Comparison of chemical solvents for mitigating CO2 emissions from coal-fired power plants

There is a growing concern about the effect of greenhouse gases on global warming. Among the many greenhouse gases, CO₂ produced from burning fossil fuels is a major contributor due to the huge volumes emitted into the atmosphere. According to the estimates of the Intergovernmental Panel on Climate Change (IPCC), a worldwide reduction in the emission of greenhouse gases by more than 60% is necessary to avert significant global climate changes.This paper examines the key issues involved in greenhouse gas emissions from coal-fired power plants. At the present time, absorption by chemical solvents appears to be best option for the separation of CO₂ from low pressure flue gas streams. The costs of separation and disposal of CO₂ from existing coal fired, air blown boilers are estimated to increase the cost of electricity by about 75%. Therefore, there is a need to optimize the selection of processing solvents and operating parameters to minimize the cost of separation. Increasing the inlet flue gas pressure did not improve mass transfer rates sufficiently to compensate for the higher compression costs. The effects of other process variables were also examined.In this work, we have examined the cost effectiveness of six ethanolamine-based solvents. Overall, monoethanolamine (MEA) was found to be the best solvent.     

A cavity ring-down analyzer for measuring atmospheric levels of methane, carbon dioxide, and water vapor

Researchers investigating global climate change need measurements of greenhouse gases with extreme precision and accuracy to enable the development and benchmarking of better climate models. Existing atmospheric monitors based on non-dispersive infrared (NDIR) sensors have known problems – they are non-linear, sensitive to water vapor concentration, and susceptible to drift. Many cannot easily be simultaneously calibrated across different sites to the level of accuracy required for use in atmospheric studies. We present results from field trials by Pennsylvania State University and the National Oceanographic and Atmospheric Administration (NOAA) of a newly available analyzer, based on cavity ring-down spectroscopy (CRDS), capable of measuring the concentrations of carbon dioxide (CO₂) and water vapor (H₂O). In addition, we present data from a new analyzer which measures CO₂, methane (CH₄), and H₂O. PACS  07.88.+y     

SO2 cooling and detection of the greenhouse effect

Summary Greenhouse effect calculations normally take into account the greenhouse gases’s (CO₂ mainly) warming effect. Only recently the inclusion of the cooling effect due to different gases (SO₂ mainly) has been suggested. Zecca and Brusa have proposed that the historical evolution of SO₂ production might have caused the apparent global cooling in the period 1940–1970 and might still now hinder the detection of greenhouse warming. In this paper it is shown that the SO₂ hypothesis could lead to a definite detection of the greenhouse warming provided that the globally averaged minimum daily and maximum daily temperatures were studied.     

A study of greenhouse gases and air trajectories at Plateau Rosa

Summary The attention paid to changes in atmospheric concentrations of greenhouse gases has recently increased, with particular regard to the relationships between variations of their annual trends and of their shorter-period fluctuations on the one hand, and some geophysical and biological natural processes (like atmospheric transport, volcanic eruptions, ENSO events, seasonal vegetation cycles, and so on) on the other hand. Careful analysis and interpretation of the above relationships, in fact, can often disclose unknown mechanisms acting on modulations of these gases and make it possible for us to better understand the contributions made to them by natural causes, contrasted with anthropogenic ones. This paper presents and discusses the results of a series of CO₂ air concentration data, measured at Plateau Rosa (3480 m a.s.l.—Italian Western Alps) over a period of about four years, and correlated with atmospheric transport processes on synoptic scale. These results have shown the leading role played by some kinds of atmospheric circulation patterns in creating situations of not fully mixed air streams (and, as such, not representative of background conditions) and have also suggested a ?meteorological? selection scheme for CO₂ data to be used in evaluating more reliable annual trends.     

MgO-decorated carbon nanotubes for CO2 adsorption: first principles calculations

The global greenhouse effect makes it urgent to deal with the increasing greenhouse gases.In this paper the performance of MgO-decorated carbon nanotubes for CO 2 adsorption is investigated through first principles calculations.The results show that the MgO-decorated carbon nanotubes can adsorb CO 2 well and are relatively insensitive to O 2 and N 2 at the same time.The binding energy arrives at 1.18 eV for the single-MgO-decorated carbon nanotube adsorbing one CO 2 molecule,while the corresponding values for O 2 and N 2 are 0.55 eV and 0.06 eV,respectively.In addition,multi-molecule adsorption is also proved to be very satisfactory.These results indicate that MgO-decorated carbon nanotubes have great potential applications in industrial and environmental processes.     

A brief introduction and some background to the article JQSRT 1998;60:1025-31 and its companion

This note provides a short introduction, some background information and relevant history related to reprint of the article “Atmospheric remote-sensing reference data from GOME: Part 1. Temperature-dependent absorption cross-sections of NO₂ in the 231-794 nm range” (JQSRT 1998;60:1025-31). The article and its companion “Atmospheric remote-sensing reference data from GOME: 2. Temperature-dependent absorption cross sections of O₃ in the 231-794 nm range” (JQSRT 1999;61:509-17) provided timely and unique data sets of the absorption cross sections of Nitrogen dioxide, NO₂, and ozone, O₃. The reported absorption cross sections have a spectral resolution sufficient to distinguish the electronic vibrational and rotational features of NO₂ and O₃ and were made in the temperature range of relevance to the earth's atmosphere, viz. 200-300 K, over a wide spectral range. These species are two of the most important trace gases in earth's atmosphere, and play key roles in determining the chemistry and dynamics of the earth's atmosphere and the conditions at the earth's surface experienced by the biosphere. Whilst providing valuable information about the electronic states of NO₂ and O₃, these spectra were determined primarily for their exploitation in the retrieval of trace gases from measurements of solar back scattered radiation by ground based and space borne instrumentation. These yield the local and global amounts and distributions of NO₂ and O₃, thereby constraining our knowledge about atmospheric chemistry and dynamics and the impact of pollution from the local to the global scale. The measurement, publication and use of these spectral sets are among many important milestones in the development of atmospheric remote sensing.     

温室气体及碳同位素比值红外光谱反演精度的影响因素研究

由于傅里叶变换红外光谱(FTIR)技术在定量反演中受到气体温度、压强等气体特性以及水汽交叉吸收的影响, 使其在温室气体及碳同位素比值高精度检测领域的应用受到限制. 本文首先研究了气体特性与水汽吸收敏感性修正方法; 然后,结合实验研究中建立的敏感性修正函数, 对标准气体实测数据进行了气体特性敏感性修正, 修正后,五种测量组分的精密度均有明显提高, 其标准偏差降低倍数分布在1.80到3.38之间. 研究结果对于FTIR技术在大气本底温室气体及碳同位素比值高精度监测领域的应用具有重要意义.     

Photonic sensing of the atmosphere by absorption spectroscopy

Chemically reactive atmospheric species play a crucial role in tropospheric processes which affect regional air quality and global climate change. Contrary to long-lived species such as greenhouse gases, interference-free accurate and precise concentration assessments of strongly reactive short-lived species represent a real challenge. In this paper, we report on the recent progress in spectroscopic instrumental developments for monitoring of OH, NO₃, HONO and NO₂ by using modern photonic sources (Quantum Cascade Laser, distributed feedback diode laser, light emitting diode) in conjunction with high-sensitivity spectroscopic measurement techniques such as multi-pass cell based long optical path length absorption spectroscopy, wavelength-modulation enhanced off-axis integrated cavity output spectroscopy, Faraday rotation spectroscopy, incoherent broadband cavity enhanced absorption spectroscopy. The main techniques available for routine atmospheric measurements of OH, NO₃ and HONO are overviewed, in comparison with the emerging modern photonic spectroscopy techniques.     

Diode laser-based sensor for high precision measurements of ambient CO<Subscript>2</Subscript> in network applications

The increasing need for better spatial and temporal measurements of greenhouse gases, especially CO₂, to support global climate change modeling is driving the expansion of monitoring networks. Currently, networks making ambient CO₂ measurements use environmentally stabilized sensors based on non-dispersive infrared absorption spectroscopy. To expand both measurement capability and coverage, much work is underway to develop highly accurate, reliable yet economical sensors for the greenhouse gases. The US Department of Energy has created specifications for a new sensor that has high performance but at a cost that permits widespread deployment. We report on a sensor designed to meet this need. We have demonstrated a compact, automated, high precision sensor for ambient CO₂ that offers good performance in an economical package. The sensor is a near-IR diode laser-based absorption spectrometer operating near 2 μm and using Integrated Cavity Output Spectroscopy (ICOS). Field demonstrations were carried out at both the UNH/AirMap Thompson Farm Observatory and the NOAA Boulder Atmospheric Observatory. The sensor has a demonstrated precision of between 0.090 and 0.125 ppmv for a 30 sec acquisition, or 1 part in 3000 to 4000.     

Emissivity of the main greenhouse gases

Based on the high-resolution data on the absorption lines of gases from the HITRAN open inter-national database in conjunction with inverse Fourier transform, the autocorrelation function of the total dipole moment of the molecules of the main greenhouse gases, such as H₂O, CO₂, O₃, N₂O, and CH₄, are determined. The spectral absorption coefficient and spectral radiance of these gases in the investigated IR region is calculated. An analysis of the emissivity of each of the gases is performed. An efficiency criterion of IR absorption and emission is introduced, according to which the studies gases are ranked.     

Review of proton conductors for hydrogen separation

There is a global push to develop a range of hydrogen technologies for timely adoption of the hydrogen economy. This is critical in view of the depleting oil reserves and looming transport fuel shortage, global warming, and increasing pollution. Molecular hydrogen (H₂) can be generated by a number of renewable and fossil-fuel-based resources. However, given the high cost of H₂ generation by renewable energy at this stage, fossil or carbon fuels are likely to meet the short- to medium-term demand for hydrogen. In view of this, effective technologies are required for the separation of H₂ from a gas feed (by-products of coal or bio-mass gasification plants, or gases from fossil fuel partial oxidation or reforming) consisting mainly of H₂ and CO₂ with small quantities of other gases such as CH₄, CO, H₂O, and traces of sulphur compounds. Several technologies are under development for hydrogen separation. One such technology is based on ion transport membranes, which conduct protons or both protons and electrons. Although these materials have been considered for other applications, such as gas sensors, fuel cells and water electrolysis, the interest in their use as gas separation membranes has developed only recently. In this paper, various classes of proton-conducting materials have been reviewed with specific emphasis on their potential use as H₂ separation membranes in the industrial processes of coal gasification, natural gas reforming, methanol reforming and the water–gas shift (WGS) reaction. Key material requirements for their use in these applications have been discussed.     

FORLI radiative transfer and retrieval code for IASI

This paper lays down the theoretical bases and the methods used in the Fast Optimal Retrievals on Layers for IASI (FORLI) software, which is developed and maintained at the “Université Libre de Bruxelles” (ULB) with the support of the “Laboratoire Atmosphères, Milieux, Observations Spatiales” (LATMOS) to process radiance spectra from the Infrared Atmospheric Sounding Interferometer (IASI) in the perspective of local to global chemistry applications. The forward radiative transfer model (RTM) and the retrieval approaches are formulated and numerical approximations are described. The aim of FORLI is near-real-time provision of global scale concentrations of trace gases from IASI, either integrated over the altitude range of the atmosphere (total columns) or vertically resolved. To this end, FORLI uses precalculated table of absorbances. At the time of writing three gas-specific versions of this algorithm have been set up: FORLI-CO, FORLI-O₃ and FORLI-HNO₃. The performances of each are reviewed and illustrations of results and early validations are provided, making the link to recent scientific publications. In this paper we stress the challenges raised by near-real-time processing of IASI, shortly describe the processing chain set up at ULB and draw perspectives for future developments and applications.     

Tribological development of TiCN coatings by adjusting the flowing rate of reactive gases

TiCN coatings were deposited by means of direct current magnetron sputtering of Ti targets in presence of N₂ and C₂H₂ reactive gases. The microstructure, composition, mechanical and tribological properties of the deposited thin films were analyzed by using X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), nanoindentation, ball-on-disc, scratch test, and three dimensional (3D) optical microscopy. The obtained results presents a reproducible processing route for tailoring microstructure, mechanical and tribological behavior of TiCN coatings by controlling flowing rate of the reactive gases.     

Is the critical Reynolds number universal?

This paper is devoted to checking whether the critical Reynolds number is universal in identical conditions for the flow of different fluids. The laminar-turbulent transition in a circular pipe flow has been tested experimentally. The flows of inert gases (He, Ne, Ar, Kr, Xe), molecular gases (N₂, CO, CO₂, SF₆), and two similar liquids (H₂O, D₂O) have been tested. A considerable, up to 40%, difference in critical Reynolds numbers was observed. The possible reasons for nonuniversality of the critical Reynolds number are discussed.     

Thermochemical nitridation of sapphire substrates of different crystallographic orientations

This paper presents the results of the study of the influence of physicochemical parameters of thermochemical nitridation of sapphire substrates of different crystallographic orientations in an N₂ + (CO,H₂) reducing atmosphere on structural characteristics, composition, and kinetics of AlN layer formation. The effective diffusion coefficients of nitrogen in sapphire at T = 1473?1773 K have been determined. The temperature dependences of the structural quality, thickness, and roughness of the AlN layer surface have been found; their strong dependence on the composition and reduction potential of the nitridation atmosphere has been shown. The structural models of matching the AlN and sapphire lattices during thermochemical nitridation have been proposed.     

Space-borne remote sensing of CO2, CH4, and N2O by integrated path differential absorption lidar: a sensitivity analysis

CO₂, CH₄, and N₂O are recognised as the most important greenhouse gases, the concentrations of which increase rapidly through human activities. Space-borne integrated path differential absorption lidar allows global observations at day and night over land and water surfaces in all climates. In this study we investigate potential sources of measurement errors and compare them with the scientific requirements. Our simulations reveal that moderate-size instruments in terms of telescope aperture (0.5–1.5 m) and laser average power (0.4–4 W) potentially have a low random error of the greenhouse gas column which is 0.2% for CO₂ and 0.4% for CH₄ for soundings at 1.6 μm, 0.4% for CO₂ at 2.1 μm, 0.6% for CH₄ at 2.3 μm, and 0.3% for N₂O at 3.9 μm. Coherent detection instruments are generally limited by speckle noise, while direct detection instruments suffer from high detector noise using current technology. The wavelength selection in the vicinity of the absorption line is critical as it controls the height region of highest sensitivity, the temperature cross-sensitivity, and the demands on frequency stability. For CO₂, an error budget of 0.08% is derived from our analysis of the sources of systematic errors. Among them, the frequency stability of ± 0.3 MHz for the laser transmitter and spectral purity of 99.9% in conjunction with a narrow-band spectral filter of 1 GHz (FWHM) are identified to be challenging instrument requirements for a direct detection CO₂ system operating at 1.6 μm. PACS 42.68.Wt; 95.75.Qr     

Determination of H2S,COS, CS2 and SO2 by an aluminium nitride nanocluster: DFT studies

ABSTRACT

Density functional theory calculations were used to investigate the potential application of an AlN nanocluster in the detection of H₂S, COS, CS₂ and SO₂ gases. In overall, the order of strength of interaction of these gases with the nanocluster is as follows: SO₂ (E_ad?=??17.6?kcal/mol)?>?H₂S (E_ad?=??14.0?kcal/mol)?>?COS (E_ad?=??8.4?kcal/mol)?>?CS₂ (E_ad?=??4.5?kcal/mol). This indicates that by increasing the electric dipole moment, the adsorption energy becomes more negative. We found that the Al₁₂N₁₂ nanocluster may be a promising work function-type sensor for SO₂ gas among the studied gases. Also, it is an electronic sensor for both SO₂ and CS₂ gases but selectively acts between them because of their different effects on the electrical conductivity. It is neither work function-type nor electronic sensor for H₂S and COS gases. The AlN nanocluster benefits from a short recovery time about 7.7?s and 18.0?ms for desorption of SO₂ and CS₂ gases from its surface at room temperature, respectively. It is also concluded that this cluster can work at a humid environment.     

Raman scattering studies of polycrystalline 3C-SiC deposited on SiO2 and AlN thin films

This paper describes the Raman scattering characteristics of the Raman spectra of 0.4- and 2.0-μm-thick polycrystalline (poly) 3C-SiC on AlN /Si and SiO₂/Si by using atmosphere pressure chemical vapor deposition (APCVD) with hexamethyldisilane (HMDS) and carrier gases (Ar+H₂). In the Raman spectra for all growth temperatures, the D and G peaks of nanocrystalline graphite were measured. The C/Si rate of poly 3C-SiC deposited in (Ar+H₂) atmosphere was higher than that in H₂ gas, although HMDS C/Si rate is 3. The biaxial stresses of 2.0-μm-thick 3C-SiC on SiO₂ and AlN, which was deposited at the growth temperature of 1180 °C after annealing AlN at 800 and 1100 °C, were calculated as 428 and 896 MPa, respectively. Therefore, poly 3C-SiC should admix with nanocrystalline graphite due to the addition of Ar gas and poly 3C-SiC on SiO₂ should be better than on AlN for harsh environmental MEMS applications.     

Pulsed laser deposited iron fluoride thin films for lithium-ion batteries

Iron fluoride thin films were successfully grown by Pulsed Laser Deposition (PLD), and their physico-chemical properties and electrochemical behaviours were examined by adjusting the deposition conditions, such as the target nature (FeF₂ or FeF₃), the substrate temperature (T_s ≤ 600 °C), the gas pressure (under vacuum or in oxygen atmosphere) and the repetition rates (2 and 10 Hz). Irrespective of the FeF₂ or FeF₃ target nature, iron fluoride thin films, deposited at 600 °C under vacuum, showed X-ray diffraction (XRD) patterns corresponding to the FeF₂ phase. On the other hand, iron fluoride thin films deposited at room temperature (RT) from FeF₂ target were amorphous, whereas the thin films deposited from FeF₃ target consisted of a two-phase mixture of FeF₃ and FeF₂ showing sharp and broad diffraction peaks by XRD, respectively. Their electrochemical behaviour in rechargeable lithium cells was investigated in the 0.05-3.60 V voltage window. Despite a large irreversible capacity on the first discharge, good cycling life was observed up to 30 cycles. Finally, their electrochemical properties were compared to the ones of iron oxide thin films.     

Self-, N2-, O2-broadening coefficients and line parameters of HFC-32 for ν7 band and ground state transitions from infrared and microwave spectroscopy

Hydrofluorocarbons have been used as replacement gases of chlorofluorocarbons, since the latter have been phased out by the Montreal Protocol due to their environmental hazardous ozone-depleting effects. This is also the case of difluoromethane (CH₂F₂, HFC-32), which nowadays is widely used in refrigerant mixtures together with CF₃CH₃, CF₃CH₂F, and CF₃CHF₂. Due to its commercial use, in the last years, the atmospheric concentration of HFC-32 has increased significantly. However, this molecule presents strong absorptions within the 8–12 μm atmospheric window, and hence it is a greenhouse gas which contributes to global warming. Although over the years several experimental and theoretical investigations dealt with the spectroscopic properties of CH₂F₂, up to now pressure broadening coefficients have never been determined. In the present work, the line-by-line parameters of CH₂F₂ are retrieved for either ground state or ν₇ band transitions by means of microwave (MW) and infrared (IR) absorption spectroscopy, respectively. In particular, laboratory experiments are carried out on 9 pure rotational transitions of the ground state and 26 ro-vibrational transitions belonging to the ν₇ band lying around 8.2 μm within the atmospheric region. Measurements are carried out at room temperature on self-perturbed CH₂F₂ as well as on CH₂F₂ perturbed by N₂ and O₂. The line shape analysis leads to the first determination of self-, N₂-, O₂-, and air-broadening coefficients, and also of line intensities (IR). Upon comparison, broadening coefficients of ground state transitions are larger than those of the ν₇ band, and no clear dependence on the rotational quantum numbers can be reported. The obtained results represent basic information for the atmospheric modelling of this compound as well as for remote sensing applications.