HIAPER Pole-to-Pole Observations (HIPPO): fine-grained, global-scale measurements of climatically important atmospheric gases and aerosols

The HIAPER Pole-to-Pole Observations (HIPPO) programme has completed three of five planned aircraft transects spanning the Pacific from 85 °?N to 67 °?S, with vertical profiles every approximately 2.2 ° of latitude. Measurements include greenhouse gases, long-lived tracers, reactive species, O(2)/N(2) ratio, black carbon (BC), aerosols and CO(2) isotopes. Our goals are to address the problem of determining surface emissions, transport strength and patterns, and removal rates of atmospheric trace gases and aerosols at global scales and to provide strong tests of satellite data and global models. HIPPO data show dense pollution and BC at high altitudes over the Arctic, imprints of large N(2)O sources from tropical lands and convective storms, sources of pollution and biogenic CH(4) in the Arctic, and summertime uptake of CO(2) and sources for O(2) at high southern latitudes. Global chemical signatures of atmospheric transport are imaged, showing remarkably sharp horizontal gradients at air mass boundaries, weak vertical gradients and inverted profiles (maxima aloft) in both hemispheres. These features challenge satellite algorithms, global models and inversion analyses to derive surface fluxes. HIPPO data can play a crucial role in identifying and resolving questions of global sources, sinks and transport of atmospheric gases and aerosols.     

Emission characteristics of coal combustion in different O2/N2, O2/CO2 and O2/RFG atmosphere

This study investigates the emission characteristics of CO(2), SO(2) and NOx in the flue gas of coal combustion by varying the compositions and concentrations of feed gas (O(2)/CO(2)/N(2)) and the ratios of recycled flue gas. The differences between O(2)/recycled flue gas (O(2)/RFG) combustion and general air combustion are also discussed. Experimental results indicate that the maximum concentration of CO(2) in O(2)/CO(2) combustion system is 95% as the feed gas is 30% O(2)/70% CO(2). The average concentration of CO(2) in the flue gas of O(2)/CO(2) coal combustion system is higher than 90% and much higher than that of O(2)/N(2) coal combustion system. This high concentration of CO(2) is beneficial for the separation of CO(2) from the flue gas by adsorption or absorption technologies. The maximum concentration of CO(2) in O(2)/N(2) combustion system is only 34% at the feed gas 50% O(2)/50% N(2), the concentration of CO(2) is increased with the concentration of O(2) in feed gas. By O(2)/CO(2) combustion technology, higher concentration of SO(2) is produced as the feed gas is 30% O(2)/70% CO(2) or 40% O(2)/60% CO(2), while higher concentration of NOx is produced as the feed gas is 20% O(2)/80% CO(2) or 50% O(2)/50% CO(2). The mass flow rates of CO(2), SO(2) and NOx in the flue gas are all increased with the ratio of recycled flue gas except for the feed gas 20% O(2)/80% CO(2). The enhanced mass flow rates of air pollutants in such O(2)/RFG combustion system are also beneficial for improving the control efficiencies of air pollution control devices. By O(2)/N(2) combustion technology, higher concentrations of SO(2) and NOx are produced as the feed gas is 21% O(2)/79% N(2). The results also indicate that the formation of NOx in general air combustion system is higher than that in O(2)/RFG or O(2)/CO(2) combustion system.     

PLLA/PBAT单轴拉共混膜的力学性能及气体透过性

目的研究单轴拉伸聚乳酸/聚对苯二甲酸丁二酯(PLLA/PBAT)共混薄膜的热学、力学和气体透过性能。方法通过双螺杆熔融挤出后再进行单轴拉伸,制备出不同共混比例的无定型PLLA/PBAT共混薄膜材料,并对其热学、力学和气体透过性进行研究。结果 PLLA和PBAT是个完全不相容的共混体系,PBAT的添加加速了PLLA的冷结晶速度,改善了单轴拉伸PLLA薄膜的纵向和横向的柔韧性,最大断裂伸长率可达29%。提高了气体透过性和CO_2/O_2选择透过性,CO_2/O_2透过比相对于纯PLLA的3.8提高到7.6。结论柔性PBAT的添加改善了PLLA的刚性,提高了材料的柔韧性,PBAT对CO_2有较好的吸附性和扩散性,提高了材料的CO_2透过量和CO_2/O_2选择透过性能。     

Determination of δ(18)O and δ(15)N in Nitrate

The analyses of both O and N isotopic compositions of nitrate have many potential applications in studies of nitrate sources and reactions in hydrology, oceanography, and atmospheric chemistry, but simple and precise methods for these analyses have yet to be developed. Testing of a new method involving reaction of potassium nitrate with catalyzed graphite (C + Pd + Au) at 520 °C resulted in quantitative recovery of N and O from nitrate as free CO(2), K(2)CO(3), and N(2). The δ(18)O values of nitrate reference materials were obtained by analyzing both the CO(2) and K(2)CO(3) from catalyzed graphite combustion. Provisional values of δ(18)O(VSMOW) for the internationally distributed KNO(3) reference materials IAEA-N3 and USGS-32 were both equal to +22.7 ± 0.5‰. Because the fraction of free CO(2) and the isotopic fractionation factor between CO(2) and K(2)CO(3) were constant in the combustion products, the δ(18)O value of KNO(3) could be calculated from measurements of the δ(18)O of free CO(2). Thus, δ(18)O(KNO)((3)) = aδ(18)O(free)(?)(CO)((2)) - b, where a and b were equal to 0.9967 and 3.3, respectively, for the specific conditions of the experiments. The catalyzed graphite combustion method can be used to determine δ(18)O of KNO(3) from measurements of δ(18)O of free CO(2) with reproducibility on the order of ±0.2‰ or better if local reference materials are prepared and analyzed with the samples. Reproducibility of δ(15)N was ±0.1‰ after trace amounts of CO were removed.     

Airborne laser infrared absorption spectrometer (ALIAS-II) for in situ atmospheric measurements of N2O, CH4, CO, HCl, and NO2 from balloon or remotely piloted aircraft platforms

The Airborne Laser Infrared Absorption Spectrometer II (ALIAS-II) is a lightweight, high-resolution (0.0003-cm(-1)), scanning, mid-infrared absorption spectrometer based on cooled (80 K) lead-salt tunable diode laser sources. It is designed to make in situ measurements in the lower and middle stratosphere on either a balloon platform or high-altitude remotely piloted aircraft. Chemical species that can be measured precisely include long-lived tracers N(2)O and CH(4), the shorter-lived tracer CO, and chemically active species HCl and NO(2). Advances in electronic instrumentation developed for ALIAS-I, with the experience of more than 250 flights on board NASA's ER-2 aircraft, have been implemented in ALIAS-II. The two-channel spectrometer features an open cradle, multipass absorption cell to ensure minimal contamination from inlet and surfaces. Time resolution of the instrument is 相似文献   

Mobile Fourier-transform infrared spectroscopy monitoring of air pollution

Fourier transform infrared spectroscopy is an efficient technique for the detection and quantification of molecules in gas mixtures. Measurement results from a mobile laboratory for ambient air analysis and for remote sensing of plume emission with the commercially available K300 spectrometer are reported. CO, CO(2), NO, NO(2), N(2)O, NH(3), CH(4), SO(2), H(2)O, HCl, and HCHO concentrations have been determined with good agreement with in situ results. The on-line multicomponent analysis software is based on line-by-line retrieval and least-squares fitting procedures, including the effects of multiple aerosol scattering and cloud and rain influences.     

SPIRALE: a multispecies in situ balloonborne instrument with six tunable diode laser spectrometers

The balloonborne SPIRALE (a French acronym for infrared absorption spectroscopy by tunable diode lasers) instrument has been developed for in situ measurements of several tracer and chemically active species in the stratosphere. Laser absorption takes place in an open Herriott multipass cell located under the balloon gondola, with six lead salt diode lasers as light sources. One mirror is located at the extremity of a deployable mast 3.5 m below the gondola, enabling the measurement of very low abundance species throughout a very long absorption path (up to 544 m). Three successful flights have produced concentration measurements of O3, CO, CO2, CH4, N2O, NO2, NO, HNO3, HCl, HOCl, COF2, and H2O2. Fast measurements (every 1.1 s) allow one to obtain a vertical resolution of 5 m for the profiles. A detection limit of a few tens of parts per trillion in volume has been demonstrated. Uncertainties of 3%-5% are estimated for the most abundant species rising to about 30% for the less abundant ones, mainly depending on the laser linewidth and the signal-to-noise ratio.     

气调包装对超市常温销售的鲜切芹菜品质影响研究

在超市常温销售的环境下,分别选用体积分数(后同)为5% O2,15% CO2,80% N2;10% O2,10% CO2,80% N2;20% O2,60% CO2,20% N2 3种气调比例对鲜切芹菜进行气调包装.测定芹菜的失重率,黄化率,维生素C,叶绿素和感官评价等指标.实验结果表明,在这3种气调搭配中,10% O2,10% CO2,80% N2对鲜切芹菜的品质保存效果最好.     

新鲜竹笋气调保鲜技术的研究

采用O2(2%)+CO2(5%)+N2(93%),O2(80%)+CO2(5%)+N2(15%),O2(80%)+CO2(20%)气调比例包装新鲜竹笋,研究不同气调处理对竹笋保鲜效果的影响。评测竹笋在保存期间水分损失率、L 值、电导率、多酚氧化酶活力、过氧化物酶活力、抗坏血酸、感官品质的变化。结果显示,O2(80%) +CO2(20%) 组水分损失少,L值变化小,电导率上升缓慢,PPO,POD 酶活力低,抗坏血酸含量高,感官品质得分高,贮藏保鲜效果好,贮藏至15d, 仍具有良好的商品品质。     

Wide-range sounding of free-tropospheric water vapor with a differential-absorption lidar (DIAL) at a high-altitude station

A differential absorption lidar (DIAL) system has been developed for the measurement of water vapor throughout the free troposphere [3 to 12 km above sea level (asl.)] with high vertical resolution varied from 50 m next to the ground to 300 m above an altitude of 10 km. The system was installed at the Schneefernerhaus high-altitude research station (2675 m asl., Zugspitze, Germany). The DIAL system is based on a tunable single-mode laser system with a high pulse energy of currently 250 mJ and a repetition rate of 20 s(-1). For lidar operation with energies typically between 100 mJ and 150 mJ and an integration time of 1000 s (10000 laser shots for both DIAL wavelengths) a vertical range of at least 10 km has been demonstrated even under dry conditions and during daytime, while daytime measurements up to 12 km have been possible under humid conditions. The system was intercompared with radiosondes, which suggests an agreement within 5% in a major part of the operating range. Further improvements are planned in the upper troposphere to approach the accuracy requirements needed in climate research.     

高氧气调包装对金针菇保鲜品质的影响

研究了不同气体配比条件对金针菇保鲜效果的影响。 分别用 3% O2 +97% N2 ,80% O2 +20% N2 ,80% O2 +10% N2 +10% CO2 ,80% O2 +20% CO2 气体配比充气包装金针菇,空气包装为对照组。 评定其水分损失率、呼吸强度、色差、相对电导率、多酚氧化酶(PPO)、过氧化物酶(POD)和感官指标等。 结果表明,80% O2 +20% CO2 组水分损失、颜色变化最少,PPO 酶活力、呼吸强度最低,POD 酶活力较高,感官变化最小,贮藏保鲜效果好。     

Application of mixed oxide catalysts to the removal of lean NOx and N2O using transient-mode cyclic operations

The storage and reduction of NO and N2O in the presence of excess O2 have been investigated over two mixed oxide catalysts. The catalysts, which were prepared via coprecipitation of solutions of mixed metal nitrates, followed by calcination, were found to have plenty storage capacities for nitrogen oxides. The storage and reduction performances varied with the catalyst composition and the duration of cycle time: the AlCoPd (1/1/0.05) mixed oxide catalyst exhibited higher efficiency for NO, and an AlCoFe (1/1/2) mixed oxide catalyst exhibited higher efficiency for N2O. The adsorptions of NO and N2O onto the mixed oxide catalysts progressed without an oxidation step, and the adsorptivity of NO surpassed that of O2. The mixed oxides showed spinel structures with sizes of 10-100 nm, and with well-developed mesopores that were formed by the evaporation of H2O and CO2 from layered double hydroxide (LDH) precursors. The storage and reduction of lean NOx and N2O over the mixed oxide catalysts were carried out via cyclic operations in a transient mode at 300 degrees C and at space velocities of around 30,000 h(-1). The removal efficiency of the cyclic operations generally increased with reduced adsorption cycle time, and reached 90% for NOx and N2O with the respective catalysts.     

Gliding arc plasma processing of CO2 conversion

Conversion of carbon dioxide (CO2) using gliding arc plasma was performed. The research was done to investigate the effect of variation of total gas flow rates and addition of auxiliary gases--N2, O2, air, water--to the CO2 conversion process. This system shows higher power efficiency than other nonthermal plasma methods. Experiment results indicate the conversion of CO2 reaches 18% at total gas flow rate of 0.8 L/min and produces CO and O2 as the main gaseous products. Among auxiliary gases, only N2 gives positive effect on CO2 conversion and the power efficiency at N2 concentration of 95% and total gas flow rate of 2 L/min increases about three times compared to pure CO2 process.     

Complete CO oxidation over Cu2O nanoparticles supported on silica gel

We find that nearly monodisperse copper oxide nanoparticles prepared via the thermal decomposition of a Cu(I) precursor exhibit exceptional activity toward CO oxidation in CO/O2/N2 mixtures. Greater than 99.5% conversion of CO to CO2 could be achieved at temperatures less than 250 degrees C for over 12 h. In addition, the phase diagram and pathway for CO oxidation on Cu2O (100) is computed by ab initio methods and found to be in qualitative agreement with the experimental findings.     

The atmospheric signature of carbon capture and storage

Compared with other industrial processes, carbon capture and storage (CCS) will have an unusual impact on atmospheric composition by reducing the CO(2) released from fossil-fuel combustion plants, but not reducing the associated O(2) loss. CO(2) that leaks into the air from below-ground CCS sites will also be unusual in lacking the O(2) deficit normally associated with typical land CO(2) sources, such as from combustion or ecosystem exchanges. CCS may also produce distinct isotopic changes in atmospheric CO(2). Using simple models and calculations, we estimate the impact of CCS or leakage on regional atmospheric composition. We also estimate the possible impact on global atmospheric composition, assuming that the technology is widely adopted. Because of its unique signature, CCS may be especially amenable to monitoring, both regionally and globally, using atmospheric observing systems. Measurements of the O(2)/N(2) ratio and the CO(2) concentration in the proximity of a CCS site may allow detection of point leaks of the order of 1000 ton CO(2) yr(-1) from a CCS reservoir up to 1 km from the source. Measurements of O(2)/N(2) and CO(2) in background air from a global network may allow quantification of global and hemispheric capture rates from CCS to the order of ±0.4 Pg C yr(-1).     

Validation of a rotational coherent anti-Stokes Raman spectroscopy model for carbon dioxide using high-resolution detection in the temperature range 294-1143 K

Experiments were performed in the temperature range of 294-1143 K in pure CO(2) using high-resolution rotational coherent anti-Stokes Raman spectroscopy (CARS), in the dual-broadband approach. Experimental single-shot spectra were recorded with high spectral resolution using a single-mode Nd:YAG laser and a relay imaging lens system on the exit of a 1 m spectrometer. A theoretical rotational CARS model for CO(2) was developed for evaluation of the experimental spectra. The evaluated mean temperatures of the recorded single-shot dual-broadband rotational coherent anti-Stokes Raman spectroscopy (DB-RCARS) spectra using this model showed good agreement with thermocouple temperatures, and the relative standard deviation of evaluated single-shot temperatures was generally 2-3%. Simultaneous thermometry and relative CO(2)/N(2)-concentration measurements were demonstrated in the product gas of premixed laminar CO/air flames at atmospheric pressure. Although the model proved to be accurate for thermometry up to 1143 K, limitations were observed at flame temperatures where temperatures were overestimated and relative CO(2)/N(2) concentrations were underestimated. Potential sources for these discrepancies are discussed.     

分离氧化亚氮和二氧化碳的变压吸附方法研究

介绍了使用变压吸附方法分离氧化亚氮和二氧化碳的实验研究,使用自制的改性吸附剂TK-103,在0.2MPa的吸附压力下,可将实验配制的含N_2O混合气中的CO_2脱除至20×10-6以下,且净化气中的N_2O收率达到约80%,该方法具有操作压力低、CO_2脱除精度高、N_2O回收率高、设备投资低及操作能耗省的优点,特别适用于从己二酸尾气中回收提纯氧化亚氮。     

Co-adsorption of CO and oxygen on W(110) surfaces

Influence of oxygen adsorption on CO chemisorption behavior over W(110) surfaces was studied using valence band spectra and thermal desorption spectroscopy (TDS). In the absence of O, CO formed a tilted and a vertical structure at 120 K on W(110). In the presence of O coadsorbate, in contrast, formation of the tilted structure of CO was suppressed. CO desorption from oxygen-covered W(110) surfaces showed indication of a strong interaction between adsorbates at ∼900 K, which was absent without O.     

Detection of H2O and CO2 with distributed feedback diode lasers: measurement of broadening coefficients and assessment of the accuracy levels for volcanic monitoring

We reproduced the chemical-physical conditions of fumarolic emission at Phlaegrean Fields, Pozzuoli, Italy, and we measured the CO(2) and H(2)O concentrations using an absorption spectrometer based on two distributed feedback laser diodes at wavelengths of 1.578 and 1.393 mum. We discuss the accuracy levels of the different methods used. Furthermore, we measured the broadening coefficients for H(2)O (self-broadening, 28.2 +/- 0.6 MHz/Torr; CO(2) broadening, 6.0 +/- 0.4 MHz/Torr) and CO(2) (self-broadening, 3.2 +/- 0.1 MHz/Torr; H(2)O broadening, 4.0 +/- 0.1 MHz/Torr). Using the present data, we evaluated a minimum detectable variation of 9% for H(2)O and 1% for CO(2).     

External cavity diode laser based photoacoustic detection of CO2 at 1.43 microm: the effect of molecular relaxation

Photoacoustic spectroscopy, based on an external cavity diode laser operating at 1431 nm, was used for measuring CO2 concentration as a minority component in a gas mixture. By using N2 as a buffer gas, a molecular relaxation effect was observed, which influenced both the amplitude and the phase of the measured photoacoustic signal and consequently reduced the sensitivity of the PA system. This molecular relaxation effect could be suppressed by adding water vapor of a constant and relatively high (approximately 4%) concentration to the gas sample. In parallel with this, the arising spectral interference between H2O and CO2 necessitated the development of a simple yet efficient signal analysis method, which increased the sensitivity of the system by more than one order of magnitude and accordingly reduced the minimum detectable CO2 concentration down to approximately 1000 ppm.