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Using the “lumped mechanism” and “counting species” methods, we developed a condensed gas-phase chemical model based on a
simplified one. The modified quasi-steady-state approximation (QSSA) scheme and the error redistribution mass conservation
technique are adopted to solve the atmospheric chemistry kinetic equations. Results show that the condensed model can well
simulate concentration variations of gas species such as SO2, NOX, O3, H2O2 and conversion rates of SO2 and NOX transformation to H2SO4 and HNO3. These results are in good agreement with those from the simplified model. The conversion rates of SO2 and NOX under different initial concentrations and meteorological conditions are computed, and the results can be directly applied
to regional acid deposition model. 相似文献
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CHAO Na JI Dong-Sheng CHEN Jia-Shan XIN Jin-Yuan HU Bo WANG Yue-Si WANG Hui MENG Ze 《大气和海洋科学快报》2014,(4):340-345
Measurements of gaseous pollutants （03, NOx, SO2, and CO） were conducted at Dinghushan background station in southern China from January to December 2013. The levels and variations of O3, NOx, SO2, and CO were analyzed and their possible causes discussed. The annual average concentrations of 03, NOx, SO2, and CO were 24.6 ± 23.9, 12.8 ± 10.2, 4.0 ± 4.8, and 348 ± 185 ppbv, respectively. The observed levels of the gaseous pollutants are comparable to those at other background sites in China. The most obvious diurnal variation of 03 was observed in autumn, with minima in the early morning and maxima in the afternoon. The diurnal variations of SO2 showed high values during the day. The diurnal cycles of NOx showed higher values in the morning and lower values during the night. Higher CO concentrations were observed in spring followed by winter, autumn, and summer. Biomass burning, in combination with the transport of regional pollution, is an important source of CO, SO2, and NOx in spring and winter. Backward trajectories were calculated and analyzed together with corresponding pollutant concentrations. The results indicate that air masses passing over polluted areas are responsible for the high concentrations of gaseous pollutants at the Dinghushan background station. 相似文献
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The gas-phase degradation of NH3 in the atmosphere still has many uncertainties. One of them is the possible isomerisation of NH2O to NHOH, as indicated by kinetic studies. Since NH2O is formed during the gas-phase oxidation of ammonia in the troposphere, this reaction can potentially influence the subsequent production of N2O and NOx. So far, the isomerisation has never been implemented into current chemical schemes describing the atmospheric gas-phase degradation of NH3 and its atmospheric relevance has never been assessed. The N2O yield from NH3 degradation is calculated to be in the range of 10–43 %. It depends on the NO2 and O3 concentrations, but is independent of the NH3 concentration. Compared with the results from recent literature, the N2O yield derived from the new mechanism is 20–80% lower, implying a smaller global N2O source strength of 0.4 Tg yr- 1. The production of NH2SO2 seems to be less important for the atmospheric degradation of NH3. NH3 oxidation is a sink for NOx at NOx mixing ratios of more than about 1 ppb and a source at lower NOx burdens. 相似文献
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本文从实验气溶胶样品、实验技术和分析方法三个方面对以往的实验室研究结果进行综合分析, 归纳总结出适合东亚地区沙尘气溶胶的非均相吸附系数γ的参考值, 并利用区域大气化学模式, 模拟研究了非均相吸附系数γ的不确定性对东亚地区沙尘气溶胶非均相化学过程的影响。为了研究非均相反应对γ的敏感性, 针对其中四种物质(HNO3、N2O5、O3和SO2) 的γ上限值和下限值, 分别进行了T-up (上限值) 和T-low(下限值)两个敏感实验; 针对相对湿度对HNO3和N2O5非均相吸附系数的影响进行了T-rh敏感实验。模拟结果与观测资料进行了对比分析, 结果表明模式可以比较好地反映气态物质、气溶胶浓度的演变过程和非均相反应过程。考虑非均相反应后模拟的硫酸盐和硝酸盐浓度与观测值更接近一些。采用γ参考值的模拟结果总体上比采用γ上限值和γ下限值更合理, 把γ系数作为相对湿度的函数来处理比作为常数处理更合理。沙尘气溶胶通过非均相化学反应, 可以使模拟区域内SO2、NOx和O3的平均浓度下降, 使硫酸盐和硝酸盐颗粒物浓度增加, 采用γ参考值计算得到3 km以下的上述物质的变化率分别为－3.44%、－5.92%、－1.75%、5.22%和23.25%, 显示沙尘表面非均相化学反应对大气化学成分特别是气溶胶有较大的影响; 不同γ取值对上述物质变化率有一定影响, 其中对硝酸盐和臭氧的影响较大, T-up和T-low 模拟结果之间可以相差13.4%和10.1%。 相似文献
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应用查表法模拟区域对流层O3、Nox分布和演化的研究 总被引：2，自引：0，他引：2
应用STEM-II气相光化学模式探讨了影响对流层O3、NOx气相光化学转化率的各物理、化学因子。表明在我国多数地区光化学污染物特征(NMHC/NOx较高)下,光辐射强度、温度、初始O3浓度和NOx浓度是影响O3、NOx气相光化学转化率的主要因子。将以上因子分档组合,计算并建立了各种情况下O3、NOx气相光化学转化率的查算表,并将之用于模拟区域O3、NOx的演化和分布。结果表明,与光化学模式直接耦合计算法相比,该方法既能显著缩短计算时间,又能基本反映大气化学反应的非线性过程,并与直接耦合法符合得较好。 相似文献
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文章介绍了一种比较简单实用的地球大气的光谱透过率和到达大气层顶的红外辐射率的计算模型,光谱波长从4 μm到∞ μm,吸收气体H2O、CO2、O3的吸收计算采用Elsasser带模式及其经验参数,H2O的连续吸收公式是美国LOWTRAN-6计算程序的水汽连续吸收经验公式。透过率的计算结果与LOWTRAN计算结果相一致。以这种透过率简化模型为基础,建立了辐射传递正演计算模型,开发了相应软件,并用于卫星遥感射出长波辐射的资料处理中,取得了良好结果。 相似文献
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The rainout-removal of SO2 and the acidification of precipitation from stratiform clouds are simulated using a one-dimensional, time-dependent model, parameterized microphysically in which dissolution and dissociation of gaseous SO2 and H2O2, and oxidation reaction in aqueous phase are taken into account. The effects of dynamic fac-tors, including updraft flow and turbulent transport, and the concentration of gaseous SO2 and H2O2 being transported into the clouds on pH value of the precipitation, the conversion rate S(IV)－S (VI) and the wet deposition rate of SO2 are discussed. 相似文献
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T. J. Luick R. W. Heckert K. Schulz R. S. Disselkamp 《Journal of Atmospheric Chemistry》1999,32(3):315-325
Infrared spectroscopy has been used to measure the vapor pressure of chlorine containing species generated from H2SO4/HNO3/H2O/HCl solutions at 200 K. The vapor pressure was observed to be a function of solution composition. Two solution compositions were investigated. One solution remained a liquid whereas the second solution was a mixed liquid and solid phase (an ice slurry). The liquid solution had a composition of 64.6 wt.% H2SO4/4.8 wt.% HNO3/30.1 wt.% H2O/0.5 wt.% HCl and produced only vapor phase HCl. The ice slurry solution had a composition of 76.6 wt.% H2SO4/3.0 wt.% HNO3/20.1 wt.% H2O/0.3 wt.% HCl and produced HCl, ClNO, and ClNO2 vapor phase components. The sulfuric acid, nitric acid, and water content of these solutions are representative of those present in polar stratospheric clouds (PSCs), however the HCl concentrations are much higher than present within these clouds. The partitioning of chlorine between vapor phase HCl (50%) and ClNO/ClNO2 (50%) for the ice slurry solution suggests a possible mechanism of halogen activation within PSCs. A reaction mechanism to model the observed chemistry is proposed. 相似文献
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The North China Plain （NCP） has recently faced serious air quality problems as a result of enhanced gas pollutant emissions due to the process of urbanization and rapid economic growth. To explore regional air pollu- tion in the NCP, measurements of surface ozone （O3）, nitrogen oxides （NOx）, and sulfur dioxide （SO2） were car- ried out from May to November 2013 at a rural site （Xianghe） between the twin megacities of Beijing and Tianjin. The highest hourly ozone average was close to 240 ppbv in May, followed by around 160 ppbv in June and July. High ozone episodes were more notable than in 2005 and were mainly associated with air parcels from the city cluster in the hinterland of the polluted NCP to the southwest of the site. For NOx, an important ozone precur- sor, the concentrations ranged from several ppbv to nearly 180 ppbv in the summer and over 400 ppbv in the fall. The occurrence of high NOx concentrations under calm condi- tions indicated that local emissions were dominant in Xianghe. The double-peak diurnal pattern found in NOx concentrations and NO/NOx ratios was probably shaped by local emissions, photochemical removal, and dilution re- sulting from diurnal variations of surface wind speed and the boundary layer height. A pronounced SO2 daytime peak was noted and attributed to downward mixing from an SO2-rich layer above, while the SO2-polluted air mass transported from possible emission sources, which differed between the non-heating （September and October） and heating （November） periods, was thought to be responsible for night-time high concentrations. 相似文献
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长江三角洲区域本底大气中致酸气体体积分数变化特征 总被引：1，自引：0，他引：1
利用2003-12—2004-11浙江临安区域大气本底站大气NOx、SO2体积分数的连续观测资料,分析其季节变化和日变化特征。结果表明：长江三角洲区域本底大气中致酸气体NOx、SO2体积分数值均为冬季最高,分别为23.81×10^-9和37.3×10^-9,主要受来自东北方向宁、沪区域城市群的相对高浓度污染物随气团传输影响;夏季最低,主要是局地源的贡献。降水对SO2去除作用明显,对NOx去除效果不大。NOx体积分数值冬季的日变化最为明显,呈现出一低一高的双峰型,09：00出现较高体积分数值,18：00出现最高体积分数值;而夏季为单峰型日变化,07：00出现最高体积分数值。SO2冬、春季的日变化明显,最高体积分数值出现在06：00左右,最低体积分数值出现在15：00左右。该区域NO2全年空气质量达到《环境空气质量标准》（GB 30952—1996）一级标准,SO2冬、春季超标较多,受到人类活动影响较明显。NO2和SO2空气污染指数在12月最大,分别为50和93。该区域NO2和SO2并未出现“周末效应”。 相似文献
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Iodine Chemistry and its Role in Halogen Activation and Ozone Loss in the Marine Boundary Layer: A Model Study 总被引：6，自引：0，他引：6
Rainer Vogt Rolf Sander Roland von Glasow Paul J. Crutzen 《Journal of Atmospheric Chemistry》1999,32(3):375-395
A detailed set of reactions treating the gas and aqueous phase chemistry of the most important iodine species in the marine boundary layer (MBL) has been added to a box model which describes Br and Cl chemistry in the MBL. While Br and Cl originate from seasalt, the I compounds are largely derived photochemically from several biogenic alkyl iodides, in particular CH2I2, CH2ClI, C2H5I, C3H7I, or CH3I which are released from the sea. Their photodissociation produces some inorganic iodine gases which can rapidly react in the gas and aqueous phase with other halogen compounds. Scavenging of the iodine species HI, HOI, INO2, and IONO2 by aerosol particles is not a permanent sink as assumed in previous modeling studies. Aqueous-phase chemical reactions can produce the compounds IBr, ICl, and I2, which will be released back into the gas phase due to their low solubility. Our study, although highly theoretical, suggests that almost all particulate iodine is in the chemical form of IO-3. Other aqueous-phase species are only temporary reservoirs and can be re-activated to yield gas phase iodine. Assuming release rates of the organic iodine compounds which yield atmospheric concentrations similar to some measurements, we calculate significant concentrations of reactive halogen gases. The addition of iodine chemistry to our reaction scheme has the effect of accelerating photochemical Br and Cl release from the seasalt. This causes an enhancement in ozone destruction rates in the MBL over that arising from the well established reactions O(1D) + H2O 2OH, HO2 + O3 OH + 2O2, and OH + O3 HO2 + O2. The given reaction scheme accounts for the formation of particulate iodine which is preferably accumulated in the smaller sulfate aerosol particles. 相似文献
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A case study was performed in Beijing in 2000 to observe concentrations of SO2 and NOx in the atmosphere and to evaluate their radiative impact. It was found that the concentrations of these gases are usually high in the morning due to a temperature inversion in the boundary layer. The average concentrations obtained from the observations are much higher than those used in the McClatchey reference atmosphere. The radiative impacts of these gases are calculated using a line-by-line radiative transfer model. The results show that the radiative forcing at the surface due to SO2 is 0.0576 W m-2 and that due to NOx is 0.0032 W m-2. These figures are almost compatible with that due to CFC11. 相似文献
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The chemistry version of the Weather Research and Forecasting model (WRF/Chem) was coupled with the anthropogenic emission inventory of David Streets to investigate the impacts of secondary aerosols on a persistent fog event from 25 to 26 October 2007, in Northern China. The spatial distribution of the simulated fog is consistent with satellite observations, and the time-height distributions of the simulated boundary layer where the fog formed are also in good agreement with these observations. The sensitivity studies show that the secondary aerosols of SO 4 , NO 3 , and NH 4 formed from gaseous precursors of SO 2 , NO x , and NH 3 had substantial impacts on the formation processes and microphysical structure of the fog event. The decrease of the secondary aerosols obviously reduced the liquid water path and column droplet number concentration of the fog below the 1-km layer, and the corresponding area-averaged liquid water path and droplet number concentration of the fog decreased by 43% and 79%, respectively. The concentrations of NO x and NO 3 were found to be extremely high in this case. The concentration of interstitial aerosol NO 3 was much higher than the SO 4 and NH 4 , but the concentration of SO 4 was highest in the cloud-borne aerosols. The average activation ratios for SO 4 , NO 3 , and NH 4 were 34%, 31%, and 30%, respectively, and the maximum ratios reached 62%, 86%, and 55% during the fog episode. 相似文献
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对辽宁农村代表区域站点——辽中县马龙村观测站2007年2月至2008年1月酸雨、气态污染物浓度观测资料进行了研究。结果表明：辽中站降水的化学组成阴离子主要为SO4^2-和NO3-阳离子主要为NH4和Ca2＋,SO4^2-／NO3-比值为2．9．Na＋／Cl-比值较大,大于1。各种离子浓度冬春季高,夏秋季较低,表明研究区域降水酸化与污染关系不显著。实测的9种主要阴离子、阳离子总浓度比（∑阴离子／∑阳离子）与降水pH值相关性不高,表明目前酸雨研究观测的主要9种阴阳离子不能完全包括降水中的离子组成。降水酸性与近地面污染气体浓度相关各异,pH与NOx、CO、NO2和O3浓度有较明显的负相关,与SO2浓度负相关不明显;降水pH值与颗粒物等碱性污染物浓度正相关明显。降水中主要致酸离子SO4^2-和NO3-的浓度与相应酸性气体污染物SO2和NOx近地面浓度的相关不明显。 相似文献
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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
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