Modeling the sudden decrease in CH4 growth rate in 1992

A two-dimensional global chemistry model is developed to study the distribution and long-term trends of methane. The model contains 34 species and 104 chemical and photochemical reactions. Using the model, the long-term trends of CH₄, CO and OH in atmosphere are simulated, comparison between the model and observations shows that the simulation is successful. Experiments are done to investigate the causes of dramatic decrease in the growth rate of CH₄ in 1992 such as OH increase due to stratospheric ozone depletion, decrease of temperature in the troposphere due to Mount Pinatubo eruption and descendent of CH₄ sources fluxes. A new explanation is proposed and verified by this model that the decrease of CO emission plays an important role for the abnormal growth rate of CH₄ in 1992. We find that the decreases of CH₄ and CO emissions are the main reasons for the sudden decrease of growth rate of CH₄ in 1992, which account for 73% and 27% respectively.     

1992年大气甲烷增长速率异常 下降的模拟研究

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。     

150年来大气甲烷浓度的长期变化

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。     

Total OH Loss Rate Measurement

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.     

NUMERICAL SIMULATION OF ATMOSPHERIC METHANE TRENDS OVER THE LAST 150 YEARS

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.     

NUMERICAL SIMULATION OF ATMOSPHERIC METHANE TRENDS OVER THE LAST 150 YEARS*

A global two-dimensional chemistry model is developed to study long-term trends of CH₄ since industrial revolution.The sources of CH₄,CO and NO_x 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.     

大气中一氧化碳浓度变化的模拟研究

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.     

Note on the Growth Rate of Water Waves Propagating at an Arbitrary Angle to the Wind

The dependence of the turbulent airflow over water waves on the angle,, between mean wind and wavedirections is investigated. To this end,an existing semi-analytical model is extended. In this model, the main simplification of the problem is obtained by using the well-established divisionof the wave boundary layer into inner and outer regions for modelling turbulence. The effect of waves on turbulence is restricted to the thin inner region. Simulations show that the influence of the wind speed component transverse to the wave direction on the air flow, and hence on the growth rate of the waves, is small. This is confirmed by calculations with a numerical model that solves the full Reynolds equations using a second-order turbulence closure scheme. The growth rate of slowly moving waves (as compared to the wind speed) is then proportional to cos², whereas, for faster waves, it has a narrower angular distribution.     

全球二维大气化学模式和大气化学成分的数值模拟

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.     

稻田土壤中甲烷产生率的实验研究

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.     

GRAPES区域集合预报模式的初值扰动增长特征

基于GRAPES-REPS（Global and Regional Assimilation and Prediction Enhanced System-Regional Ensemble Prediction System）区域集合预报模式和集合变换卡尔曼滤波（Ensemble Transform Kalman Filter,ETKF）初值扰动方法,对2015年6月1~15日10 km与15 km水平分辨率分别进行集合预报试验,通过分析ETKF初值扰动分量、初值扰动方差准确率、动能谱、扰动能量演变、日变化及集合离散度、均方根误差等特征,揭示GRAPES-REPS区域集合预报ETKF初值扰动结构及增长特征。结果表明:（1）ETKF初值扰动方案产生的扰动能够保持所有正交、不相关方向的误差方差,且ETKF分量α参数值及放大因子具有较好的稳定性。（2）ETKF初值扰动方法生成的扰动场以大尺度扰动为主,扰动结构及能量具有随流型依赖特征,低层以内能扰动为主,高层以动能扰动为主,且集合扰动可以有效捕捉预报误差的结构。（3）GRAPES区域集合预报初值扰动总能量和集合离散度随预报时效的延长均呈发展趋势,但离散度增长率小于均方根误差增长率,即集合预报总体存在集合离散度不足的问题。（4）水平分辨率提高可以增加中高层大尺度扰动波谱能量,明显改进等压面及近地面风场及温度场的集合预报效果。值得指出的是,GRAPES-REPS区域集合预报低层内能扰动能量存在明显的日变化特征,特别是青藏高原地区更加显著,需要进一步研究青藏高原初值扰动结构的合理性。     

Rate constant measurement for the reactions of OH and Cl with peroxyacetyl nitrate at 298 K

The gas phase reactions of peroxyacetyl nitrate (PAN) with OH and Cl have been studied using the discharge-flow EPR method. The rate constants are found to be k ₃=(7.5±1.4)×10^-14 and k ₄=(3.7±1.7)×10^-13 cm³ molecule^-1 s^-1 at 298 K, respectively. These results confirm that the OH+PAN reaction will be the dominant sink of PAN in the middle and upper troposphere, whereas the reaction Cl+PAN will be negligible in contrast with previous estimations.     

江西常见树种失水率分析

2006年秋季,对江西18种常见树种的枝、叶每天进行失水率和含水率的测定,建立了失水率与温度关系的数学模型,分析了树种间、枝和叶间含水率和失水率的差异,研究了失水率与时间的变化关系,并得出了不同树种的枝条失水率稳定在11 d,树叶稳定在8 d。综合含水率和失水率2个指标,认为木荷、马尾松、珊瑚树、鹅掌楸、油茶是较好的防火树种。     

Photochemistry in the Arctic Free Troposphere: Ozone Budget and Its Dependence on Nitrogen Oxides and the Production Rate of Free Radicals

Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NO_x mixing ratiosup to 300 pptv in February and for NO_x mixing ratios up to 500 pptv in May. These NO_x limits are an order of magnitude higher thanmedian NO_x levels observed, illustrating the strong dependence ofgross ozone production rates on NO_x mixing ratios for the majority of theobservations. The threshold NO_x mixing ratio needed for netpositive ozone production was also calculated to increase from NO_x 10pptv in February to 25 pptv in May, suggesting that the NO_x levels needed to sustain net ozone production are lower in winter than spring. This lower NO_x threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NO_x neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.     

生长旺盛期呼伦贝尔草甸草原生态系统呼吸与CH_4吸收通量的日变化研究

利用静态箱法于2011年结实期和2012年开花期与结实期分别对不同人类活动(自由放牧和刈割)影响下的呼伦贝尔草甸草原及相应的封育草原的CH4通量和植物土壤系统呼吸作用排放的CO2通量进行野外定位观测研究。结果表明:呼伦贝尔草甸草原(放牧和刈割及其对应的封育样地)均表现为CH4的汇,3个观测时期汇强的变化范围为:-23.98±6.40~-95.96±28.57μg Cm-2 h-1。呼伦贝尔草甸草原CH4通量的日变化对温度的响应较为复杂。不同时期呼伦贝尔草甸草原的植物土壤系统呼吸速率的日变化存在差异,水分和温度的共同影响造成2012年结实期日均CO2排放量低于2011年结实期。放牧对呼伦贝尔草甸草原CH4吸收通量的日变化模式的影响较小,但在2011年结实期和2012年开花期促进了CH4日均通量(促进幅度12.05%~93.35%),2012年结实期放牧降低了CH4日均通量(降低幅度23.32%~30.43%);刈割降低CH4吸收日均通量11.55%~60.62%。呼伦贝尔草甸草原日均累计碳排放量中CH4所占比例为0.35%~2.62%,而放牧和刈割行为对呼伦贝尔草甸草原的日均累计碳排放的影响结果在不同物候期以及不同植被群落类型均有不同。     

1992—2012年东北水稻生育期变化分析

生产实践中水稻生育期变化是气候条件和品种更新等因素共同作用的结果。利用东北地区13个农业气象站点1992—2012年水稻试验观测资料,分析水稻生育期的变化及其与东北变暖趋势、水稻品种调整的关系。结果表明：水稻生长季平均气温和≥10℃积温在1992—2001年呈显著增加趋势,水稻生长季积温的差别最大可达500℃?d,从2002年开始升温趋势减缓,并略有下降。相应地,2002—2012年与1992—2001年的物候期基本上呈现相反的变化特征,其中抽穗期、乳熟期、成熟期在1992—2001年明显提前,分别提前了3.1、2.9、4.5 d/10a,移栽期、分蘖期、成熟期则在2002—2012年呈现出明显的推迟趋势,分别推迟了4.6、4.7、2.0 d/10a;生育期的变化受多种因素影响,但播种-移栽期、乳熟-成熟期在1992—2001年分别缩短了0.7、1.6 d/10a,而在2002—2012年则分别延长了2.9、2.8 d/10a;总的来说,1992—2012年水稻全生育期整体延长了3.7 d/10a,其主要归因于营养生长期的延长。在试验资料比较完整的12个站点所做的分析表明,在东北水稻种植的生产实践中,不断地通过品种调整适应气候条件的改变,多数站点水稻实际生育期与品种审定生育日数差别较小,说明其品种的选择能够与当年的气候条件较好地匹配,充分利用了当地的气候资源。延吉站、梅河口站、通化站随着气候的持续波动又显示出水稻实际生育期与品种审定生育日数偏差增大的趋势,宁安站和前郭尔罗斯站的水稻种植品种的审定生育日数几乎没有改变。因此,迫切需要对东北气候变化的科学事实和水稻种植适应气候变化的生产实践进行系统的总结,为东北水稻生产适应气候变化提供科学支撑。     

基于模式分析一次沙尘暴过程中沙尘表面非均相化学过程对中国地区污染物浓度的影响

利用戈达德对地观测系统（GEOS）提供的再分析气象场GEOS-5驱动的GEOS-Chem模式,模拟中国地区2009年4月22~29日沙尘暴期间沙尘气溶胶表面非均相化学过程对我国污染物的影响。模拟结果表明,沙尘暴期间,全国平均沙尘硝酸盐和沙尘硫酸盐浓度分别为0.2 μg m-3和0.4 μg m-3,占总硝酸盐（非沙尘硝酸盐与沙尘硝酸盐之和）和总硫酸盐（非沙尘硫酸盐与沙尘硫酸盐之和）的24%和10%。我国西部地区沙尘硝酸盐占比（ > 80%）要大于其他地区,而西部地区的沙尘硫酸盐占比则要小于下游地区。考虑非均相化学反应后,沙尘暴期间,全国平均的二氧化硫（SO₂）、硝酸（HNO₃）、臭氧（O₃）、非沙尘硫酸盐、总硫酸盐、非沙尘硝酸盐、总硝酸盐、NH₃、总铵盐浓度变化量分别为-7%、-15%、-2%、-8%、3%、-2%、14%、21%、-5%。     

中国沙漠沙尘气溶胶对沙漠源区及北太平洋地区大气辐射加热的影响

针对2001年春季中国沙漠和北太平洋上空沙尘气溶胶的空间分布情况,利用辐射传输模式,分别计算了沙尘气溶胶对沙漠和海洋大气的辐射加热（冷却）率,并讨论了低云、中云、高云对辐射加热率的影响。结果表明:春季,位于中国沙漠和太平洋上空的沙尘层对大气具有明显的加热作用。当沙漠上空光学厚度为1.0,海洋上空光学厚度为0.3时,取春季平均太阳高度角,沙尘层对应的净辐射加热率分别为2.8 K/d和0.4 K/d。由于WMO推荐的沙尘模型比东亚沙尘模型对太阳辐射吸收强,采用该模型计算得到的中国沙漠和海洋上空的加热率比采用东亚沙尘模型分别高1.5 K/d和0.2 K/d。沙尘对大气的加热率很大程度上依赖于沙尘的大气载荷。这种依赖性首先受太阳高度角的影响, 其次也受地表反照率的影响。云对沙尘层辐射加热（冷却）率的影响与云的高度和厚度有关。低云能够加热沙漠和海洋上空的沙尘大气,冷却地面和洋面。中、高云冷却沙漠上空的沙尘层。在海洋上空,中云对云层以上的沙尘层有加热作用,对云层以下的沙尘层有冷却作用。高云对海洋上空沙尘层的辐射加热（冷却）率的影响比较小,加热还是冷却,取决于云的厚度,当云层较薄时,加热沙尘层,而当云层较厚的时候,有可能冷却沙尘层。     

EM 对稻田甲烷排放抑制作用的初步研究

该文主要讨论采用有效微生物菌剂（Effective Microorganisms）抑制稻田甲烷气体排放的试验结果。试验表明:第一年中抑制作用明显,平均在59%以上,并且使负通量（即稻田成为吸收大气中CH4的汇）的出现频率增加。这可能是EM中含有的光合细菌作用所致。试验还表明使用EM时可以取代化肥使产量增加。     

The global distribution of methane in the troposphere

Methane has been measured in air samples collected at approximately weekly intervals at 23 globally distributed sites in the NOAA/GMCC cooperative flask sampling network. Sites range in latitude from 90° S to 76° N, and at most of these we report 2 years of data beginning in early 1983. All measurements have been made by gas chromatography with a flame ionization detector at the NOAA/GMCC laboratory in Boulder, Colorado. All air samples have been referenced to a single secondary standard of methane-in-air, ensuring a high degree of internal consistency in the data. The precision of measurements is estimated from replicate determinations on each sample as 0.2%. The latitudinal distribution of methane and the seasonal variation of this distribution in the marine boundary layer has been defined in great detail, including a remarkable uniformity in background levels of methane in the Southern Hemisphere. We report for the first time the observation of a complete seasonal cycle of methane at the South Pole. A significant vertical gradient is observed between a sea level and a high altitude site in Hawaii. Globally averaged background concentrations in the marine boundary layer have been calculated for the 2 year-period May 1983–April 1985 inclusive, from which we find an average increase of 12.8 ppb per year, or 0.78% per year when referenced to the globally averaged concentration (1625 ppb) at the mid-point of this period. We present evidence that there has been a slowing down in the methane growth rate.Presented at the Conference on the Scientific Application of Baseline Observations of Atmospheric Composition (SABOAC), Aspendale, Australia, 7–9 November 1984.