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1.
对临安大气本底站2003-2004年冬、夏季二氧化氮(NO2)、二氧化硫(SO2)、臭氧(O3)进行了分析.结果表明:冬季NO2和SO2平均体积分数分别为19.48×10-9和35.74 x10-9,而夏季的平均体积分数分别为4.81×10-9和8.12×10-9,冬季高于夏季;O3在夏季的平均体积分数为33.55×10-9,略高于冬季的25.44×10-9;夜间NO2和SO2体积分数比白天高,并且NO2呈明显的单峰单谷型分布,O3也呈单峰型但峰值出现在白天.NO2、SO2体积分数存在着明显的“假日效应”,假日比非假日低,周五高于假日和非假日;但O3体积分数没有明显的假日效应.降水对SO2有明显的清除作用,但对NO2的清除作用不明显.与风向对比发现,夏季高体积分数的NO2、SO2都受到NW、WNW风的影响,冬季则分别受NE和SW、SSW风的影响;而O3受风向的影响较复杂,与局地光化学反应有关. 相似文献
2.
NUMERICAL SIMULATION OF THE INFLUENCE OFO3,CO2 AND SPECTRUM VARIATION ON THE PHOTOSYNTHESIS OF CROP CANOPY* 
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下载免费PDF全文 Coupled the photosynthesis with transpiration and adjustment of stoma,a dynamic ecological model for simulating the canopy photosynthesis of winter wheat was established by scaling up from the biochemical scale to canopy scale,in which the effects of O3,CO2 and solar spectrum on crop photosynthesis were fully considered.Validation of the model against the data measured with CI-301PS portable photosynthesis analyzer showed that the leaf photosynthesis model passed the correlation significance test and had a fairly high accuracy.Numerical analysis showed that the canopy photosynthesis rate would be reduced by 29% if the O3 concentration increases from 0 ppbv to 200 ppbv,whereas the canopy photosynthesis rate would increase by about 37% while the CO2 concentration increases from 330 ppmv to 660 ppmv,and the canopy photosynthesis rate would be reduced by 27%0 or so under the condition that the spectrum coefficient changed from 0.5 to 0.4.If the O3 concentration reached 200 ppbv at noon on the typical sunny day with higher radiation,the canopy photosynthesis will be reduced slightly in the suburb area where the pollution is serious and the photochemical fog is easy to be formed,contrast with that in the clear region and regardless of the climate change,due to the fact that the positive effect of CO2 on crop photosynthesis can not compensate the negative effect of O3 on crop photosynthesis.The canopy photosynthesis will be reduced by 35% or so than the BASE value at present,when the spectrum of photosynthetic active radiation(PAR) reduces to 0.4 or so. 相似文献
3.
F. H. Adema J. R. Ybema P. Heeres H. C. P. Wegh 《Journal of Atmospheric Chemistry》1990,11(3):255-269
In a nighttime system and under relatively dry conditions (about 15 ppm H2O), the reaction mixture of NO2, O3, and NH3 in purified air turns out to result in the formation of nitrous oxide (N2O). The experiments were performed in a continuous stirred flow reactor, in the concentration region of 0.02–2 ppm.N2O is thought to arise through the heterogeneous reaction of gaseous N2O5 and absorbed NH3 at the wall of the reaction vessel % MathType!MTEF!2!1!+-% feaafeart1ev1aaatCvAUfeBSjuyZL2yd9gzLbvyNv2CaerbuLwBLn% hiov2DGi1BTfMBaeXatLxBI9gBaerbd9wDYLwzYbItLDharqqtubsr% 4rNCHbGeaGqiVu0Je9sqqrpepC0xbbL8F4rqaqpepeea0xe9qqVa0l% b9peea0lb9sq-JfrVkFHe9peea0dXdarVe0Fb9pgea0xa9pue9Fve9% Ffc8meGabaqaciGacaGaaeqabaWaaeaaeaaakeaatCvAUfKttLeary% qr1ngBPrgaiuaacqWFOaakcqWFobGtcqWFibasdaWgaaWcbaGae83m% amdabeaakiab-LcaPmaaBaaaleaacqWFHbqyaeqaaOGaey4kaSIaai% ikaiab-5eaonaaBaaaleaacqWFYaGmaeqaaOGae83ta80aaSbaaSqa% aiab-vda1aqabaGccaGGPaWaaSbaaSqaaiaadEgaaeqaaOGaeyOKH4% Qae8Nta40aaSbaaSqaaiab-jdaYaqabaGccqWFpbWtcqGHRaWkcqWF% ibascqWFobGtcqWFpbWtdaWgaaWcbaGae83mamdabeaakiabgUcaRi% ab-HeainaaBaaaleaacqWFYaGmaeqaaOGae83ta8eaaa!59AC!\[(NH_3 )_a + (N_2 O_5 )_g \to N_2 O + HNO_3 + H_2 O\]In principle, there is competition between this reaction and that of adsorbed H2O with N2O5, resulting in the formation of HNO3. At high water concentrations (RH>75%), no formation of N2O was found. Although the rate constant of adsorbed NH3 with gaseous N2O5 is much larger than that of the reaction of adsorbed H2O with gaseous N2O5, the significance of the observed N2O formation for the outside atmosphere is thought to be dependent on the adsorption properties of H2O and NH3 on a surface. A number of NH3 and H2O adsorption measurements on several materials are discussed. 相似文献
4.
The growth of monodisperse particles (0.07 to 0.5 µm) exposed to SO2 (0–860 ppb), H2O2 (0–150 ppb) and sometimes NH3 (0–550 ppb) in purified air at 22 °C at relative humidities ranging from 25 to 75% were measured using the Tandem Differential Mobility Analyzer technique. The experiments were performed in a flow reactor with aqueous (NH4)2SO4 and Na2SO4 droplets. For (NH4)2SO4 droplets the fractional diameter growth was independent of size above 0.3 µm but decreased with decreasing size below that. When NH3 was added the fractional growth increased with decreasing size. Measurements were compared with predictions of a model that accounts for solubility of the reactive gases, the liquid phase oxidation of SO2 by H2O2, and ionic equilibria. Agreement between measured and predicted droplet growth is reasonable when the ionic strength effects are included. Theory and experiments suggest that NH3 evaporation is responsible for the decrease in relative growth rates for small aqueous ammonium sulfate particles. The observed droplet growth rates are too slow to explain observed growth rates of secondary atmospheric sulfate particles. 相似文献
5.
基于典型城市站太原站2018年3月—2019年2月的大气CO2在线观测资料,利用筛分法(Meteorological filtering method, MET)和黑碳示踪法(Black Carbon tracer, BC)进行本底/非本底的筛分,得到了本底浓度的变化特征。结果表明,太原大气CO2浓度季均值冬季最高,夏季最低;不同季节呈“单峰型”日变化特征,日振幅均在26.0×10-6以上;4个季节CO2浓度与地面风速存在显著负相关关系;CO2浓度抬升区域主要受当地工业布局的影响,最大抬升幅度在秋季达17.4×10-6;使用气象筛分法(MET)得到年均本底浓度为(431.4±19.9)×10-6,人为排放等对其影响为23.5×10-6,年振幅比同纬度其它本底站大,为34.5×10-6;黑碳示踪法(BC)得到冬季季均本底浓度为(445.0±22.9)×10-6,比MET筛... 相似文献
6.
A method for the estimation of the reaction probability of the heterogeneous N2O5+H2O 2HNO3 reaction using the deposition profile in a laminar flow tube, in which the walls are coated with the condensed aqueous phase of interest, is presented. The production of gas phase nitric acid on the surface followed by its absorption complicates the deposition profiles and hence the calculation of the reaction probability. An estimation of the branching ratio for this process enables a more appropriate calculation to be carried out. Reaction probabilities of N2O5 on substances including some normally constituting atmospheric aerosols, NaCl, NH4HSO4, as well as Na2CO3 are estimated and found to depend on relative humidity and characteristics of the coating used. These fell within the range (0.04–2.0)×10–2. 相似文献
7.
厌氧条件下土壤反硝化气体(N2、N2O、NO)和CO2排放——氦环境培养—气体同步直接测定法的应用初探 总被引：3，自引：1，他引：2
反硝化过程是维系闭合氮循环所必需的氮素形态转化环节。土壤反硝化过程速率及产物比的直接测定是研究氮循环过程机理的基础,但却是一个难题。为解决此难题,德国卡尔斯鲁厄技术研究所与中国科学院大气物理研究所最近合作新建了一套通过氦环境培养-气体同步直接测定土壤反硝化气体--氮气（N2）、氧化亚氮（N2O）、一氧化氮（NO）和二氧化碳（CO2）排放的系统和与之配套的三阶段培养方法。为检验该新建系统和配套方法测定土壤反硝化过程的准确性和可靠性,以华北地区广泛分布的盐碱地农田土壤（采自山西运城）为研究对象开展实验室培养试验,在初始可溶性有机碳（DOC）供应比较充足约300 mgC kg–1干土（d.s.）的条件下,测试了不同初始土壤硝态氮含量水平（10、100 mgN kg–1d.s.左右,分别表示为10N和100N）的反硝化气体和CO2排放过程。结果显示：100N的反硝化速率（定义为N2、N2O 和NO 排放速率之和）显著高于10N 处理（统计检验显著水平p＜0.01）;两个处理的反硝化产物均以N2为主（质量比分别占77%和75%）,产物的NO/N2O摩尔比分别为1.2和1.5,N2O/N2摩尔比均为0.19;土壤反硝化气体动态排放速率及相关指标的测定结果表明,培养土壤中消失的硝态氮被回收81%～87%,培养前后的氮平衡率达92%～95%。因此,该新建方法测定土壤反硝化速率和产物比的结果具有很好的可靠性,为定量研究土壤反硝化过程提供了有效的直接测定手段。研究中检测到的土壤反硝化产物NO/N2O摩尔比大于1,不同于以往用液体培养基纯培养反硝化细菌得出的NO/N2O摩尔比远小于1的结论。这意味着,不能用NO/N2O摩尔比小于1与否来推断土壤排放的N2O和NO是主要来源于反硝化作用还是硝化作用。 相似文献
8.
Laboratory experiments were carried out to investigate the linear depolarization ratios (LDRs) of crystallized H2O/H2SO4 acid clouds at angles of 45°, 135° and 157° to the forward direction. LDR is the ratio of the returned energies in the planes of polarization perpendicular and parallel to that of the source (Sassen, 1974). Experiments were carried out for different concentrations of aqueous solution of sulfuric acid. A cloud of supercooled droplets is formed inside an experimental chamber kept in a walk-in cold room by heating an aqueous solution of sulfuric acid, and the ice crystal formation is initiated by momentarily introducing a rod dipped in liquid nitrogen into the cloud. A 2-mW polarized He:Ne laser beam is directed through the cloud and a photomultiplier tube measures the scattered intensity. It is found that the scattered energy is higher in the direction of 157° and 135° than that at 45°. Microscopic examination of the crystals formed from acid concentrations above 50% shows dark fuzzy spots on the surface of the ice crystals suggesting that this could be a film of acid drops. This film also alters the shape of the crystals, and the crystal boundaries are no longer sharp and well defined like that observed for pure water clouds and this is found to influence the LDR. 相似文献
9.
The photochemical oxidation of SO2 in the presence of NO and C3H6 was studied in a 18.2 liter pyrex reactor. When light intensity, irradiation time and SO2 concentration were constant, SO4
2- concentration, derived from the total volume of aerosol produced, peaked when [C3H6]/[NO] was approximately 6.0. Another increase im SO4
2- formation was reached at very high ratios (>50). The experimental observations are consistent with the two SO2 oxidation mechanisms. At low [C3H6]/[NO] ratios, the processes proceed via the HO–SO2 reaction, while at high ratios the O3–C3H6 adduct is assumed to oxidize SO2 to produce SO4
2- aerosols. 相似文献
10.
2018年1月,利用颗粒物采样器采集武汉市大气PM2.5样品并进行水溶性无机离子（F-、Cl-、NO3-、SO42-、Na+、NH4+、K+、Mg2+、Ca2+）的分析.结果表明,NO3-、SO42-、NH4+是PM2.5中最主要的3种水溶性无机离子,除Mg2+与Ca2+外,PM2.5与WSⅡs （水溶性无机离子）之间的相关性显著,且移动源贡献占主导地位.阴阳离子平衡表明武汉市冬季灰霾期PM2.5呈中性或弱酸性.通过混合单粒子拉格朗日综合轨迹模式模拟并采用分层聚类得出了4种主要的后向气流轨迹及相应的PM2.5和水溶性离子浓度,结果表明区域传输对此次灰霾期影响较大. 相似文献
11.
CH4和N2O作为主要温室气体,自工业革命以来排放量急剧增加,已经被列入《京都议定书》要求控制它们的排放。本文利用高光谱分辨率的辐射传输模式,计算了CH4、N2O在晴空大气和有云大气条件下的瞬时辐射效率和平流层调整的辐射效率,以及它们的全球增温潜能(GWP)和全球温变潜能(GTP),并根据模式结果拟合了CH4和N2O的辐射强迫的简单计算公式。本文的研究表明:CH4和N2O在有云大气下的平流层调整的辐射效率分别为4.142×10-4 W m-2 ppb-1和3.125×10-3 W m-2 ppb-1 (1ppb=10-9),经大气寿命调整后的辐射效率分别为3.732×10-4 W m-2 ppb-1和2.987×10-3 W m-2 ppb-1,与IPCC(2007)的相应结果高度一致。CH4和N2O 100年的全球增温潜能GWP分别为16和266;100年的脉冲排放的全球温变潜能GTPP分别为0.24和233;持续排放的全球温变潜能GTPS分别为18和268。它们在未来全球变暖和气候变化中,影响仅次于CO2,仍然起着非常关键的作用。 相似文献
12.
RESEARCH ON SURFACE O3 WITH METEOROLOGICAL CONDITIONS UNDER ATMOSPHERIC BACKGROUND CONDITIONS IN NORTHEAST CHINA* 下载免费PDF全文
下载免费PDF全文 Ding Guo''an Xu Xiaobin Xiang Rongbiao Li Xingsheng Zhang Zhonghua 《Acta Meteorologica Sinica》1997,11(4):478-488
Surface O3 concentration and its precursors have been observed at Longfengshan station,Heilongjiang Province for a period of one year from August 13,1994 to July 30,1995. Relationship between surface O3 and the meteorological conditions during this period is analyzed in this study.Observation results show that diurnal variation of surface O3 follows a pattern of double-peaks with amplitude of 27-28 ppb under fine days in summer and autumn.Although the diurnal variation is small(14 ppb),it is still detectable when it is overcast.Diurnal variation of O3 is irregular under rainy days.Surface O3 concentration rises when wind speed starts to increase at 0800 BT(Beijing Time)from 0 to 6 m s-1in autumn,winter and summer.Relative high surface O3 concentration is noticed frequently when S,SSW,SW and WSW wind are encountered at the station during all seasons.At 0800 BT and 1400 BT the surface O3 concentration increases with the increase of global radiation accordingly during fine days in winter,spring and autumn.During fine days average peak of O3 concentration in summer is 20 ppb higher than that in winter while the average peak of global radiation in summer is almost twice as high as that in winter.The average surface O3 concentration under fine days in autumn at Longfengshan station is 14 ppb lower in comparison to the observation results from Lin'an station where Lin'an is at about the same longitude and lower latitude,with same environment,which is mainly caused by the difference of global radiation due to different latitudes in these two areas(difference of average peak global radiation about 100 W m-2). 相似文献
13.
由于电离层中分子性离子与电子的复合要比氧离子与电子的复合快得多,因此H2在电离层高度释放可有效地引起电子的消耗。本文基于一个包括中性气体扩散方程和离子化学反应方程的二维动力学模型,对H2在电离层高度释放过程进行了数值模拟研究,并分析了不同释放条件下的电子扰动特性。结果表明:1)500 mol H2释放后,迅速向周围空间扩散,释放中心处的电子密度30 s内下降了近4%,F2层临界频率下降了1%左右;2)在不同高度处释放H2时,最大的电子密度相对变化率并不是在峰值高度附近处释放时出现的;3)释放化学物质的量越多,电子密度的扰动幅度也越大,但两者之间并不存在线性关系;4)相同量的H2在电离层峰值高度处释放,白天的电子密度扰动幅度要大于夜间的扰动幅度。 相似文献
14.
We present here experimental determinations of mass accommodation coefficients using a low pressure tube reactor in which monodispersed droplets, generated by a vibrating orifice, are brought into contact with known amounts of trace gases. The uptake of the gases and the accommodation coefficient are determined by chemical analysis of the aqueous phase.We report in this article measurements of exp=(6.0±0.8)×10–2 at 298 K and with a total pressure of 38 Torr for SO2, (5.0±1.0)×10–2 at 297 K and total pressure of 52 Torr for HNO3, (1.5±0.6)×10–3 at 298 K and total pressure of 50 Torr for NO2, (2.4±1.0)×10–2 at 290 K and total pressure of 70 Torr for NH3.These values are corrected for mass transport limitations in the gas phase leading to =(1.3±0.1)×10–1 (298 K) for SO2, (1.1±0.1)×10–1 (298 K) for HNO3, (9.7±0.9)×10–2 (290 K) for NH3, (1.5±0.8)×10–3 (298 K) for NO2 but this last value should not be considered as the true value of for NO2 because of possible chemical interferences.Results are discussed in terms of experimental conditions which determine the presence of limitations on the mass transport rates of gaseous species into an aqueous phase, which permits the correction of the experimental values. 相似文献
15.
The paper focuses on the redistribution of aerosol particles (APs) during the artificial nucleation and subsequent growth of ice crystals in a supercooled cloud. A significant number of the supercooled cloud droplets during icing periods (seeding agents: C3H8, CO2) did not freeze as was presumed prior to the experiment but instead evaporated. The net mass flux of water vapour from the evaporating droplets to the nucleating ice crystals (Bergeron–Findeisen mechanism) led to the release of residual particles that simultaneously appeared in the interstitial phase. The strong decrease of the droplet residuals confirms the nucleation of ice particles on seeding germs without natural aerosol particles serving as ice nuclei. As the number of residual particles during the seedings did not drop to zero, other processes such as heterogeneous ice nucleation, spontaneous freezing, entrainment of supercooled droplets and diffusion to the created particle-free ice germs must have contributed to the experimental findings. During the icing periods, residual mass concentrations in the condensed phase dropped by a factor of 1.1–6.7, as compared to the unperturbed supercooled cloud. As the Bergeron–Findeisen process also occurs without artificial seeding in the atmosphere, this study demonstrated that the hydrometeors in mixed-phase clouds might be much cleaner than anticipated for the simple freezing process of supercooled droplets in tropospheric mid latitude clouds. 相似文献
16.
An experimental study has been carried out in the Mainz vertical wind tunnel to determine the rate at which NH3 in the presence of CO2 is absorbed by freely suspended water drops. The experimental uptake rates were found to be in good agreement with the rates predicted by the Kronig-Brink convective diffusion model and, for gas concentrations in the ppbv range also by the model in which it is assumed that the absorbed gas is well mixed inside the drop (henceforth called well mixed model). The same conclusion was shown to apply also to the desorption of NH3 from a drop previously exposed to NH3. The latter result is in contrast to the desorption of SO2 which must be described by a model which accounts for the diffusion of the species inside the drop. Comparison of our experimental results with theory show further that the uptake of NH3 in presence of CO2 is significantly overestimated if the slow reaction CO2(aq)+H2OHCO
3
–
+H+ is neglected in the theoretical computation. 相似文献
17.
为了解闪电对对流层上部微量气体的贡献,利用全球水资源和气候中心(GHRC)提供的1995年4月—2006年6月的闪电卫星格点资料,以及高层大气研究卫星(UARS)上的卤素掩星试验(HALOE)1991年10月—2005年11月的观测资料,分析了全球闪电与对流层上部NO和O3体积分数的时空分布特征及其相关性。结果表明:全球闪电12、1、2月集中在南半球,6—8月集中在北半球,全球闪电的季节分布与NO、O3类似;NO体积分数在350 h Pa附近达到最大,该高度的南半球NO体积分数变化范围为7×10-12~11×10-12、北半球为3×10-12~17×10-12;450~300 h Pa,北半球夏季O3体积分数呈明显增加趋势,且同一高度上夏季的值比年平均值大25%左右,南半球夏季O3体积分数高于冬季,但差异并不大。结论进一步证明了闪电与对流层上部NO及O3的密切关系,也为研究全球气候变化提供有力证据。 相似文献
18.
We use a global atmospheric chemistry transport model to study the possible influence of aqueous phase reactions of peroxynitric acid (HNO4) on the concentrations and budgets of NOx, SOx, O3 and H2O2. Laboratory studies have shown that the aqueous reaction of HNO4aq withHSO–
3aq, and the uni-molecular decomposition of the NO4
– anion to form NO2
– (nitrite) occur on a time scale of about a second. Despite a substantial contribution of the reaction of HSO–
3aq with HNO4aq to the overall in-cloud conversion of SO2 to SO4
2–, a simultaneous decrease of other oxidants (most notably H2O2) more than compensated the increase in SO4
2– production. The strongest influence of heterogeneous HNO4 chemistry was found in the boundary layer, where calculated monthly average ozone concentrations were reduced between 2% to 10% andchanges of H2O2 between –20% to +10%compared to a simulation which ignores this reaction. Furthermore, SO2 was increased by 10% to 20% and SO4
2–depleted by up to 10%. Since the resolution of our global model does not enable a detailed comparison with measurements in polluted regions, it is not possible to verify whether considering heterogeneous HNO4 reactions results in a substantial improvement of atmospheric chemistry transport models. However, the conversion of HNO4 in the aqueous phase seems to be efficient enough to warrant further laboratory investigations and more detailed model studies on this topic. 相似文献
19.
The gas phase concentration of hydrogen peroxide at Summit, Central Greenland, has been measured continuously during June/July 1990 using a coil scrubber technique combined with liquid phase fluorometry. The concentrations ranged between 0.3 ppbv and 3.5 ppbv, which is considerably higher than expected from model calculations and can be explained by low deposition rates. The record shows pronounced diurnal variations with minimum concentrations during night and maximum concentrations in the afternoon. The nocturnal minima can be explained by scavenging of H2O2 by hoarfrost. The scavenging mechanisms of H2O2 by snow and the redistribution of H2O2 during firnification are discussed. There is indirect evidence, that H2O2 is uniformly distributed in the ice lattice and that the fractionation between H2O2 and H2O is small during diffusional crystal growth from the vapor phase (co-condensation). 相似文献
20.
利用瓦里关和上甸子大气本底站观测的月平均CO2浓度数据对GOSAT卫星反演的CO2浓度数据进行验证,结果表明GOSAT产品与台站观测数据有较好的一致性.利用2009年6月—2011年5月GOSAT反演的CO2浓度数据,分析了江苏地区CO2浓度的时空变化特征,结果表明:1)975 hPa高度层CO2浓度高于850 hPa高度层,CO2浓度的水平变化要小于垂直变化;2)在季节变化上,CO2浓度冬季最高,夏季最低,这可能与植被光合作用的强弱变化有关;比较前后两年的CO2浓度数据,夏季和秋季的增速较快,冬季和春季的增速较慢;3)在日变化上,发现徐州和南京站02时CO2浓度最高,14时CO2浓度最低,这可能也与植被光合作用的强弱有关. 相似文献