Algorithm for retrieving surface pressure from hyper-spectral measurements in oxygen A-band

An algorithm for retrieving the surface pressure from oxygen A-band measurements in the future Chinese CO2 satellite （CarbonSpec/TanSat） was developed. The full physical radiative transfer model, vector radiative transfer model based on successive order of scattering, which is based on the successive order of scattering approach, was used to simulate the measurements of CarbonSpec/TanSat, as well as the kernel matrix in the inversion algorithm, and then the surface pressure and other related atmospheric parameters such as aerosol optical depth （AOD）, surface albedo, and temperature were derived through optimal estimation theory. Sensitivities of the algorithm to surface albedo, solar zenith angle （SZA）, viewing zenith angle （VZA）, aerosol type, and AOD were investigated, and the results showed that the absolute error of retrieved surface pressure increases with decreasing surface albedo or increasing SZA and VZA. An accuracy of 〈4 hPa over bright surfaces （surface albedo 〉0.15） could be derived for various SZAs and viewing geometries. Moreover, the algorithm can simultaneously retrieve the surface albedo, AOD, and its vertical distribution indicated by scale height.     

Development of CMAQ for East Asia CO2 data assimilation under an EnKF framework: a first result

Under an Ensemble Kalman Filter(EnKF)framework,Regional Atmospheric Modeling System and Models-3 Community Multi-scale Air Quality(RAMS–CMAQ)modeling system is developed to be a CO2data assimilation system EnKF–CMAQ,and the EnKF–CMAQ system is then applied to East Asia for validation with real continuous surface CO2concentration observations available in the study domain instead of using an observation simulation system experiment.Experiments with an experimental period of January 23 to February 7,2007 are conducted,and the experimental results of the EnKF–CMAQ system and the RAMS–CMAQ model are compared against continuous surface CO2observations from assimilation sites and independent reference sites.Distributions of daily mean CO2concentration increments show that the EnKF–CMAQ system confines the update of daily mean CO2within areas nearby and downwind of the assimilation sites.Both the CO2concentration ensemble spreads and background error covariances show flow-dependent patterns.The results indicate the crucial role of wind transport in the CO2data assimilation,which agrees with the previous studies.The average bias and the average root-mean-square error(RMSE)of daily mean CO2concentration at the assimilation sites are reduced by 1.00 and1.83 ppm,respectively,and those at the reference sites are reduced by 0.24 and 0.22 ppm,respectively.The results demonstrate the EnKF–CMAQ system is capable of assimilating the continuous surface CO2concentration observations to improve the simulation accuracy of the atmospheric CO2synoptic variation.Since growing CO2observations over East Asia are being available nowadays,this work is our first step to generate consistent spatial and temporal atmospheric CO2concentration fields over East Asia,particularly over China,using both in situ and satellite observations.     

星载CO2探测频率步进扫描IPDA激光雷达回波信号反演及误差分析

设计了星载CO₂探测频率步进扫描积分路径差分吸收（IPDA）激光雷达,弥补了欧洲航天局A-SCOPE项目单波长CO₂探测IPDA激光雷达对波长依赖性较强等不足.仿真计算了一个扫描周期内的激光雷达回波信号和系统的相对随机误差、大气压强不确定性误差以及频率不稳定性误差.当频率步进扫描到on-line波长为6 361.235 0 cm-1时,在海面反射率为0.035 sr-1、大气压强不确定性为0.001以及激光频率不稳定性为0.3 MHz条件下,系统综合相对误差为0.084 2%.结果表明,采用频率步进扫描方法结合IPDA激光雷达技术探测大气CO₂浓度不仅可以观察到相对误差随on-line波长变化的关系,而且可以有效地减小测量误差,使其小于0.5×10-6.      

Satellite-derived surface water pCO2 and air–sea CO2 fluxes in the northern South China Sea in summer

An empirical approach is presented for the estimation of the partial pressure of carbon dioxide (pCO2) and air–sea CO2 fluxes in the northern South China Sea in summer using satellite-derived sea surface temperatures (SSTs), chlorophyll-a (Chl a) concentrations, and wind fields. Two algorithms were tested. The first used an SST-dependent equation, and the other involved the introduction of Chl a. Regression equations were developed for summer based on in situ data obtained in July, 2004. Using the monthly average SST and Chl a fields derived from the advanced very high resolution radiometer (AVHRR) and the SeaWiFS (sea-viewing wide field of view sensor), respectively, the monthly pCO2 fields were computed. The derived pCO2 was compared with the shipboard pCO2 observations conducted in July, 2000. This resulted in a root-mean-square error of 4.6 μatm, suggesting that the satellite-derived pCO2 was in general agreement with the in situ observations. The air–sea CO2 flux was further computed with the aid of the monthly mean QuikSCAT wind speed. We contend that more shipboard data are necessary for refining the empirical algorithms and reducing the uncertainty in the results.     

Carbon isotopic composition,turnover and origins of soil CO<Subscript>2</Subscript> in a monsoon evergreen broadleaf forest in the Dinghushan Biosphere Reservoir,South China

Carbon isotopic compositions of soil CO2 in rainy season (July) from two natural soil profiles (DHLS & DHS) in the monsoon evergreen broadleaf forest in the Dinghushan Biosphere Reservoir (DBR), South China, are presented. Turnover and origins of soil CO₂ are preliminarily discussed in this paper. Results show that the content of soil CO2 varies between 6120 and 18718 ppmv, and increases with increasing depth until 75 cm, and then it declines. In DHLS, soil CO₂ δ¹³C ranges from −24.71‰ to −24.03‰, showing a significant inverse correlation (R²＝0.91) with the soil CO₂ content in the same layer. According to a model related to soil CO₂ δ¹³C, the soil CO₂ is mainly derived from the root respiration (>80%) in DHLS. While in DHS, where soil CO₂ ? 13C ranges from −25.19‰ to −22.82‰, soil CO₂ is primarily originated from the decomposition of organic matter (51%–94%), excluding the surface layer (20 cm, 90%). Radiocarbon data suggest that the carbon in soil CO₂ is modern carbon in both DHLS and DHS. Differences in ¹⁴C ages between the “oldest” and “youngest” soil CO₂ in DHLS and DHS are 8 months and 14 months, respectively, indicating that soil CO₂ in DHLS has a faster turnover rate than that in DHS. The ¹⁴C values of soil CO₂, which range between 100.0‰ and 107.2‰ and between 102.5‰ and 112.1‰ in DHLS and DHS, respectively, are obviously higher than those of current atmospheric CO₂ and SOC in the same layer, suggesting that soil CO₂ is likely an important reservoir for Bomb-¹⁴C in the atmosphere.     

Retrieval of column-averaged volume mixing ratio of CO2 with ground-based high spectral resolution solar absorption

The total column-averaged volume mixing ratio of atmospheric carbon dioxide （Xco2） has been retrieved with high spectral resolution solar absorption data obtained from ground-based Fourier transform spectrometer （FTS） measurements at Xichong, a coastal site in the district of Shenzhen in southern China. Based on differential optical absorption spectroscopy （DOAS） theory, the Xco2 was retrieved by finding the best match of observed high spectral resolution solar absorption data and monochromatic radia- tion transfer model calculations. The averaged Xco2 in the whole observation period was about 394.9 ppm. The uncertainty of the retrieval was estimated to be 2.0 ppm （0.51%） by comparing retrievals at two bands. The preliminary results show that Xc% retrieved by this method can be used to validate satellite remote sensing of Xco2.     

Trend, seasonal and diurnal variations of atmospheric CO2 in Beijing

The concentration of atmospheric CO₂ in Beijing increased rapidly at a mean growth rate of 3.7% · a⁻¹ from 1993 to 1995. After displaying a peak of (409.7±25.9) μmol · mol⁻¹ in 1995, it decreased slowly. Both the almost stable anthropogenic CO₂ source and increasing biotic CO₂ sink contribute to the drop of CO₂ concentration from 1995 to 2000. The seasonal variation of CO₂ concentration exhibits a clear cycle with a maximum in winter, averaging (426.8±20.6) μmol · mol⁻¹, and a minimum in summer, averaging (369.1±6.1) μmol·mol⁻¹. The seasonal variation of CO₂ concentration is mainly controlled by phenology. The mean diurnal variation of atmospheric CO₂ concentration for a year in Beijing is highly clear: daily maximum CO₂ concentration usually occurs at night, but daily minimum CO₂ concentration does in the daytime, with a mean diurnal difference more than 34.7 μmol·mol⁻¹. It has been revealed that the interannual variations of atmospheric CO₂ concentration in winter and autumn regulated the interannual trend of atmospheric CO₂, whereas the interannual variation of CO₂ concentration in summer affected the general tendency of atmospheric CO₂ in a less degree.     

基于差分吸收检测技术的非分散红外CO2呼吸气体传感器

采用非分散红外(non-dispersive infrared,NDIR)气体传感器实时检测呼吸气体中的CO2气体浓度,进而反映人体运动机能和代谢功能等身体状态,可以满足人类日益增强的对自身健康状况进行了解的需求.利用电调制微机电系统(micro-electro-mechanical system,MEMS)光源和双通道热释电传感器分别作为红外光源和探测器,采用气室结构设计和压电微泵相结合的方法为传感器提供稳定的气体流速,设计出红外呼吸CO2气体传感器.通过测量不同CO2标准气体浓度下热释电传感器参考通道和测量通道的电压比值进行传感器标定,获得了在室温下、检测量程0％～8％内,绝对误差小于0.5％,相对误差3％,系统响应时间小于1.5 s的传感器,提高了基于NDIR气体传感器检测呼吸气体的抗干扰能力,可望满足运动机能和代谢功能检测等应用对CO2气体监测的需求.     

Simulation of CO2 variations at Chinese background atmospheric monitoring stations between 2000 and 2009: Applying a CarbonTracker model

We carried out a downscaling treatment over China using the CarbonTracker numerical model, which was applied using double grid nesting technology (3° × 2° over the whole globe, 1° × 1° over China), simulating and analyzing atmospheric CO₂ concentrations over 10 recent years (2000–2009). The simulation results agreed very well with observed data from four background atmospheric monitoring stations in China (The periods for which the simulation results and observed values be compared were January 2000 to December 2009 for the WLG station and June 2006 to December 2009 for the SDZ, LFS, and LAN stations), giving correlation coefficients of >0.7. The high-resolution simulation data correlated slightly better than the low resolution simulation data with the observed data for three of the regions’ atmospheric background stations. Further analysis of the annual, seasonal CO₂ concentration variations at the background stations showed that the CO₂ concentration increased each year over the study period, with an average annual increase of more than 5%, and annual increases of more than 7% at the Shangdianzi and Lin’an stations. Seasonal CO₂ variations were greater at the Longfengshan station than at the Shangdianzi or Lin’an stations. However, the CO₂ concentrations were higher at the Shangdianzi and Lin’an stations because they are greatly affected by human activities in the Jingjinji and Changjiang Delta economic zones. Spatial distribution in CO₂ concentrations and fluxes were higher in eastern than in western China.     

Au@SiO2 core/shell nanoparticle-decorated TiO2 nanorod arrays for enhanced photoelectrochemical water splitting

To improve the separation efficiency of photoinduced charge carries,Au@SiO2nanoparticles(NPs)with core–shell structure were loaded onto the surface of TiO2nanorods grown on fluorine-doped tin oxide substrate by a facile two-step process.The resulted Au@SiO2/TiO2photoanodes were characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,as well as photoelectrochemical measurements.Compared with pristine TiO2nanorod film,the Au@SiO2/TiO2films showed remarkable enhancement in photoelectrochemical water splitting,with incident photonto-current conversion efficiency increasing from 31%to37%at 380 nm at 0.7 V versus saturated calomel electrode.This could be interpreted by the effect of metallic surface plasmon resonance of Au@SiO2NPs,which would generate an intense electromagnetic field with spatially nonhomogenous distributed intensity.As a result,the charge carriers generated in the near-surface region of TiO2nanorods could be easily separated.This modification method based on the effect of metallic surface plasmon resonance for promoted charge carrier separation provides a promising way to develop semiconductor photoelectrodes with high solar water-splitting performance.     

注超临界CO_2开采高温废弃气藏地热机制与采热能力分析

高温废弃气藏具有巨大的地热开采潜力。在对比分析超临界CO2和常规携热介质水的热物性基础上,提出注超临界CO2开采高温废弃气藏地热的方法。利用数值模拟方法对CO2在高温废弃气藏中的采热能力及影响因素进行评估。结果表明,由于CO2具有很高的可注性和流动性,超临界CO2的采热速率可达到水的1.5倍;利用CO2循环开采高温气藏地热,不仅可以实现高效地热开发,还可以实现CO2地质埋存;对废弃气藏而言,可以充分利用现有井网和地面设施,减少初期资本投入,实现高温废弃气藏地热的有效和经济开发,进一步提高气藏的利用价值,延长其经济寿命。     

Incorporating temporal variability to improve geostatistical analysis of satellite-observed CO2 in China

Observations of atmospheric carbon dioxide (CO2 ) from satellites offer new data sources to understand global carbon cycling. The correlation structure of satellite-observed CO2 can be analyzed and modeled by geostatistical methods, and CO2 values at unsampled locations can be predicted with a correlation model. Conventional geostatistical analysis only investigates the spatial correlation of CO2 , and does not consider temporal variation in the satellite-observed CO2 data. In this paper, a spatiotemporal geostatistical method that incorporates temporal variability is implemented and assessed for analyzing the spatiotemporal correlation structure and prediction of monthly CO2 in China. The spatiotemporal correlation is estimated and modeled by a product-sum variogram model with a global nugget component. The variogram result indicates a significant degree of temporal correlation within satellite-observed CO2 data sets in China. Prediction of monthly CO2 using the spatiotemporal variogram model and spacetime kriging procedure is implemented. The prediction is compared with a spatial-only geostatistical prediction approach using a cross-validation technique. The spatiotemporal approach gives better results, with higher correlation coefficient (r2 ), and less mean absolute prediction error and root mean square error. Moreover, the monthly mapping result generated from the spatiotemporal approach has less prediction uncertainty and more detailed spatial variation of CO2 than those from the spatial-only approach.     

Antilocalization sensing of interactions between two-dimensional electrons and surface species

We apply antilocalization measurements to experimentally study the interactions and exchange between InAs surface accumulation electrons and local magnetic moments of the rare earth ions Sm3?,Gd3?,Ho3?,and Dy3?,of the transition metal ions Ni2?,Co2?,and Fe3?,and of Fe3O4nanoparticles and Fe3?-phthalocyanine deposited on the surface.The influence of the deposited species on the surface electrons is observed through the changes in the spin–orbit scattering and magnetic spin-flip scattering rates,which carry information about magnetic interactions.Experiments indicate a temperature-dependent magnetic spin-flip scattering for Ho3?,Dy3?,Ni2?,and Co2?.Concerning the spin–orbit scattering rate,we observe an increase,except for the cases of Ni2?,Fe3?,Fe3O4nanoparticles and Fe3?-phthalocyanine.We also observe an increase in SO scattering in another system where we study the interactions of Au nanoparticles and ferromagnetic Co0.6Fe0.4nanopillars and an In0.53Ga0.47As quantum well.Experimental results are analyzed and compared to theoretical models.Our method provides a controlled way to probe the quantum properties of two-dimensional electron systems,either on the surface of InAs or in a quantum well.     

High efficiency synthesis of HKUST-1 under mild conditions with high BET surface area and CO2 uptake capacity

This study focuses on the development of a hydrothermal method for the rapid synthesis of good quality copper benzene-1,3,5-tricarboxylate(referred to as HKUST-1)with high yield under mild preparation conditions to address the issues associated with reported methods.Different synthesis conditions and activation methods were studied to understand their influence on the properties of HKUST-1.It was found that mixing the precursors at50°C for 3 h followed by activation via methanol refluxing led to the formation of a product with the highest BET specific surface area of 1615 m~2/g and a high yield of 84.1%.The XRD and SEM data illustrated that the product was highly crystalline.The sample was also tested on its capacity in CO_2 adsorption.The results showed strong correlation between surface area of the sample and its CO_2 uptake at 1 bar and 27°C.The HKUST-1 prepared in this study demonstrated a high CO_2 uptake capacity of 4.2 mmol/g.It is therefore concluded that this novel and efficient method can be used in the rapid preparation of HKUST-1 with high surface area and CO_2 uptake capacity.     

CO2混相调节剂驱油机理室内研究

为了深入了解混相调节剂降低CO_2/原油最小混相压力的作用,测试CO_2混相调节剂降低最小混相压力的机理,开展了室内实验,并深入研究调节剂的效果。实验结果表明,混相调节剂可以降低CO_2/原油表面张力、促进CO_2抽提原油轻质组分效果、增加CO_2在原油中溶解度、降低原油黏度的作用;其中,主要的机理为降低表面张力和提高抽提轻质组分效果;当原油中调节剂质量浓度达0.3%以上,气液表面张力消失,达到混相;加入调节剂后,采出端气体突破时,CO_2萃取、抽提轻质烃体积百分数增加14倍以上。调节剂作用机理研究,深入了对调节剂改善CO_2驱油效果的认识,并对进一步筛选和研发新型调节剂具有指导意义。     

Effect of H2S concentration on the corrosion behavior of pipeline steel under the coexistence of H2S and CO2

The effect of H2S concentration on H2S/CO2 corrosion of API-X60 steel was studied by scanning electron microscopy, a weight-loss method, potentiodynamic polarization tests, and the electrochemical impedance spectroscopy technique. It is found that the cor-rosion process of the steel in an environment where H2S and CO2 coexist at different H2S concentrations is related to the morphological structure and stability of the corrosion product film. With the addition of a small amount of H2S, the size of the anode reaction region is de-creased due to constant adsorption and separation of more FeS sediment or more FeHS＋ions on the surface of the steel. Meanwhile, the dou-ble-layer capacitance is diminished with increasing anion adsorption capacity. Therefore, the corrosion process is inhibited. The general cor-rosion rate of the steel rapidly decreases after the addition of a small amount of H2S under the coexistence of H2S and CO2. With a further increase in H2S concentration, certain parts of the corrosion product film become loose and even fall off. Thus, the protection provided by the corrosion product film worsens, and the corrosion rate tends to increase.     

CO2和O2共注入下方解石溶解对黄铁矿氧化固铀的影响

我国大型可地浸砂岩型铀矿床普遍存在黄铁矿和方解石与铀矿物密切共生现象。中性地浸采铀过程中O₂和CO₂的共注入会诱导黄铁矿氧化和方解石溶解,目前针对二者共存体系中方解石溶解对黄铁矿氧化固铀的影响尚不明确。本文通过静态批实验和数值模拟的方法对比研究了CO₂和O₂条件下方解石溶解对黄铁矿氧化固铀的影响。结果表明:无CO₂分压下中性Tris缓冲体系中黄铁矿氧化对U(VI)的吸附率高达90%,有CO₂分压下碳酸铀酰体系中铀的固定率明显降低,约有32%的铀被吸附。在方解石和黄铁矿共存体系中,单独通O₂条件下铀的吸附率为27%,CO₂和O₂共通时黄铁矿氧化对铀的吸附率仅为2%,结合数值模拟结果表明O₂₊黄铁矿+方解石体系和CO₂₊O₂₊黄铁矿+方解石体系中Ca₂(UO₂)(CO₃)₃质量比分别为80%和95%。X射线衍射(X-ray diffraction,XRD)、X射线光电子能谱(X-ray photoelectron spectroscopy,XPS)和傅里叶红外光谱(Fourier transform infrared,FT-IR)结果表明黄铁矿表面发生微氧化形成针铁矿和纤铁矿会增加U(VI)的吸附,方解石溶解促进Ca-UO₂-CO₃络合物的形成影响了黄铁矿及其氧化产物对U(VI)的固定,提高了U(VI)的迁移能力。     

CO2的温室效应饱和度分析及其大气体积分数预测模型

通过精确的LBLRTM逐线积分模式建立CO_2体积分数变化模型,分析了CO_2的温室效应饱和度,并对未来地表温升的变化趋势进行了预测.结果表明,目前CO_2的持续排放只能使其在680cm~(-1)强吸收带中心达到饱和,而在未来相当长一段时间内,其仍将通过该吸收带的翼区以及1 000cm~(-1),1 350cm~(-1)与1 900cm~(-1)等弱吸收带对地表红外辐射表现出强烈的吸收,CO_2的温室效应还远未达到饱和;如果按照当前CO_22.2(mL/·m~(-3))/a的年排放速率,CO_2的大气体积分数将会持续增加,从而造成地表温度不断升高,到2056年,地表温升将会达到2K.     

Changes of photosynthetic capacity of some plant species under very high CO2 concentrations in Biosphere 2

Conclusions The initial slope of A/ light curve became steep under high CO₂ (700 μmol · mol^-1) compared with that under low CO₂ (350 μmol · mol^-1) for the C₃ species growing in very high CO₂(>2 200 μmol · mol^-1) for a long period. The light compensation points remained unchanged, but the light saturation points were found increased. The ϕ_m,_app and A_max of the C₃ species increased respectively by 79 % and 80 %, while those of C₄ species decreased by 10% and 14%, respectively. The shape of A/light curve of C₄ species did not change. Such results indicated that C₃ species increased the capacity of photosynthesis, while C₄ did not change, otherwise it decreased a little. This work only compared the changes of capacity in photosynthesis of some species under different CO₂ levels in Biosphere 2. We need further investigation on the effects of high CO₂ on the same species outside Biosphere 2, in order to fully undertand the effects and mechanism of response of plants to the elevated CO₂.     

The v-v energy transfer of highly vibrationally excited states (I)

The relaxation of the highly vibrationally excited CO (v = 1–8) by CO₂ is studied by timeresolved Fourier transform infrared emission spectroscopy (TR FTIR). 193 nm laser photolysis of the mixture of CHBr₃ with O₂ generates the highly vibrationally excited CO(v) molecules. TR FTIR records the intense infrared emission of CO(v→v-1). The vibrational populations of each level of CO(v) have been determined by the method of spectral simulation. Based on the evolution of the time resolved populations and the differential method, 8 energy transfer rate constants of CO(v = 1–8) to CO₂ molecules areobtained: (5.7±0.1), (5.9±0.1), (5.2±0.2), (3.4±0.2), (2.4±0.3), (2.2±0.4), (2.0±0.4) and (1.8±0.6) (10¹⁴ cm³ · molecule⁻¹ · s⁻¹), respectively. A two-channel energy transfer model can explain the feature of the quenching of CO(v) by CO². For the lower vibrational states of CO, the vibrational energy transfers preferentially to the u³ mode of CO² For the higher levels, the major quenching channel changes to the vibrational energy exchange between CO(v→v-1) and the u¹ mode of CO².