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1.IntroductionMethane(CH#)isanimportantgreenhousegasinatmosphere.ThemainremovalprocessofCH4inatmosphereisreactedwithOHwhichisdeterminedbytheabundanceofmethane,carbonmonoxide(CO)andnitrousoxides(NO.)whoseemissionshaveincreasedgreatlybecauseofhumanacti... 相似文献
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应用作者建立的全球二维大气化学模式,采用2种CH4排放源的长期增长方案,同时考虑了CH4排放源以及对OH自由基浓度有重要影响的CO和NOx排放源的长期变化,模拟了CH4和OH从1840~2020年的长期变化趋势。考虑了世界人口增长的排放源方案可以更好地模拟CH4的长期变化,模拟结果表明,工业革命前的大气CH4浓度和年排放总量分别为760×10-9(V/V)和280×109kg,1991年大气CH4的浓度和年排放总量分别为1611.9×10-9(V/V)和533.9×109kg,对流层OH自由基数浓度从1840年的7.17×105分子数/cm3下降到1991年的5.79×105分子数/cm3,降低了19%。工业革命以来大气CH4的增长一方面是由于CH4排放源的增长,另一方面是由于大气OH浓度的下降。 相似文献
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A global two-dimensional chemistry model is developed to study long-term trends of CH_4 sinceindustrial revolution.The sources of CH_4,CO and NO_x are parameterized as functions of latitudeand time.With two long-term emission scenarios,long-term trends of CH_4 are simulated.The resultshave a good agreement with observation from ice cores.The modeled CH_4 increased from 760 ppbvin 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OHdecreased from 7.17×10~5 cm~(-3)in 1840 to 5.79×10~5 cm~(-3) in 1991.The increase of atmosphericCH_4 can be explained by the increase of emission of CH_4 and build-up because of decrease of OHradicals that remove CH_4 from the atmosphere.The model is also used to simulate the distribution of CH_4.Comparisons between the modelresults and observations show that the model can simulate both latitudinal distribution and seasonalvariation of CH_4 well. 相似文献
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A global two-dimensional chemistry model is developed to study long-term trends of CH4 since industrial revolution.The sources of CH4,CO and NOx are parameterized as functions of latitude and time.With two long-term emission scenarios,long-term trends of CH4 are simulated.The results have a good agreement with observation from ice cores.The modeled CH4 increased from 760 ppbv in 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OH decreased from 7.17×105 cm-3 in 1840 to 5.79×105 cm-3 in 1991.The increase of atmospheric CH4 can be explained by the increase of emission of CH4 and build-up because of decrease of OH radicals that remove CH4 from the atmosphere.The model is also used to simulate the distribution of CH4.Comparisons between the model results and observations show that the model can simulate both latitudinal distribution and seasonal variation of CH4 well. 相似文献
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应用全球二维大气化学模式,模拟了CO、CH4和OH自由基等成分自工业革命到2020年的长期变化.模拟的全球CO平均体积分数在1840年、1991年和2020年分别为27×10-6、76×10-6和105×10-6.从1840到1991年,OH自由基数浓度从7.17×105个分子/cm3下降到5.79×105个分子/cm3,降低了19%.模拟的CH4长期变化与冰芯资料相符.模拟的20世纪80年代CO体积分数年增长率为1.03%~1.06%.大气中CO在20世纪90年代前是增长的,而到90年代初观测到CO体积分数突然下降.应用二维大气化学模式对此原因进行了模拟研究,结果表明,CO排放源的减少是CO体积分数下降的主要因子,平流层臭氧减少是另一个重要因子.尽管CO排放源的减少对大气CH4增长率的变化有较大影响,而CH4排放源减少对CO体积分数变化却几乎没有影响. 相似文献
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建立了一个全球二维纬向平均化学模式,模式包括了从90°S到90°N,从地面到20 km高度的大气.模式中应用的流场来自根据加热率计算得到的剩余环流.模式化学部分包括34种大气成分、104个化学反应和光化学反应.其中,甲烷、一氧化碳和氮氧化物排放分为季节性和非季节性排放源,并将其参数化为时间和纬度的函数再应用到模式中去.按1990年的甲烷、一氧化碳和氮氧化物的的排放水平模拟得到了多种大气组成的分布,模拟结果与观测有较好的一致性.由于模式考虑了一氧化碳的季节变化,模拟得到的OH自由基分布更为合理.模式的建立为今后进一步研究大气微量成分的全球循环过程及其长期变化提供了有效的手段. 相似文献
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A new instrument has beendeveloped to measure the total decay rate of OH in ambient air. Theinstrument is based on the discharge flow technique in which OHgenerated within the instrument is reacted with ambient air pulled intothe flow tube. The OH decay is monitored by laser-induced fluorescence. Thistotal decay rate is compared to the sum of the individual decay rates ofOH with each trace species measured in the air to test for missing OHreactants. OH decay rates measured in an urban environment in thesummer of 1999 illustrates the promise of this technique. 相似文献
8.
1992年大气甲烷增长速率异常
下降的模拟研究 总被引:4,自引:0,他引:4
应用初步建立的全球二维大气化学模式,模拟了甲烷、一氧化碳和OH自由基自工业革命以来的长期变化,对1992年大气中甲烷增长速率突然下降这一异常现象的可能原因如平流层O3下降,皮纳图博火山引起对流层温度下降、甲烷排放源减少等逐一进行了定量研究。研究还发现一氧化碳排放源的减少是另一重要影响因子,并进行了验证。结果表明,1992年甲烷增长速率急剧下降的主要原因来自甲烷和一氧化碳排放源的减少。 相似文献
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应用初步建立的全球二维大气化学模式,对工业革命以来甲烷的长期变化进行了模拟研究。模式将CH4、CO和NOx排放源方案进行了参数化。在考虑了CH4排放源以及对OH浓度有重要影响的CO和NOx排放源的长期变化的基础上,模拟了CH4和OH浓度自1840年到20世纪90年代的长期变化趋势。结果表明,工业革命前的大气甲烷体积分数和年排放总量分别为760×10-9和280Tg,1991年大气甲烷的体积分数和年排放总量分别为1611.9×10-9和533.9Tg。而对流层中OH的数密度则由1840年的7.17×105cm-3变化到1991年的5.79×105cm-3,下降了19%。如果CH4、CO及NOx这三种排放源继续按给定的方案增长,那么到2020年大气甲烷的体积分数和年排放总量将增加为2090.7×10-9和966.2Tg,而OH的数密度将为5.47×105cm-3,比1840年降低24%。 相似文献
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K.-Y. Wang J. A. Pyle D. E. Shallcross S. M. Hall 《Journal of Atmospheric Chemistry》2001,40(2):123-170
In part 3 of this series of papers on a new 3-D global troposphericchemical transport model, using an Integrated Modelling System (IMS), anevaluation of the model performance in simulating global distributions andseasonal variations for volatile organic compounds (VOCs) in the atmosphere,is presented. Comparisons of model OH concentrations with previous modelstudies show consistent modelled OH levels from the subtropics tomidlatitudes, while more discrepancies occur over the tropical lowlatitudes, with IMS predicting the highest levels of OH. The close agreementbetween modelled OH concentrations over midlatitudes, where high surfaceNOxand VOC concentrations are also found, is indicative of the strongphotochemical coupling between NOx, VOCs and O3 overthese latitudes. IMSOH concentrations in the Northern Hemisphere (NH) midlatitudes during summerare generally lower than available measurements, implying that models ingeneral are underestimating OH levels at this location and time of year.Substantial differences between model OH concentrations over low latitudesclearly highlight areas of uncertainty between models. IMS OH concentrationsare the highest in general of the models compared, one possible reason isthat biogenic emissions of species such as isoprene and monoterpenes arehighest in IMS, leading to higher O3 levels and hence higher OH.Generally, the IMS VOC concentrations show a similar seasonality to themeasurements at most locations. In general though, IMS tends to underestimatethe NH wintertime VOC maximum and overestimate the NH summertime VOCminimum. Such an overestimate in summer could be due to IMSunderestimating OH levels, or an overestimation of VOC emissions or possiblya problem with model transport, all of these possibilities are explored.Except for n-pentane, the model underprediction of a VOC maximum during theNH winter month strongly suggests a missing emission mechanism in the modelor an underestimate of an existing one. It is very likely that there is alack of time varying emission sources in the model to account for theseasonal change in emission behaviour such as increasing energy usage (e.g.,electricity and gas), road transportation, engine performance, and otheranthropogenic factors which show strong seasonal characteristics. Theanomalous overprediction of wintertime n-pentane compared with its closesummertime prediction with the measurements suggest that emissions in thiscase may be too high. 相似文献
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使用二维云分辨模式研究冰晶增长过程(云水到冰晶的冻结增长和通过水汽凝华冰晶到雪的增长)对热量收支的影响。采用4种冰晶增长参数化方案模拟了热带到中纬度地区的4个降水个例。研究发现:(1)高冰核浓度的ZENG方案和SHEN方案引起对流层中上层辐射加热增多,这与它们模拟的冰晶在对流层中上层增多有关。(2)高冰核浓度的ZENG方案导致模拟区域—平均的局地温度变化在对流层上层出现异常减小值,这与它在热带个例中导致垂直热量通量辐合减少和在中纬度个例中导致潜热加热减少有关。(3)尽管高冰核浓度的ZENG方案引起质量加权平均的辐射加热增多,但是它在热带个例中引起地表感热通量减少和在中纬度个例中引起潜热加热减少,最终导致4种参数化方案计算的模拟区域—质量加权平均的局地温度变化基本一致。 相似文献
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P. J. Fraser R. A. Rasmussen J. W. Creffield J. R. French M. A. K. Khalil 《Journal of Atmospheric Chemistry》1986,4(3):295-310
New CH4 emission data from a number of Northern and Southern Hemispheric, tropical and temperate termites, are reported, which indicate that the annual global CH4 source due to termites is probably less than 15 Tg. The major uncertainties in this estimate are identified and found to be substantial. Nevertheless, our results suggest that termites probably account for less than 5% of global CH4 emissions. 相似文献
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气相化学过程是硫沉降过程中的重要过程。气相化学反应既是SO2气体的氧化去除过程,也为液相化学过程提供初值条件。首先建立了一个适合于研究硫沉降过程的气相化学数值模式,模式包括了52个方程、31个物种。然后利用这个气相化学模式探讨了SO2的气相氧化过程对大气温度、湿度、太阳光强等条件的敏感性并给出了SO2气相氧化率的日变化。 相似文献
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初步建立了以二氧化硫、硫酸盐、黑碳、沙尘气溶胶等作为主要研究对象的全球环境大气输送模式(Global Environmental Atmospheric Transport Model,GEATM),其水平分辨率为1°×1°,垂直方向分为20层,采用地形追随坐标系,考虑了上述大气化学成分的地面源排放、平流与扩散、化学转化以及干沉降、湿清除等过程.利用NCEP/NCAR再分析资料作为驱动气象场,对2004年进行长期模拟,分析了二氧化硫、硫酸盐、黑碳、沙尘气溶胶的浓度分布和输送态势.与观测的比较表明,模式对于大气化学成分分布状况具有较强的模拟能力,在欧洲的Jarczew和Leba观测站,二氧化硫日平均浓度的相关系数分别达到了0.69和0.66;在中国,有47个站点的二氧化硫日平均浓度相关系数高于0.50,其中北京、天津、上海等28个站点的浓度相关系数达到了0.60以上.同时,模拟的沙尘气溶胶总体柱浓度分布状况与卫星观测输出的气溶胶光学厚度具有很好的一致性,体现了气溶胶粒子的输送态势和分布特征.模拟结果显示二氧化硫、硫酸盐、黑碳的浓度高值区主要位于污染排放较大的欧洲、东亚和北美地区,二氧化硫地面最大年均浓度值为1500×10-12,硫酸盐为500×10-12,黑碳气溶胶为1000ng/m3.沙尘浓度与下垫面土壤类型以及地面气象条件关系密切,全球沙尘浓度主要分布在撒哈拉沙漠、阿拉伯半岛、中亚地区、澳大利亚西部以及拉丁美洲南部地区,并且呈现了较为显著的季节变化特征,撒哈拉沙漠输送最强时期是在6~8月,影响范围覆盖了整个赤道大西洋,最西端伸展到了北美的加勒比海地区;阿拉伯半岛沙尘输送最强时期是3~8月,影响范围包括阿拉伯海和孟加拉湾地区;亚洲在3~5月有非常强烈的沙尘东传过程,浓度输送带一直贯穿了整个北太平洋地区. 相似文献
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本实验旨在研究稻田土壤中甲烷产生率对稻田CH_4排放的影响.观测结果表明:土壤各深度的甲烷产生率有很大的变化范围(1—4639ng·h~(-1)·g~(-1)d.w.).主要的甲烷产生区域是7—17cm深的土壤层,其中以13cm深的土壤层上的生成速率最大.土壤中甲烷产生率与稻田CH_4排放率在水稻生长的某些阶段有较好的相关性,但它的季节变化却不能与排放的季节变化完全耦合.在水稻生长期,土壤中甲烷产生率随时间而增大,并在8月份水稻收割前达到最大,其日平均值在38—767 ng·h~(-1)·g~(-1)d.w.间变动.稻田土壤中甲烷产生率也存在日变化,一般在下午达到最大值,但却没有发现它与土壤温度有明显的相关关系.在不同施肥及水稻品种的稻田土壤中也观测到不同的甲烷产生率.在土壤中产生的甲烷最多只有28.8%被排放到大气中,而其余多于71.2%的则被氧化在土壤中. 相似文献
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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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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 ki-netic 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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19.
Yves J. Balkanski Daniel J. Jacob Richard Arimoto Mark A. Kritz 《Journal of Atmospheric Chemistry》1992,14(1-4):353-374
The atmospheric distribution of222Rn over the north Pacific is simulated with a three-dimensional chemical tracer model using meteorological input from the NASA-GISS general circulation model (4°×5° resolution). Radon-222 (half-life 3.8 days) is a tracer of continental air. Model results are in good agreement with measurements from ships and aircraft. Strong Asian influence is found throughout the tropospheric column over the north Pacific in spring, reflecting a combination of frequent convection over the continent, strong westerly winds at altitude, and subsidence over the ocean. In summer, the upper troposphere over the north Pacific is heavily affected by deep convection over China; however, Asian influences at the surface are then at their yearly minimum. In winter, strong Asian influence is found near the surface but not at high altitudes. Transport of American air over the Pacific is important only at low latitudes. American sources account for 11% of total222Rn in the model at Midway, 30% at Mauna Loa and 59% at Oahu. Results for Hawaii indicate two seasonal peaks of American influence, one in summer and one in winter. The tropical western Pacific is particularly remote from continental influences year round. 相似文献
20.
山谷风环流控制下的大气污染物输送和扩散过程:二维数值模拟研究 总被引:3,自引:0,他引:3
本文以兰州地区的实际地形为背景,建立了一个二维小尺度数值模式,并用它对山谷之间热力差异造成的山谷风环流及其控制下山谷中高架源排放的污染物输送和扩散过程进行了模拟研究。结果表明,在山谷风环流控制下,造成山谷内高污染浓度的主要因素有两个:一是日出前和日落后山谷风的转换;二是在白天由于山谷风环流所造成的山谷上空较强的下沉气流。 相似文献