROx (OH + HO2+ RO2) is 3.9 ppbv h-1. HONO photolysis is the largest primary ROx source (41％). Reaction of NO2 + OH is the largest contributor to radical termination (41％), followed by reactions of RO2 + NO2 (26％). The average diurnal maximum O3 production and loss rates are 32.9 ppbv h-1 and 4.3 ppbv h-1, respectively. Sensitivity tests without the HONO constraint lead to decreases in daytime average primary ROx production by 55％ and O3 photochemical production by 42％, highlighting the importance of accurate HONO measurements when quantifying the ROx budget and O3 photochemical production. Considering heterogeneous reactions of trace gases and radicals on aerosols, aerosol uptake of HO2 contributes 11％ to ROx sink, and the daytime average O3 photochemical production decreases by 14％. The O3-NOx-VOCs sensitivity shows that the O3 production at Xianghe during the investigation period is mainly controlled by VOCs.  相似文献   

14.
Temporal Surface Ozone Patterns in Urban Manitoba, Canada   总被引：1，自引：0，他引：1  
This study examined temporal surface ozone patternsfor two urban centres in Manitoba,Canada by analyzing hourly concentrations at theWinnipeg downtown (1995–1999), Winnipegresidential (1995–1999) and Brandon industrial(1998–1999) monitoring sites. The characteristicannual ozone cycle and diurnalcycles for June and December were attributable to: (1) theannual and diurnal solar radiation cycles,(2) temporal variations in the emissions of precursorchemical compounds, in particular the source strength ofnitrogen oxides, (3) temporal variationsin the height of the mixed layer, which determinethe degree of dilution of these emissions byatmospheric dispersion, and (4) an in situvolatile organic compound sensitive photochemicalregime, which resulted in decreased concentrations ofozone in response to increasedconcentrations of nitrogen oxides. Onlyone exceedance of the maximum acceptable level of82 ppb was recorded in the study period; itoccurred at the Brandon monitoring site on June 6, 1999.The sequence of weather and the hourly concentrationsof ozone and nitrogen oxides indicatedthat: (1) ozone fumigation, with the transition fromthe nocturnal boundary layer to the daytime mixed layer, mayhave supplemented photochemical ozone formation duringthe morning hours, and (2) during theevening hours, the post cold-frontal downward flux ofozone rich air, which was in the region dueto atmospheric transport, stratosphere-troposphere-exchangeor, possibly, due to the multiplicityof thunderstorms in the area in lateafternoon – early evening, may have been the main cause ofthis rare exceedance event.  相似文献   

15.
中国地区臭氧前体物对地面臭氧的影响   总被引：5，自引：1，他引：4  
利用GEOS-Chem模式的数值试验结果,研究中国地区NOx和两类VOCs对O3质量浓度分布及其化学机理的影响。研究表明,NOx的减少会使得中国西部O3质量浓度显著降低,但在冬季NOx的减少会使得东北、华北地区O3质量浓度上升。而京津唐地区由于VOCs/NOx比值偏低,不能通过单一减少NOx来控制O3质量浓度。VOCs排放的减少会使得我国东部地区O3质量浓度大幅减少,其中人为VOCs的减少能降低我国东部地面O3质量浓度,而生物VOCs的减少只能在夏秋季有效减少我国东部地区35°N以南区域的地面O3质量浓度。控制地面O3质量浓度时,中国西部主要考虑NOx的减排,东部35°N以北主要考虑AVOCs的减排,而30~35°N应同时考虑AVOCs和BVOCs的减排,在30°N以南的地区,则需要全面考虑NOx和VOCs的减排。  相似文献   

16.
Particulate matter with diameters of 2.5 μm or smaller(PM_(2.5)) and ozone(O_3) are major pollutants in the urban atmosphere. PM_(2.5) can affect O_3 by altering the photolysis rate and heterogeneous reactions. However, these two processes and their relative importance remain uncertain. In this paper, with Nanjing in China as the target city, we investigate the characteristics and mechanism of interactions between particles and O_3 based on ground observations and numerical modeling.In 2008, the average concentrations of PM_(2.5) and O_3 at Caochangmen station are 64.6 ± 47.4 μg m~(-3) and 24.6 ± 22.8 ppb,respectively, while at Pukou station they are 94.1 ± 63.4 μg m~(-3) and 16.9 ± 14.9 ppb. The correlation coefficient between PM_(2.5) and O_3 is -0.46. In order to understand the reaction between PM_(2.5) and O_3, we construct a box model, in which an aerosol optical property model, ultraviolet radiation model, gas phase chemistry model, and heterogeneous chemistry model,are coupled. The model is employed to investigate the relative contribution of the aforementioned two processes, which vary under different particle concentrations, scattering capability and VOCs/NOxratios(VOCs: volatile organic compounds;NOx: nitric oxide and nitrogen dioxide). Generally, photolysis rate effect can cause a greater O_3 reduction when the particle concentrations are higher, while heterogeneous reactions dominate O_3 reduction with low-level particle concentrations.Moreover, in typical VOC-sensitive regions, O_3 can even be increased by heterogeneous reactions. In Nanjing, both processes lead to O_3 reduction, and photolysis rate effect is dominant. Our study underscores the importance of photolysis rate effect and heterogeneous reactions for O_3, and such interaction processes should be fully considered in future atmospheric chemistry modeling.  相似文献   

17.
UV attenuation in the cloudy atmosphere   总被引：1，自引：0，他引：1  
Ultraviolet (UV) energy absorption plays a very important role in the Earth–atmosphere system. Based on observational data for Beijing, we suggest that some atmospheric constituents utilize or transfer UV energy in chemical and photochemical (C&P) reactions, in addition to those which absorb UV energy directly. These constituents are primarily volatile organic compounds (VOCs) emitted from both vegetative and anthropogenic sources. The total UV energy loss in the cloudy atmosphere for Beijing in 1990 was 78.9 Wm−2. This attenuation was caused by ozone (48.3 Wm−2), other compounds in the atmosphere (26.6 Wm−2) and a scattering factor (4.0 Wm−2). Our results for a cloudy atmosphere in the Beijing area show that the absorption due to these other compounds occurs largely through the mediation of water vapor. This fraction of energy loss has not been fully accounted for in previous models. Observations and previous models results suggest that 1) a cloudy atmosphere absorbs 25∼30 Wm−2 more solar shortwave radiation than models predict; and 2) aerosols can significantly decrease the downward mean UV-visible radiation and the absorbed solar radiation at the surface by up to 28 and 23 Wm−2, respectively. Thus, quantitative study of UV and visible absorption by atmospheric constituents involved in homogeneous and heterogeneous C&P reactions is important for atmospheric models.  相似文献   

18.
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.  相似文献   

19.
Hydrogen is named as possible energy carrier for future energy systems. However, the impact of large-scale hydrogen use on the atmosphere is uncertain. Application of hydrogen in clean fuel cells reduces emissions of air pollutants, but emissions from hydrogen production and leakages of molecular hydrogen could influence atmospheric chemistry. This paper combines a global energy system model and a global atmospheric model to explore the range of impacts of hydrogen on atmospheric chemistry. We found that emissions of molecular hydrogen may range from 0.2 up to 10% (or 25-167 Tg hydrogen/yr) for a global hydrogen energy system. The lower end of this range would in fact be equal to current emissions from fossil fuel combustion. Hydrogen energy use leads to a clear decrease in emissions of carbon monoxide, nitrogen oxides and sulphur dioxide, but large-scale hydrogen production from coal may lead to net increase in emissions of nitrous oxide and volatile organic compound. Compared to a reference scenario, this would lead to positive impacts on surface concentrations of carbon monoxide, nitrogen oxides and ozone. However, if hydrogen leakage would not be minimised it leads to an increase in methane lifetimes and a decrease in stratospheric ozone concentrations.  相似文献   

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