Estimates of anthropogenic CO<Subscript>2</Subscript> uptake in a global ocean model

A global ocean general circulation model (L30T63) is employed to study the uptake and distribution of anthropogenic CO₂ in the ocean. A subgrid-scale mixing scheme called GM90 is used in the model. There are two main GM90 parameters including isopycnal diffusivity and skew (thickness) diffusivity. Sensitivities of the ocean circulation and the redistribution of dissolved anthropogenic CO₂ to these two parameters are examined. Two runs estimate the global oceanic anthropogenic CO₂ uptake to be 1.64 and 1.73 Pg C yr^-1 for the 1990s, and that the global ocean contained 86.8 and 92.7 Pg C of anthropogenic CO₂ at the end of 1994, respectively. Both the total inventory and uptake from our model are smaller than the data-based estimates. In this presentation, the vertical distributions of anthropogenic CO₂ at three meridional sections are discussed and compared with the available data-based estimates. The inventory in the individual basins is also calculated. Use of large isopycnal diffusivity can generally improve the simulated results, including the exchange flux, the vertical distribution patterns, inventory, storage, etc. In terms of comparison of the vertical distributions and column inventory, we find that the total inventory in the Pacific Ocean obtained from our model is in good agreement with the data-based estimate, but a large difference exists in the Atlantic Ocean, particularly in the South Atlantic. The main reasons are weak vertical mixing and that our model generates small exchange fluxes of anthropogenic CO₂ in the Southern Ocean. Improvement in the simulation of the vertical transport and sea ice in the Southern Ocean is important in future work.     

Consequences of Uncertainties in CO<Subscript>2</Subscript> Density for Estimating Net Ecosystem CO<Subscript>2</Subscript> Exchange by Open-path Eddy Covariance

Errors in the estimation of CO₂ surface exchange by open-path eddy covariance, introduced during the removal of density terms [Webb et al. Quart J Roy Meteorol Soc 106:85–100, (1980) - WPL], can happen both because of errors in energy fluxes [Liu et al. Boundary-Layer Meteorol 120:65–85, (2006)] but also because of inaccuracies in other terms included in the density corrections, most notably due to measurements of absolute CO₂ density (ρ _c ). Equations are derived to examine the propagation of all errors through the WPL algorithm. For an open-path eddy covariance system operating in the Sierra de Gádor in south-east Spain, examples are presented of the inability of an unattended, open-path infrared gas analyzer (IRGA) to reliably report ρ _c and the need for additional instrumentation to determine calibration corrections. A sensitivity analysis shows that relatively large and systematic errors in net ecosystem exchange (NEE) can result from uncertainties in ρ _c in a semi-arid climate with large sensible heat fluxes (H _s ) and (wet) mineral deposition. When ρ_c is underestimated by 5% due to lens contamination, this implies a 13% overestimation of monthly CO₂ uptake.     

Comparative Measurements Of Co2flux Over A Forest Using Closed-Path And Open-Path Co2analysers

An eddy covariance system using a closed-path CO₂analyser was constructed for long-term CO₂flux measurements above a forest, and its total frequency response was valuated experimentally. The amplitude and phase responses of the system wereexamined through a preliminary test, in which a prescribed pattern of CO₂fluctuation was input to the system. The result showed that the amplitude of the output from the system was attenuated as frequency increased, with a half-power frequency of 0.3 Hz. The phase was delayed by the air sampling through a long tube, but the delay in phase decreased asfrequency increased. We then presented a new technique for the correction of flux loss due to the inadequate system response for the eddy covariance measurements of CO₂ flux. Using the present system and the correction technique, diurnal variations in CO₂ flux were measured over a temperate deciduous forest on three days in 1997. The results were compared with the CO₂fluxes measured with a fast response open-path gas analyser. The CO₂fluxes from the closed-path system agreed with those from the open-path system after the Webb, Pearman and Leuning correction was made for the latter. In the present test over a forest, the contribution of the frequency-response correction to the CO₂fluxes was small and its averaged percentage was only 3%in the daytime. However, the percentage would likely increase, if the system were applied to a shorter vegetation site where high frequency components are more important. The comparison confirmed that we can obtain correct measurements of CO₂flux using the present closed-path system and the correction technique.     

Multi-Phase Chemistry of C<Subscript>2</Subscript> and C<Subscript>3</Subscript> Organic Compounds in the Marine Atmosphere

A box model is used to explore the detailed chemistry of C₂ and C₃ organic compounds in the marine troposphere by tracing the individual reaction paths resulting from the oxidation of ethane, ethene, acetylene, propane, propene and acetic acid. The mechanisms include chemical reactions in the gas phase and in the aqueous phase of clouds and aerosol particles at cloud level under conditions resembling those in the northern hemisphere. Organic hydroperoxides are found to be important intermediate products, with subsequent reactions leading partly to the formation of mixed hydroxy or carbonyl hydroperoxides that are readily absorbed into cloud water, where they contribute significantly to the formation of multifunctional organic compounds and organic acids. Organic hydroperoxides add little to the oxidation of sulfur dioxide dissolved in the aqueous phase, which is dominated by H₂O₂. Next to acetaldehyde and acetone, glycol aldehyde, glyoxal, methyl glyoxal and hydroxy propanone are prominent oxidation products in the gas and the aqueous phase. Acetaldehyde is not efficiently converted to acetic acid in clouds; the major local sources of acetic acid are gas-phase reactions. Other acids produced include hydroperoxy acetic, glycolic, glyoxylic, oxalic, pyruvic, and lactic acid. The mechanism of Schuchmann et al. (1985), which derives glycolic and glyoxylic acid from the oxidation of acetate, is found unimportant in the marine atmosphere. The principal precursors of glyoxylic acid are glyoxal and glycolic acid. The former derives mainly from acetylene and ethene, the latter from glycolaldehyde, also an oxidation product of ethene. The oxidation of glyoxylic acid leads to oxalic acid, which accumulates and is predicted to reach steady state concentrations in the range 30–90 ng m⁻³. This is greater, yet of the same magnitude, than the concentrations observed over the remote Pacific Ocean.     

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。     

On the relationship between the eddy covariance,the turbulent flux,and surface exchange for a trace gas such as CO<Subscript>2</Subscript>

In the context of CO₂ surface exchange estimation, an analysis combining the basic principles of diffusion and scalar conservation shows that the mixing ratio is the appropriate variable both for defining the (eddy covariance) turbulent flux and also for expressing the relationship between the turbulent flux and surface exchange in boundary-layer budget equations. Other scalar intensity variables sometimes chosen, both the CO₂ density and molar fraction, are susceptible to the influence of surface exchange of heat and water vapour. The application of a hypsometric analysis to the boundary-layer “control volume” below the tower measurement height reveals flaws in previously applied approaches: (a) incompressibility cannot be assumed to simplify mass conservation (the budget in terms of CO₂ density); (b) compressibility alone makes the analysis of mass conservation vulnerable to uncertainties associated with resultant non-zero vertical velocities too small to measure or model over real terrain; and (c) the WPL (Webb et al. (1980) Quart J Roy Meteorol Soc 106:85–100) “zero dry air flux” assumption is invalidated except at the surface boundary. Nevertheless, the definition and removal of the WPL terms do not hinge upon this last assumption, and so the turbulent CO₂ flux can be accurately determined by eddy covariance using gas analysers of either open- or closed-path design. An appendix discusses the necessary assumptions and appropriate interpretations for deriving the WPL terms.     

On the Significance of the Webb Correction to Fluxes

For establishing correct mass or energy balances at the Earth's surface, detailed and correct measurements of air constituent fluxes are needed. Flux measurements obtained from the eddy covariance technique have to pass several corrections of different relevance in order to give correct flux data. One of these corrections, the Webb correction, is analysed herein from latent heat flux and CO₂ flux data recorded during two field experiments. The significance of this correction for the latent heat flux data varies with the air humidity and the Bowen ratio. The correction changes the latent heat flux values only a little, but significantly (by 2 to 3%). For other air constituents (like CO₂), the Webb correction is much more important (20 to 30% of the flux).     

Satellite Measurements of Tropospheric Column O<Subscript>3</Subscript> and NO<Subscript>2</Subscript> in Eastern and Southeastern Asia: Comparison with a Global Model (MOZART-2)

Satellite measurements of tropospheric column O₃ and NO₂ in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O₃ is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO₂ is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O₃ and NO₂ fields. The analysis of the model results show that the industrial emission of NO_x (NO + NO₂) contributes about 50%–80% to tropospheric column NO₂ in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NO_x to tropospheric column O₃ ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NO_x emissions have a small effect on tropospheric O₃ in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NO_x on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.     

Long-term effects of anthropogenic CO<Subscript>2</Subscript> emissions simulated with a complex earth system model

A new complex earth system model consisting of an atmospheric general circulation model, an ocean general circulation model, a three-dimensional ice sheet model, a marine biogeochemistry model, and a dynamic vegetation model was used to study the long-term response to anthropogenic carbon emissions. The prescribed emissions follow estimates of past emissions for the period 1751–2000 and standard IPCC emission scenarios up to the year 2100. After 2100, an exponential decrease of the emissions was assumed. For each of the scenarios, a small ensemble of simulations was carried out. The North Atlantic overturning collapsed in the high emission scenario (A2) simulations. In the low emission scenario (B1), only a temporary weakening of the deep water formation in the North Atlantic is predicted. The moderate emission scenario (A1B) brings the system close to its bifurcation point, with three out of five runs leading to a collapsed North Atlantic overturning circulation. The atmospheric moisture transport predominantly contributes to the collapse of the deep water formation. In the simulations with collapsed deep water formation in the North Atlantic a substantial cooling over parts of the North Atlantic is simulated. Anthropogenic climate change substantially reduces the ability of land and ocean to sequester anthropogenic carbon. The simulated effect of a collapse of the deep water formation in the North Atlantic on the atmospheric CO₂ concentration turned out to be relatively small. The volume of the Greenland ice sheet is reduced, but its contribution to global mean sea level is almost counterbalanced by the growth of the Antarctic ice sheet due to enhanced snowfall. The modifications of the high latitude freshwater input due to the simulated changes in mass balance of the ice sheet are one order of magnitude smaller than the changes due to atmospheric moisture transport. After the year 3000, the global mean surface temperature is predicted to be almost constant due to the compensating effects of decreasing atmospheric CO₂ concentrations due to oceanic uptake and delayed response to increasing atmospheric CO₂ concentrations before.     

Reductions of PM<Subscript>2.5</Subscript> in Beijing-Tianjin-Hebei urban agglomerations during the 2008 Olympic Games

The Atmospheric Environmental Monitoring Network successfully undertook the task of monitoring the atmospheric quality of Beijing and its surrounding area during the 2008 Olympics.The results of this monitoring show that high concentrations of PM2.5 pollution exhibited a regional pattern during the monitoring period(1 June-30 October 2008).The PM2.5 mass concentrations were 53 μg m 3,66 μg m 3,and 82 μg m 3 at the background site,in Beijing,and in the Beijing-Tianjin-Hebei urban agglomerations,respectively.The PM2.5 levels were lowest during the 2008 Olympic Games(8-24 August):35 μg m 3 at the background site,42 μg m 3 in Beijing and 57 μg m 3 in the region.These levels represent decreases of 49%,48%,and 56%,respectively,compared to the prophase mean concentration before the Olympic Games.Emission control measures contributed 62%-82% of the declines observed in Beijing,and meteorological conditions represented 18%-38%.The concentration of fine particles met the goals set for a "Green Olympics."     

An Alternative Approach for CO2 Flux Correction Caused by Heat and Water Vapour Transfer

Energy and CO₂ fluxes are commonly measured above plant canopies using an eddy covariance system that consists of a three-dimensional sonic anemometer and an H₂O/CO₂ infrared gas analyzer. By assuming that the dry air is conserved and inducing mean vertical velocity, Webb et al. (Quart. J. Roy. Meteorol. Soc. 106, 85-100, 1980) obtained two equations to account for density effects due to heat and water vapour transfer on H₂O/CO₂ fluxes. In this paper, directly starting with physical consideration of air-parcel expansion/compression, we derive two alternative equations to correct for these effects that do not require the assumption that dry air is conserved and the use of the mean vertical velocity. We then applied these equations to eddy flux observations from a black spruce forest in interior Alaska during the summer of 2002. In this ecosystem, the equations developed here led to increased estimates of CO₂ uptake by the vegetation during the day (up to about 20%), and decreased estimates of CO₂ respiration by the ecosystem during the night (approximately 4%) as compared with estimates obtained using the Webb et al. approach.     

Intercomparison of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>, SO<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and aromatic hydrocarbons measured by a commercial DOAS system and traditional point monitoring techniques

A field-based intercomparison study of a(DOAS) instrument (OPSIS AB, Sweden) andcommercial Differential Optical Absorption Spectroscopydifferent point-sample monitoring techniques (PM, basedon an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted inBeijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2,03, benzene, and toluene were monitored continuously during the four months. A good agreement betweenthe DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene,and NO obtained by DOAS were significantly lower than those measured by the point monitors. Theozone levels monitored by the DOAS were generally higher than those measured by point monitors. Theseresults may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics atthe measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer ofthe DOAS system, the error in the DOAS analysis can also not be excluded.     

Reconstructed light extinction coefficients using chemical compositions of PM<Subscript>2.5</Subscript> in winter in Urban Guangzhou,China

The objective of this study was to reconstruct light extinction coefficients (b ext ) according to chemical composition components of particulate matter up to 2.5 μm in size (PM 2.5 ). PM 2.5 samples were collected at the monitoring station of the South China of Institute of Environmental Science (SCIES, Guangzhou, China) during January 2010, and the online absorbing and scattering coefficients were obtained using an aethalometer and a nephelometer. The measured values of light absorption coefficient by particle (b ap ) and light scattering coefficient by particle (b sp ) significantly correlated (R 2 > 0.95) with values of b ap and b sp that were reconstructed using the Interagency Monitoring of Protected Visual Environments (IMPROVE) formula when RH was <70%. The measured b ext had a good correlation (R 2 > 0.83) with the calculated b ext under ambient RH conditions. The result of source apportionment of b ext showed that ammonium sulfate [(NH 4 ) 2 SO 4 ] was the largest contributor (35.0%) to b ext , followed by ammonium nitrate (NH 4 NO 3 , 22.9%), organic matter (16.1%), elemental carbon (11.8%), sea salt (4.7%), and nitrogen dioxide (NO 2 , 9.6%). To improve visibility in Guangzhou, the effective control of secondary particles like sulfates, nitrates, and ammonia should be given more attention in urban environmental management.     

Actinic flux and photolysis frequency comparison computations using the model PHOTOGT

The accurate radiative transfer model GOMETRAN, initially designed to yield radiances at TOA in the wavelength range 240–790 nm, has been extended to allow for the computation of actinic fluxes down to 175 nm and for the calculation of photolysis frequencies in the atmosphere. The capability of the extended model PHOTOGT (PHOTOGOMETRAN) is demonstrated in a number of successful comparison studies both with recent experiments (ground-based, balloonborne, airborne) and model calculations of radiances, actinic fluxes and photolysis frequencies in the stratosphere and troposphere. In an atmospheric case study, the impact of new quantum yield data for the O₃ » O₂+O(¹ d) photodissociation channel on the photolytic production of O(¹ d) atoms in the lower atmosphere has been quantified.     

太平洋海气CO2通量对气候事件的响应

应用一个嵌套了海洋生物地球化学循环的太平洋环流碳循环模式,分析了1960～2000年太平洋不同海区海气碳通量随时间的变化。模拟结果显示,赤道太平洋为大气CO₂的排放区,南、北太平洋(南、北纬15°至模式计算区域南、北边界)为吸收区。3个海区海气碳通量随时间均存在显著的波动,其中赤道太平洋海气碳通量年际波动最显著。3个海区海气碳通量年际波动对气候事件的响应并不一致,在El Niño年赤道太平洋冷舌的强度和总溶解无机碳(DIC)的浓度以及输出生产力均会受到上升流减弱的影响而降低,La Niña年这些海气碳通量控制要素的分布情况则正好相反,但在南北太平洋副热带以及高纬度海区,El Niño和La Niña对这些要素带来的影响却并不一定相反,对输出生产力的影响甚至是一致的。以海表温度(SST)为例考察海气碳通量与物理场之间的关系表明,在赤道太平洋上升流对DIC的影响是控制海气碳通量变化的主要因素,而在其他海区,尤其是副热带海区,由于垂直运动的年际变化较小,且生物生产力水平较低,SST的波动对海气碳通量年际变化的影响更加重要。     

[Bmin][BF4]+AMP复合溶液捕集温室气体CO2

采用基于离子液体[Bmin][BF₄]+AMP作为捕集CO₂的复合溶液,在膜吸收-热再生循环装置上,研究了该复合溶液捕集CO₂的过程和传质性能;通过阻力层传质模型,比较了预测值与实验值.结果表明：在相同条件和较高负载下,复合溶液具有较高的传递推动力和更高的传质系数;模型预测值和实验值符合较好,平均误差为12.8%.实验证明复合溶液的传质性能优于单一溶液.     

Influence of leaf water potential on diurnal changes in CO2 and water vapour fluxes

Mass and energy fluxes between the atmosphere and vegetation are driven by meteorological variables, and controlled by plant water status, which may change more markedly diurnally than soil water. We tested the hypothesis that integration of dynamic changes in leaf water potential may improve the simulation of CO₂ and water fluxes over a wheat canopy. Simulation of leaf water potential was integrated into a comprehensive model (the ChinaAgrosys) of heat, water and CO₂ fluxes and crop growth. Photosynthesis from individual leaves was integrated to the canopy by taking into consideration the attenuation of radiation when penetrating the canopy. Transpiration was calculated with the Shuttleworth-Wallace model in which canopy resistance was taken as a link between energy balance and physiological regulation. A revised version of the Ball-Woodrow-Berry stomatal model was applied to produce a new canopy resistance model, which was validated against measured CO₂ and water vapour fluxes over winter wheat fields in Yucheng (36°57′ N, 116°36′ E, 28 m above sea level) in the North China Plain during 1997, 2001 and 2004. Leaf water potential played an important role in causing stomatal conductance to fall at midday, which caused diurnal changes in photosynthesis and transpiration. Changes in soil water potential were less important. Inclusion of the dynamics of leaf water potential can improve the precision of the simulation of CO₂ and water vapour fluxes, especially in the afternoon under water stress conditions.