江苏地区二氧化碳浓度时空分布特征分析

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.     

东亚地区二氧化碳体积分数变化特征

利用2004年以来东亚地区10个本底观测站大气φ(CO₂)观测资料,分析了各站大气φ(CO₂)的变化特征及其各站之间的差异,讨论了下垫面特征、源汇作用等对φ(CO₂)变化的影响.结果表明:10个本底站大气月均φ(CO₂)有明显的季节变化,高值多出现在冬春等寒冷季节,而低值则多出现在6—9月,属于北半球的夏季;大气φ(CO₂)日变化趋势较为一致,15时(当地时间)前后达到全天最低,随后φ(CO₂)升高,并在日落后继续积累,至清晨7时(当地时间)前后达到全天最高,之后φ(CO₂)随着太阳辐射的增强而逐渐降低,且平均φ(CO₂)水平与下垫面植被量成反比,φ(CO₂)日变化的幅度与下垫面植被量成反比.作为全球基准站之一的瓦里关山站,2004—2008年φ(CO₂)年均值逐年增加,年增长率为2.28×10^-6/a.     

钢铁工业CO2的排放现状及主要的捕集方法

简要讨论了目前CO₂等温室气体的危害、钢铁工业CO₂的排放现状及来源,并针对我国钢铁行业的发展状况,分析了温室气体CO₂的捕集方法.     

海洋对人为CO2吸收的三维模式研究

文中用包含海洋化学过程和一个简单生物过程的三维碳循环模式模拟了海洋对大气CO₂的吸收,并分析了碳吸收的纬度分布。模拟工业革命以来海洋对大气CO₂的吸收表明:海洋碳吸收再加上大气CO₂的增加只占由化石燃料燃烧、森林砍伐和土地利用的变化而释放到大气中的CO₂的2/3。1980～1989年期间海洋年平均吸收2.05GtC。海洋人为CO₂的吸收有明显的纬度特征。模式计算的海洋CO₂的吸收在总量与纬度分布上与观测结果比较相符。     

大气CO2浓度升高及气候变化对作物冠层光合影响的数值模拟

利用美国Licor-6200光合作用测定仪,对黄淮海地区代表性冬小麦品种鲁麦23号叶片光合作用速率进行了较为全面的测定,分别确定了冬小麦叶片光—光合作用响应曲线和CO₂—光合作用响应曲线,在此基础上,建立了叶片光合作用模式,并进而建立了一个具有瞬时时间尺度,空间积分为叶片尺度的冬小麦冠层模式,利用模式分别分析了大气中CO₂浓度升高和温度变化对冠层光合作用的不同影响,并在此基础上进一步进行了综合数值分析。单因子分析表明:晴天状况下,冠层光合速率随CO₂浓度升高而上升,当CO₂浓度由330×10^-6上升至660×10^-6时,冠层光合日总量可增加19.7%;冠层光合速率随辐射增加而增大,辐射量增加10.0%,冠层光合日总量可增加6.7%;冠层光合速率随温度升高而下降,温度升高1℃,冠层光合日总量减少2.9%。多因子综合数值分析表明:在辐射量较大的气候背景下,冠层光合日总量对温度和CO₂变化响应更加敏感。本文的实测数据为研究气候变化对中国农业影响提供了最基本的可靠模型参数,冠层光合模型为未来改进作物模型提供了理论基础。     

应用涡动相关法计算水热、CO2通量的国内外进展概况

目前涡动相关法被认为是国内外测定CO₂、水热通量的最可靠方法。国外应用此方法解决了均匀下垫面假设下森林和农田等生态系统的CO₂、水热通量的计算问题,目前致力于非理想下垫面(真实地形)的CO₂、水热通量的计算。而国内应用涡动相关技术起步较晚,用此方法测定水热通量已有一定的知识积累,但测定CO₂通量还处于资料收集阶段。我国自然生态系统、环境外交和社会经济可持续发展都要求精确查明我国CO₂的时空变化特征和动力学机制,这应是今后研究的重点,并提出了应用该方法存在的主要问题及可能的解决方法,指出值得深入研究的领域。     

锡林浩特草原CO2通量特征及其影响因素分析

利用锡林浩特国家气候观象台开路涡度相关系统、辐射土壤观测系统,测得的长期连续通量观测数据,对锡林浩特草原2009—2011年期间的CO₂通量观测特征进行了分析。结果表明:CO₂通量存在明显的年际、季节和日变化特征。3 a中NEE年际变率达到200 g·m^-2,季节变率最大达到460 g·m^-2,日变化幅度生长季最大达到0.25 mg·m^-2·s^-1。通过不同时间尺度碳通量与温度、水分、辐射等环境因子的分析,认为CO₂通量日变化主要受温度和光合有效辐射影响,而季节变化和年变化主要受降水和土壤含水量的影响。降水强度及时间分布是制约牧草CO₂吸收的关键因素,大于15%的土壤含水量有利于促进牧草生长。     

大气CO2富集对根际NaCl盐渍的人参果植株干物质生产和水分利用的影响

对单株砂培盆栽的半木质化枝条扦插生根的一月龄人生果(Solanum muricatum Ait.)栽培品种"Xotus",每周浇两次200mL NaCl质量浓度分别为0mg·L^-1和25mg·L^-1的Hoagland营养液处理2个月,第二个月在控制空气CO₂体积分数为(350±10)×10^-6、(700±10)×10^-6和(1050±10)×10^-6的植物生长箱内试验。结果表明,人参果植株干物质生产量和耗水量受根际NaCl盐渍而下降,又随大气CO₂升高而增加。根际NaCl盐渍能增大植株叶片蒸腾系数、根/冠比和干物质向枝干和根部分配的比例及积累量,降低根系吸收水分的效率和耗水量。升高大气CO₂能促进叶片发育及干物质向地上部其他器官和地下部组织分配,增加总叶面积、比叶干重和各种器官中干物质增长量,提高干物质生产率和水分利用率。根际经25mg·L^-1NaCl盐渍处理的植株,总干物质增长量和水分利用率相应下降50%～54%和24%～37%;与350×10^-6CO₂的处理的植株相比,700×10^-6及1050×10^-6CO₂的处理分别使这两项指标提高到79%～106%和61%～88%以及133%～189%和99%～142%。大气CO₂富集能改善受NaCl盐渍的植株干物质生产力、提高水分利用率。根际NaCl盐渍和大气CO₂富集对人参果植株干物质生产和水分利用有生物互作效应。它们的共同作用会促进植株干物质的增长及叶片中合成的干物质向其他器官分配,提高干物质生产率和水分利用率,同时减少总叶面积、枝条和根系干重、根系吸水效率、植株耗水量和叶片蒸腾系数。因此,全球大气CO₂富集将有利于该作物的干物质生产和水分利用。     

膜基—气体吸收耦合分离混合气中CO2性能评价

在膜基—气体吸收耦合实验装置上,评价了疏水性PP(聚丙烯)微孔膜,活化MDEA(N-甲基二乙醇胺)溶液分离混合气中CO₂传质性能,研究了气液流速、吸收剂和混合气的浓度等因素对总传质系数的影响,采用阻力层关联方程模型预测总传质系数K_ov值。结果表明:活化MDEA溶液能提高总传质系数K_ov值,模型的计算值和实验值符合较好。     

黑云杉林大气CO2稳定同位素组成δ13C,δ18O的分析

研究CO₂稳定同位素特征可以揭示光合、呼吸作用等众多信息,从而有助于了解生态系统与环境之间的碳循环过程。利用大气CO₂浓度及其稳定同位素的测定资料,分析稳定同位素比δ¹³C、δ¹⁸O,发现两者具有相似的时空分布特征。主要表现在δ¹³C和δ¹⁸O在冠层内具有明显的垂直变化趋势,冠层上部重同位素含量较高,而底部含量较低。从时间变化看,δ¹³C和δ¹⁸O在午后到日落具有较高的水平,而凌晨,δ¹³C和δ¹⁸O较低。运用Keeling图法分析δ¹³C、δ¹⁸O和CO2浓度的关系,发现δ¹³C值主要受光合和呼吸作用影响,与CO₂浓度的高低密切相关;而δ¹⁸O的变化比较复杂,因为δ¹⁸O除受光合、呼吸强度影响外,还取决于环境空气湿度。     

The NO2 Absorption Spectrum. IV: The 200–400 nm Region at 220 K

Previous experiments in the 400–500 nm region (Coquart et al., 1995) have been extended to the 200–400 nm region to determine the absorption cross-sections of NO₂ at 220 K. The NO₂ and N₂O₄ cross-sections are obtained simultaneously from a calculation applied to the data resulting from measurements at low pressures. A comparison between the NO₂ cross-sections at 220 K and at ambient temperature shows that the low temperature cross-sections are generally lower, except in the region of the absorption peaks. Comparisons are also made with previous data at temperature close to 220 K.     

Variations in atmospheric CO2 at the Meteorological Research Institute, Tsukuba, Japan

Since April 1986, measurements of the CO₂ concentration in the surface air have been conducted at the Meteorological Research Institure (MRI, 36°04 N, 140°07 E, 25 m above sea level) in Tsukuba, located 50 km northeast of Tokyo, Japan. The CO₂ data measured over times between 11:00 Japan Standard Time (JST) and 16:00 JST (C _N ) were considered to be representative of the air (within a few ppmv) in the planetary boundary layer. To evaluate the representative CO₂ level on a spatial scale larger than that of the C _N record, the CO₂ data with hour-to-hour variation less than 1 ppmv were selected (C _P ). Comparison of these data with those of Ryori (39°02 N, 141°50 E), a continental station operated by the Japan Meteorological Agency, indicates that the C _P record provides a representative CO₂ level in the air on spatial scales of at least a few hundred kilometers.The C _N record allows an investigation of the internanual changes in photosynthesis/respiration against changes in climatological parameters. Within a small temperature anomaly (ca.±1 °C) respiration is sensitive to the temperature change, while photosynthesis is less sensitive. When the temperature anomaly is large, however, photosynthesis and respiration tend to be competitive.     

NO<Subscript>3</Subscript> Vertical Profile Measurements from Remote Sensing Balloon-Borne Spectrometers and Comparison with Model Calculations

Eleven vertical profiles of stratospheric NO₃ have been obtained since 1992 using the AMON and SALOMON balloon-borne UV-visible spectrometers. The measurements are compared to the SLIMCAT 3D model and calculations based on the steady-state hypothesis for NO₃. The calculations cannot reproduce some parts of the profiles which exhibit strong concentration fluctuations over few kilometres, as a consequence of the dependence of NO₃ on local temperature variations. A statistical use of the data allows us to estimate the influence of the temperature dependence of the absorption cross-section on the data analysis, and the validity of the recommended reaction rates available in the literature. Discrepancies exist between the model based on recommended kinetics and observations at warmer temperatures. Nevertheless, the analysis is biased by local temperature inhomogeneities, and only a low-resolution vertical shape of the NO₃ profiles can be retrieved.     

Photochemistry of N2O4 Adsorbed on Ice Surfaces at 193 nm

A multi-layer deposited ice film was prepared through water vapor deposition on a Ni plate in a vacuum chamber at 90 K, and was used as it was or after annealing at 140 K. NO₂ was adsorbed as N₂O₄ approximately 90 K on the ice film prepared as above, and irradiated by 193 nm excimer laser light. The time-of-flight (TOF) spectra of the desorbed species, i.e., NO₂, NO, O₂ and O, were measured by a quadrupole mass spectrometer. The photochemical process obeyed an one-photon process. The relative yields of the products and their TOF spectra were dependent on the preparation condition of the ice film and also varied with the continuation of the laser irradiation. From the ice film annealed at 140 K, NO₂, NO and O₂ were desorbed with an approximate ratio of 1:1:0.01. From the non-annealed film, the relative yield of NO₂ was much smaller than that of NO. The TOF spectrum of NO from the non-annealed ice film consisted of distinctly different two components corresponding to the 1700 and 100 K translational temperature, respectively. The fast component was lost when additional ice was deposited on the adsorbed N₂O₄. NO was supposed to be a predissociation product from the electronically excited NO₂ prepared through the photodissociation of N₂O₄.     

我国东西部地区地气温差的年代际变化特征

利用1960~2006年我国地温、气温逐日4个时次[02:00(北京时间,下同)、08:00、14:00和20:00]的台站观测资料,计算并分析了我国东南、西北地区各季地气温差的年代际变化特征。分析结果表明:我国东南部地区各季地气温差在20世纪70年代末以前,大部分年份偏高,高于平均值,而在20世纪70年代末以后,我国东南部地区各季地气温差偏低,在夏季和冬季表现尤为明显。我国西北地区春季和夏季地气温差在20世纪70年代末以前大部分年份偏低,低于平均值;而在20世纪70年代末以后,地气温差则大部分年份明显偏高。我国西北地区秋季地气温差的年代际变化特征不明显,而冬季地气温差的年代际变化趋势与春夏季相反,在20世纪70年代末以前大部分年份偏高,高于平均值,而在20世纪70年代末以后偏低。另外,发现地温和气温对我国东南、西北地区各季地气温差的年代际变化在各季所起的贡献作用不同。     

Heterogeneous Chemistry and the O3 Budget in the Lower Mid-Latitude Stratosphere

A photochemical box model including a detailed heterogeneous chemistrymodule has been used to analyze in detail the effects of temperature andaerosol surface area on odd oxygen production/depletion in the lowerstratosphere at 30° S. Results show that for background aerosolloading, the hydrolysis of BrONO₂ and N₂O₅are most important atall temperatures studied except when the temperature falls below about205 K, when ClONO₂ hydrolysis becomes most important. Thisprocessing leads to removal of active nitrogen to form nitric acid andenhancement of HO_x, BrO_x, ClO_x levels. Detailed O₃ budgets asa function of temperature are presented showing how ozone loss andproduction terms vary with changes in stratospheric sulfate aerosol loadingfor the individual families. For (most) aerosol loading levels, thelargest ozone losses occurred at warmer temperatures due to the strongtemperature dependence of the NO_x ozone-destroying reactions. Theexception to this occurred for the conditions representative of volcanicloading, which showed a strong increase in ozone destruction due toincreases in destruction from the ClO_x and HO_x families.The ozoneproduction term k[NO][HO₂] did not show a strong dependence oneithertemperature or aerosol loading, due to the offsetting effect of reducedNO_xand increased HO_x concentrations.     

Products and Mechanism of the NO<Subscript>3</Subscript> Reaction with Thiophene

Products of the gas-phase reaction of the NO₃ radical with thiophene have been investigated using different experimental systems. On the one hand, experiments have been conducted in our laboratory using two different methods, a Teflon static reactor coupled to a gas chromatograph combined with mass-spectrometry (GC-MS) and a discharge flow tube with direct MS spectroscopic detection. A qualitative analysis in these cases indicates that possible products for the reaction of thiophene+NO₃ at room temperature include: sulphur dioxide, acetic and formic acids, a short-chain aldehyde, 2-nitrothiophene and 3-nitrothiophene. On the other hand, quantitative experiments have been performed in the European Photoreactor (EUPHORE) in Valencia, Spain. In this case, the major products were: HNO₃ (≈80%), nitrothiophenes (≈30%), SO₂ (≈20%), propanal (3%) and a fraction of particles (≈10%). The results obtained indicate that at least 70% of the reaction of NO₃ with thiophene proceeds by an H-abstraction process at room temperature. The mechanism of the reaction studied is proposed on the basis of experimental results.     

Multi-Model Projection of July–August Climate Extreme Changes over China under CO_2 Doubling. Part II: Temperature

This is the second part of the authors’ analysis on the output of 24 coupled climate models from the Twentieth-Century Climate in Coupled Models (20C3M) experiment and 1% per year CO 2 increase experiment (to doubling) (1pctto2x) of phase 3 of the Coupled Model Inter-comparison Project (CMIP3). The study focuses on the potential changes of July–August temperature extremes over China. The pattern correlation coefficients of the simulated temperature with the observations are 0.6–0.9, which are higher than the results for precipitation. However, most models have cold bias compared to observation, with a larger cold bias over western China (>5°C) than over eastern China (<2°C). The multi-model ensemble (MME) exhibits a significant increase of temperature under the 1pctto2x scenario. The amplitude of the MME warming shows a northwest–southeast decreasing gradient. The warming spread among the models (～1°C– 2°C) is less than MME warming (～2°C–4°C), indicating a relatively robust temperature change under CO 2 doubling. Further analysis of Geophysical Fluid Dynamics Laboratory coupled climate model version 2.1 (GFDL-CM2.1) simulations suggests that the warming pattern may be related to heat transport by summer monsoons. The contrast of cloud effects also has contributions. The different vertical structures of warming over northwestern China and southeastern China may be attributed to the different natures of vertical circulations. The deep, moist convection over southeastern China is an effective mechanism for "transporting" the warming upward, leading to more upper-level warming. In northwestern China, the warming is more surface-orientated, possibly due to the shallow, dry convection.     

The equilibrium constant of NO2 with N2O4 and the temperature dependence of the visible spectrum of NO2: A critical review and the implications for measurements of NO2 in the polar stratosphere

Measurements of stratospheric NO₂ by ground-based visible spectrometers rely on laboratory measurements of absorption cross-sections. We review low-temperature laboratory measurements, which disagree by amounts claimed to be significant. Our recalculation of their errors shows that in general disagreements are not significant and that errors in the ratios of cross-sections at low to room temperature are between ±3% and ±8.8%. Of these errors, up to ±3.5% was contributed by errors in the equilibrium constant,K _p, in those measurements where the pressure was above 0.1 mbar.We review measurements and calculations ofK _p, which were accurate to ±5% from 300 to 233 K. Each method was potentially flawed. For example, infrared measurements of the partial pressure of NO₂ ignored the dependence of absorption on total pressure. From thermodynamic theory, formulae forK _pcan be derived from expressions for the variation of heat capacity with temperature. Contrary to common belief, coefficients in the formulae used by spectroscopists were not derived from the thermodynamic quantities. Rather, they were fitted to measurements or to calculations. Hence, they are empirical and it is dangerous to extrapolate below 233 K, the lowest temperature of the measurements.There are no measurements of NO₂ cross-sections below 230 K. Extrapolation of these cross-sections to analysis of measurements of NO₂ at the low temperatures of the Arctic and Antarctic stratosphere is also dangerous. For satisfactory analysis of polar spectra, the NO₂ cross-sections should be measured at temperatures down to 190 K with a relative accuracy of ±1%. This difficult experiment would need a cell of minimum length 32 m whose length can be adjusted. Because their effects are circular, many errors cannot be removed simply. Although circular errors also arise in the measurements ofK _pand of the infrared spectrum, their weights differ from those in the visible spectrum. The optimum experiment might therefore simultaneously measure the visible and infrared spectra andK _p.     

Impact of precursor levels and global warming on peak ozone concentration in the Pearl River Delta Region of China

The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.