Preparation,characterization, and gas permeation properties of blend membranes of polysulfone and polyethylene glycol inclusive alumina nanoparticles     

T. Tamiji  E. Ameri 《International Journal of Environmental Science and Technology》2017,14(6):1235-1242

The effect of incorporation of alumina nanoparticles on the gas separation properties of the polysulfone–polyethylene glycol blend membranes containing 20% polyethylene glycol was examined. At first, a number of nanocomposite polysulfone–polyethylene glycol/alumina membranes were synthesized with alumina nanoparticles loaded into the polymer matrixes. The hybrid membranes were synthesized with six different alumina contents of 2.5, 5, 10, 15, 20, and 30 wt%. The polysulfone–polyethylene glycol and their hybrids inclusive alumina membranes were prepared via thermal phase-inversion method. The membranes were initially characterized using Fourier transform infrared spectroscopy, scanning electron microscope, and X-ray diffraction. Gas permeation properties of these membranes with different alumina contents were investigated for pure CO₂, CH₄, N₂, and O₂ gases. The results showed that not only these gases permeability but the CO₂/N₂, CO₂/CH₄, and O₂/N₂ ideal selectivity were improved with increasing alumina nanoparticle content of the membrane as well. Also the effect of feed pressure on the permeation properties of these membranes was investigated for pure CO₂ gas. Finally, the results from the synthesized membranes were compared with Robeson’s upper bound line.  相似文献   

Adsorption kinetics of CO2, CH4, and their equimolar mixture on coal from the Black Warrior Basin,West-Central Alabama     

M.S. Gruszkiewicz  M.T. Naney  J.G. Blencoe  D.R. Cole  J.C. Pashin  R.E. Carroll 《International Journal of Coal Geology》2009,77(1-2):23-33

Laboratory experiments were conducted to investigate the adsorption kinetic behavior of pure and mixed gases (CO_2, CH₄, approximately equimolar CO₂ + CH₄ mixtures, and He) on a coal sample obtained from the Black Warrior Basin at the Littleton Mine (Twin Pine Coal Company), Jefferson County, west-central Alabama. The sample was from the Mary Lee coal zone of the Pottsville Formation (Lower Pennsylvanian). Experiments with three size fractions (45–150 µm, 1–2 mm, and 5–10 mm) of crushed coal were performed at 40 °C and 35 °C over a pressure range of 1.4–6.9 MPa to simulate coalbed methane reservoir conditions in the Black Warrior Basin and provide data relevant for enhanced coalbed methane recovery operations. The following key observations were made: (1) CO₂ adsorption on both dry and water-saturated coal is much more rapid than CH₄ adsorption; (2) water saturation decreases the rates of CO₂ and CH₄ adsorption on coal surfaces, but it appears to have minimal effects on the final magnitude of CO₂ or CH₄ adsorption if the coal is not previously exposed to CO₂; (3) retention of adsorbed CO₂ on coal surfaces is significant even with extreme pressure cycling; and (4) adsorption is significantly faster for the 45–150 μm size fraction compared to the two coarser fractions.  相似文献   

Dynamics of greenhouse gases in the river–groundwater interface in a gaining river stretch (Triffoy catchment,Belgium)     

Anna Jurado  Alberto V. Borges  Estanislao Pujades  Pierre Briers  Olha Nikolenko  Alain Dassargues  Serge Brouyère 《Hydrogeology Journal》2018,26(8):2739-2751

This study investigates the occurrence of greenhouse gases (GHGs) and the role of groundwater as an indirect pathway of GHG emissions into surface waters in a gaining stretch of the Triffoy River agricultural catchment (Belgium). To this end, nitrous oxide (N₂O), methane (CH₄) and carbon dioxide (CO₂) concentrations, the stable isotopes of nitrate, and major ions were monitored in river and groundwater over 8 months. Results indicated that groundwater was strongly oversaturated in N₂O and CO₂ with respect to atmospheric equilibrium (50.1 vs. 0.55 μg L^?1 for N₂O and 14,569 vs. 400 ppm for CO₂), but only marginally for CH₄ (0.45 vs. 0.056 μg L^?1), suggesting that groundwater can be a source of these GHGs to the atmosphere. Nitrification seemed to be the main process for the accumulation of N₂O in groundwater. Oxic conditions prevailing in the aquifer were not prone for the accumulation of CH₄. In fact, the emissions of CH₄ from the river were one to two orders of magnitude higher than the inputs from groundwater, meaning that CH₄ emissions from the river were due to CH₄ in-situ production in riverbed or riparian zone sediments. For CO₂ and N₂O, average emissions from groundwater were 1.5?×?10⁵ kg CO₂ ha^?1 year^?1 and 207 kg N₂O ha^?1 year^?1, respectively. Groundwater is probably an important source of N₂O and CO₂ in gaining streams but when the measures are scaled at catchment scale, these fluxes are probably relatively modest. Nevertheless, their quantification would better constrain nitrogen and carbon budgets in natural systems.  相似文献   

Sabatier-based CO2-methanation by catalytic conversion     

K. Müller  M. Städter  F. Rachow  D. Hoffmannbeck  D. Schmeißer 《Environmental Earth Sciences》2013,70(8):3771-3778

The catalytic conversion of CO₂ is an important component for the reintegration of secondary products like CO₂ or H₂ into the energy supply. An example is the “power to gas” concept with a conversion of CO₂ into CH₄. The CO₂ is transferred into a carrier of chemical energy, with the possibility to feed the produced CH₄ into the existing network of natural gas. At temperatures of around 350 °C, hydrogenation of CO₂ to CH₄ is possible by the Sabatier reaction CO₂ + 4H₂ → CH₄ + 2H₂O. One prerequisite for efficient kinetics of the Sabatier reaction is the application and optimization of catalysts. The focus of catalyst development is given to their performance under the conditions to be expected in the special application. As a part of the project Geoenergy-Research (GeoEn), we address questions related to the catalytic utilization of CO₂ produced in the course of the oxyfuel combustion of lignite. In this contribution, we report on the experimental setup in laboratory scale, which enables an advanced characterization of the catalytic performance, including thermodesorption measurements at atmospheric pressure in order to determine the amount of adsorbed CO₂ under real conditions. We also show data for activation energies, the catalytic performance as function of temperature and the long time stability of a commercial Ru-based catalyst.  相似文献   

Stable carbon isotope composition and concentrations of CO₂ and CH₄ in the deep catotelm of a peat bog     

Philipp Steinmann  Bernd Eilrich  Markus Leuenberger 《Geochimica et cosmochimica acta》2008,72(24):6015-6026

Vertical profiles of concentration and C-isotopic composition of dissolved methane and carbon dioxide were observed over 26 months in the catotelm of a deep (6.5 m) peat bog in Switzerland. The dissolved concentrations of these gases increase with depth while CO₂ predominates over CH₄ (CO₂ ca. 5 times CH₄). This pattern can be reproduced by a reaction-advection-ebullition model, where CO₂ and CH₄ are formed in a ratio of 1:1. The less soluble methane is preferentially lost via outgassing (bubbles). The isotopic fractionation between CO₂ and CH₄ also increases with depth, with α_C values ranging from 1.045 to 1.075. The isotopic composition of the gases traces the passage of respiration-derived CO₂ (from the near surface) through a shallow zone with methanogenesis of low isotopic fractionation (splitting of fermentation-derived acetate). This solution then moves through the catotelm, where methanogenesis occurs by CO₂ reduction (large isotopic fractionation). In the upper part of the catotelm the C-13-depleted respiration-derived CO₂ pool buffers the isotopic composition of CO₂; the δ¹³C of CO₂ increases only slowly. At the same time strongly depleted CH₄ is formed as CO₂ reduction consumes the depleted CO₂. In the lower part of the catotelm, the respiration-derived CO₂ and shallow CH₄ become less important and CO₂ reduction is the dominant source of CO₂ and CH₄. Now, the δ¹³C values of both gases increase until equilibrium is reached with respect to the isotopic composition of the substrate. Thus, the δ¹³C values of methane reach a minimum at intermediate depth, and the deep methane has δ¹³C values comparable to shallow methane. A simple mixing model for the isotopic evolution is suggested. Only minor changes of the observed patterns of methanogenesis (in terms of concentration and isotopic composition) occur over the seasons. The most pronounced of these is a slightly higher rate of acetate splitting in spring.  相似文献   

Carbon Dioxide and Methane Emissions from Mangrove-Associated Waters of the Andaman Islands,Bay of Bengal     

Neetha Linto  J. Barnes  Ramesh Ramachandran  Jennifer Divia  Purvaja Ramachandran  R. C. Upstill-Goddard 《Estuaries and Coasts》2014,37(2):381-398

We estimated CO₂ and CH₄ emissions from mangrove-associated waters of the Andaman Islands by sampling hourly over 24 h in two tidal mangrove creeks (Wright Myo; Kalighat) and during transects in contiguous shallow inshore waters, immediately following the northeast monsoons (dry season) and during the peak of the southwest monsoons (wet season) of 2005 and 2006. Tidal height correlated positively with dissolved O₂ and negatively with pCO₂, CH₄, total alkalinity (TAlk) and dissolved inorganic carbon (DIC), and pCO₂ and CH₄ were always highly supersaturated (330–1,627 % CO₂; 339–26,930 % CH₄). These data are consistent with a tidal pumping response to hydrostatic pressure change. There were no seasonal trends in dissolved CH₄ but pCO₂ was around twice as high during the 2005 wet season than at other times, in both the tidal surveys and the inshore transects. Fourfold higher turbidity during the wet season is consistent with elevated net benthic and/or water column heterotrophy via enhanced organic matter inputs from adjacent mangrove forest and/or the flushing of CO₂-enriched soil waters, which may explain these CO₂ data. TAlk/DIC relationships in the tidally pumped waters were most consistent with a diagenetic origin of CO₂ primarily via sulphate reduction, with additional inputs via aerobic respiration. A decrease with salinity for pCO₂, CH₄, TAlk and DIC during the inshore transects reflected offshore transport of tidally pumped waters. Estimated mean tidal creek emissions were ～23–173 mmol m^?2 day^?1 CO₂ and ～0.11–0.47 mmol m^?2 day^?1 CH₄. The CO₂ emissions are typical of mangrove-associated waters globally, while the CH₄ emissions fall at the low end of the published range. Scaling to the creek open water area (2,700 km²) gave total annual creek water emissions ～3.6–9.2?×?10¹⁰ mol CO₂ and 3.7–34?×?10⁷ mol CH₄. We estimated emissions from contiguous inshore waters at ～1.5?×?10¹¹ mol CO₂?year^?1 and 2.6?×?10⁸ mol CH₄?year^?1, giving total emissions of ～1.9?×?10¹¹ mol CO₂?year^?1 and ～3.0?×?10⁸ mol CH₄?year^?1 from a total area of mangrove-influenced water of ～3?×?10⁴ km². Evaluating such emissions in a range of mangrove environments is important to resolving the greenhouse gas balance of mangrove ecosystems globally. Future such studies should be integral to wider quantitative process studies of the mangrove carbon balance.  相似文献   

Enrichment of nitrogen and 13C of methane in natural gases from the Khuff Formation,Saudi Arabia,caused by thermochemical sulfate reduction     

《Organic Geochemistry》2015

Permian Khuff reservoirs along the east coast of Saudi Arabia and in the Arabian Gulf produce dry sour gas with highly variable nitrogen concentrations. Rough correlations between N₂/CH₄, CO₂/CH₄ and H₂S/CH₄ suggest that non-hydrocarbon gas abundances are controlled by thermochemical sulfate reduction (TSR). In Khuff gases judged to be unaltered by TSR, methane δ¹³C generally falls between −40‰ and −35‰ VPDB and carbon dioxide δ¹³C between −3‰ and 0‰ VPDB. As H₂S/CH₄ increases, methane δ¹³C increases to as much as −3‰ and carbon dioxide δ¹³C decreases to as little as −28‰. These changes are interpreted to reflect the oxidation of methane to carbon dioxide.Khuff reservoir temperatures, which locally exceed 150 °C, appear high enough to drive the reduction of sulfate by methane. Anhydrite is abundant in the Khuff and fine grained nodules are commonly rimmed with secondary calcite cement. Some cores contain abundant pyrite, sphalerite and galena. Assuming that nitrogen is inert, loss of methane by TSR should increase N₂/CH₄ of the residual gas and leave δ¹⁵N unaltered. δ¹⁵N of Paleozoic gases in Saudi Arabia varies from −7‰ to 1‰ vs. air and supports the TSR hypothesis. N₂/CH₄ in gases from stacked Khuff reservoirs varies by a factor of 19 yet the variation in δ¹⁵N (0.3–0.5‰) is trivial.Because the relative abundance of hydrogen sulfide is not a fully reliable extent of reaction parameter, we have attempted to assess the extent of TSR using plots of methane δ¹³C versus log(N₂/CH₄). Observed variations in these parameters can be fitted using simple Rayleigh models with kinetic carbon isotope fractionation factors between 0.98 and 0.99. We calculate that TSR may have destroyed more than 90% of the original methane charge in the most extreme instance. The possibility that methane may be completely destroyed by TSR has important implications for deep gas exploration and the origin of gases rich in nitrogen as well as hydrogen sulfide.  相似文献   

Methane and CO₂ sorption and desorption measurements on dry Argonne premium coals: pure components and mixtures     

Andreas Busch  Yves Gensterblum  Bernhard M. Krooss 《International Journal of Coal Geology》2003,55(2-4):205-224

Sorption and desorption behaviour of methane, carbon dioxide, and mixtures of the two gases has been studied on a set of well-characterised coals from the Argonne Premium Coal Programme. The coal samples cover a maturity range from 0.25% to 1.68% vitrinite reflectance. The maceral compositions were dominated by vitrinite (85% to 91%). Inertinite contents ranged from 8% to 11% and liptinite contents around 1% with one exception (Illinois coal, 5%). All sorption experiments were performed on powdered (−100 mesh), dry coal samples.Single component sorption/desorption measurements were carried out at 22 °C up to final pressures around 51 bar (5.1 MPa) for CO₂ (subcritical state) and 110 bar (11 MPa) for methane.The ratios of the final sorption capacities for pure CO₂ and methane (in molar units) on the five coal samples vary between 1.15 and 3.16. The lowest ratio (1.15) was found for the North Dakota Beulah-Zap lignite (VR_r=0.25%) and the highest ratios (2.7 and 3.16) were encountered for the low-rank coals (VR_r 0.32% and 0.48%) while the ratio decreases to 1.6–1.7 for the highest rank coals in this series.Desorption isotherms for CH₄ and CO₂ were measured immediately after the corresponding sorption isotherms. They generally lie above the sorption isotherms. The degree of hysteresis, i.e. deviation of sorption and desorption isotherms, varies and shows no dependence on coal rank.Adsorption tests with CH₄/CO₂ mixtures were conducted to study the degree of preferential sorption of these two gases on coals of different rank. These experiments were performed on dry coals at 45 °C and pressures up to 180 bar (18 MPa). For the highest rank samples of this sequence preferential sorption behaviour was “as expected”, i.e. preferential adsorption of CO₂ and preferential desorption of CH₄ were observed. For the low rank samples, however, preferential adsorption of CH₄ was found in the low pressure range and preferential desorption of CO₂ over the entire pressure range.Follow-up tests for single gas CO₂ sorption measurements consistently showed a significant increase in sorption capacity for re-runs on the same sample. This phenomenon could be due to extraction of volatile coal components by CO₂ in the first experiment. Reproducibility tests with methane and CO₂ using fresh sample material in each experiment did not show this effect.  相似文献   

Displacement behavior of CH4 adsorbed on coals by injecting pure CO2, N2, and CO2–N2 mixture     

Sohei Shimada  Huoyin Li  Yoshito Oshima  Kazuhide Adachi 《Environmental Geology》2005,49(1):44-52

Gas adsorption isotherms of Akabira coals were established for pure carbon dioxide (CO₂), methane (CH₄), and nitrogen (N₂). Experimental data fit well into the Langmuir model. The ratio of sorption capacity of CO₂, CH₄, and N₂ is 8.5:3.5:1 at a lower pressure (1.2 MPa) regime and becomes 5.5:2:1 when gas pressure increases to 6.0 MPa. The difference in sorption capacity of these three gases is explained by differences in the density of the three gases with increasing pressure. A coal–methane system partially saturated with CH₄ at 2.4 MPa adsorption pressure was experimentally studied. Desorption behavior of CH₄ by injecting pure CO₂ (at 3.0, 4.0, 5.0, and 6.0 MPa), and by injecting the CO₂–N₂ mixture and pure N₂ (at 3.0 and 6.0 MPa) were evaluated. Results indicate that the preferential sorption property of coal for CO₂ is significantly higher than that for CH₄ or N₂. CO₂ injection can displace almost all of the CH₄ adsorbed on coal. When modeling the CH₄–CO₂ binary and CH₂–CO₂–N₂ ternary adsorption system by using the extended Langmuir (EL) equation, the EL model always over-predicted the sorbed CO₂ value with a lower error, while under-predicting the sorbed CH₄ with a higher error. A part of CO₂ may dissolve into the solid organic structure of coal, besides its competitive adsorption with other gases. According to this explanation, the EL coefficients of CO₂ in EL equation were revised. The revised EL model proved to be very accurate in predicting sorbed ratio of multi-component gases on coals.  相似文献   

Phase relations and melting of carbonated peridotite between 10 and 20 GPa: a proxy for alkali- and CO<Subscript>2</Subscript>-rich silicate melts in the deep mantle     

Sujoy?GhoshEmail author  Konstantin?Litasov  Eiji?Ohtani 《Contributions to Mineralogy and Petrology》2014,167(2):964

We determined the melting phase relations, melt compositions, and melting reactions of carbonated peridotite on two carbonate-bearing peridotite compositions (ACP: alkali-rich peridotite + 5.0 wt % CO₂ and PERC: fertile peridotite + 2.5 wt % CO₂) at 10–20 GPa and 1,500–2,100 °C and constrain isopleths of the CO₂ contents in the silicate melts in the deep mantle. At 10–20 GPa, near-solidus (ACP: 1,400–1,630 °C) carbonatitic melts with < 10 wt % SiO₂ and > 40 wt % CO₂ gradually change to carbonated silicate melts with > 25 wt % SiO₂ and < 25 wt % CO₂ between 1,480 and 1,670 °C in the presence of residual majorite garnet, olivine/wadsleyite, and clinoenstatite/clinopyroxene. With increasing degrees of melting, the melt composition changes to an alkali- and CO₂-rich silicate melt (Mg# = 83.7–91.6; ~ 26–36 wt % MgO; ~ 24–43 wt % SiO₂; ~ 4–13 wt % CaO; ~ 0.6–3.1 wt % Na₂O; and ~ 0.5–3.2 wt % K₂O; ~ 6.4–38.4 wt % CO₂). The temperature of the first appearance of CO₂-rich silicate melt at 10–20 GPa is ~ 440–470 °C lower than the solidus of volatile-free peridotite. Garnet + wadsleyite + clinoenstatite + carbonatitic melt controls initial carbonated silicate melting at a pressure < 15 GPa, whereas garnet + wadsleyite/ringwoodite + carbonatitic melt dominates at pressure > 15 GPa. Similar to hydrous peridotite, majorite garnet is a liquidus phase in carbonated peridotites (ACP and PERC) at 10–20 GPa. The liquidus is likely to be at ~ 2,050 °C or higher at pressures of the present study, which gives a melting interval of more than 670 °C in carbonated peridotite systems. Alkali-rich carbonated silicate melts may thus be produced through partial melting of carbonated peridotite to 20 GPa at near mantle adiabat or even at plume temperature. These alkali- and CO₂-rich silicate melts can percolate upward and may react with volatile-rich materials accumulate at the top of transition zone near 410-km depth. If these refertilized domains migrate upward and convect out of the zone of metal saturation, CO₂ and H₂O flux melting can take place and kimberlite parental magmas can be generated. These mechanisms might be important for mantle dynamics and are potentially effective metasomatic processes in the deep mantle.  相似文献   

Interaction of peridotite with Ca-rich carbonatite melt at 3.1 and 6.5 GPa: Implication for merwinite formation in upper mantle,and for the metasomatic origin of sublithospheric diamonds with Ca-rich suite of inclusions     

Igor?S.?SharyginEmail authorView author&#;s OrcID profile  Anton?Shatskiy  Konstantin?D.?Litasov  Alexander?V.?Golovin  Eiji?Ohtani  Nikolay?P.?Pokhilenko 《Contributions to Mineralogy and Petrology》2018,173(3):22

We performed an experimental study, designed to reproduce the formation of an unusual merwinite?+?olivine-bearing mantle assemblage recently described as a part of a Ca-rich suite of inclusions in sublithospheric diamonds, through the interaction of peridotite with an alkali-rich Ca-carbonatite melt, derived from deeply subducted oceanic crust. In the first set of experiments, we studied the reaction between powdered Mg-silicates, olivine and orthopyroxene, and a model Ca-carbonate melt (molar Na:K:Ca?=?1:1:2), in a homogeneous mixture, at 3.1 and 6.5 GPa. In these equilibration experiments, we observed the formation of a merwinite?+?olivine-bearing assemblage at 3.1 GPa and 1200 °C and at 6.5 GPa and 1300–1400 °C. The melts coexisting with this assemblage have a low Si and high Ca content (Ca#?=?molar 100?×?Ca/(Ca?+?Mg)?>?0.57). In the second set of experiments, we investigated reaction rims produced by interaction of the same Ca-carbonate melt (molar Na:K:Ca?=?1:1:2) with Mg-silicate, olivine and orthopyroxene, single crystals at 3.1 GPa and 1300 °C and at 6.5 GPa and 1400 °C. The interaction of the Ca-carbonate melt with olivine leads to merwinite formation through the expected reaction: 2Mg₂SiO₄ (olivine)?+?6CaCO₃ (liquid)?=?Ca₃MgSi₂O₈ (merwinite)?+?3CaMg(CO₃)₂ (liquid). Thus, our experiments confirm the idea that merwinite in the upper mantle may originate via interaction of peridotite with Ca-rich carbonatite melt, and that diamonds hosting merwinite may have a metasomatic origin. It is remarkable that the interaction of the Ca-carbonate melt with orthopyroxene crystals does not produce merwinite both at 3.1 and 6.5 GPa. This indicates that olivine grain boundaries are preferable for merwinite formation in the upper mantle.  相似文献   

Selection of coals of different maturities for CO₂ Storage by modelling of CH₄ and CO₂ adsorption isotherms     

Ch. GarnierG. Finqueneisel  T. ZimnyZ. Pokryszka  S. LafortuneP.D.C. Défossez  E.C. Gaucher 《International Journal of Coal Geology》2011,87(2):80-86

CO₂ injection in unmineable coal seams could be one interesting option for both storage and methane recovery processes. The objective of this study is to compare and model pure gas sorption isotherms (CO₂ and CH₄) for well-characterised coals of different maturities to determine the most suitable coal for CO₂ storage. Carbon dioxide and methane adsorption on several coals have been investigated using a gravimetric adsorption method. The experiments were carried out using both CO₂ and CH₄ pure gases at 25 °C from 0.1 to 5 MPa (1 to 50 bar). The experimental results were fitted using Temkin's approach but also with the corrected Langmuir's and the corrected Tóth's equations. The two last approaches are more accurate from a thermodynamical point of view, and have the advantage of taking into account the fact that experimental data (isotherms) correspond to excess adsorption capacities. These approaches allow better quantification of the adsorbed gas. Determined CO₂ adsorption capacities are from 0.5 to 2 mmol/g of dry coal. Modelling provides also the affinity parameters of the two gases for the different coals. We have shown these parameters determined with adsorption models could be used for classification and first selection of coals for CO₂ storage. The affinity ratio ranges from a value close to 1 for immature coals to 41 for high rank coals like anthracites. This ratio allows selecting coals having high CO₂ adsorption capacities. In our case, the modelling study of a significant number of coals from various ranks shows that anthracites seem to have the highest CO₂ storage capacities. Our study provides high quality affinity parameters and values of CO₂ and CH₄ adsorption capacities on various coals for the future modelling of CO₂ injection in coal seams.  相似文献   

Groundwater Discharge as a Source of Dissolved Carbon and Greenhouse Gases in a Subtropical Estuary   总被引：1，自引：0，他引：1  

Mahmood Sadat-Noori  Damien T. Maher  Isaac R. Santos 《Estuaries and Coasts》2016,39(3):639-656

Groundwater may be highly enriched in dissolved carbon species, but its role as a source of carbon to coastal waters is still poorly constrained. Exports of deep and shallow groundwater-derived dissolved carbon species from a small subtropical estuary (Korogoro Creek, Australia, latitude ?31.0478°, longitude 153.0649°) were quantified using a radium isotope mass balance model (²³³Ra and ²²⁴Ra, natural groundwater tracers) under two hydrological conditions. In addition, air-water exchange of carbon dioxide and methane in the estuary was estimated. The highest carbon inputs to the estuary were from deep fresh groundwater in the wet season. Most of the dissolved carbon delivered by groundwater and exported from the estuary to the coastal ocean was in the form of dissolved inorganic carbon (DIC; 687 mmol m^?2 estuary day^?1; 20 mmol m^?2 catchment day^?1, respectively), with a large export of alkalinity (23 mmol m^?2 catchment day^?1). Average water to air flux of CO₂ (869 mmol m^?2 day^?1) and CH₄ (26 mmol m^?2 day^?1) were 5- and 43-fold higher, respectively, than the average global evasion in estuaries due to the large input of CO₂- and CH₄-enriched groundwater. The groundwater discharge contribution to carbon exports from the estuary for DIC, dissolved organic carbon (DOC), alkalinity, CO₂, and CH₄ was 22, 41, 3, 75, and 100 %, respectively. The results show that CO₂ and CH₄ evasion rates from small subtropical estuaries surrounded by wetlands can be extremely high and that groundwater discharge had a major role in carbon export and evasion from the estuary and therefore should be accounted for in coastal carbon budgets.  相似文献   

Assessment of greenhouse gas emissions from coal and natural gas thermal power plants using life cycle approach   总被引：2，自引：1，他引：1  

K. Kr. Agrawal  S. Jain  A. Kr. Jain  S. Dahiya 《International Journal of Environmental Science and Technology》2014,11(4):1157-1164

The importance of mitigation of climate change due to greenhouse gas (GHG) emissions from various developmental and infrastructure projects has generated interest at global level to reduce environmental impacts. Life cycle assessment may be used as a tool to assess GHG emissions and subsequent environmental impacts resulting from electricity generation from thermal power plants. This study uses life cycle approach for assessing GHG emissions and their impacts due to natural gas combined cycle (NGCC) and imported coal thermal power plants using the IPCC 2001 and Eco-Indicator 99(H) methods in India for the first time. The total GHG emission from the NGCC thermal power plant was 584 g CO₂ eq/kWh electricity generation, whereas in case of imported coal, it was 1,127 g CO₂ eq/kWh electricity generation. This shows that imported coal has nearly ~2 times more impacts when compared to natural gas in terms of global warming potential and human health as disability-adjusted life years from climate change due to GHG emissions such as carbon dioxide (CO₂), methane (CH₄) and nitrous oxide (N₂O).  相似文献   

Study of carbon dioxide and methane equilibrium adsorption on silicoaluminophosphate-34 zeotype and T-type zeolite as adsorbent     

M. Salmasi  S. Fatemi  M. Doroudian Rad  F. Jadidi 《International Journal of Environmental Science and Technology》2013,10(5):1067-1074

Carbon dioxide is known as a hazardous material with acidic property that can be found as impurity in natural gas reservoirs with a broad range of 2 up to 40 %. Therefore, many efforts have been directed to remove and separate carbon dioxide from methane to prevent corrosion problems as well as improving the natural gas energy content. In this study, two molecular sieves, silicoaluminophosphate-34 (SAPO-34) zeotype and T-type zeolite, were synthesized by the hydrothermal method for the comparative study of adsorptive separation of carbon dioxide from methane. The synthesized adsorbents were characterized by X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy, and Brunner–Emmett–Teller techniques. These characterization tests confirmed formation of both materials with acceptable crystallinity. Both adsorbents were tested in equilibrium adsorption experiments in order to evaluate maximum capacity and adsorption affinity. Adsorption capacity of carbon dioxide and methane on SAPO-34 and zeolite T were measured in a pressure range of 0.1–2.0 MPa and temperature of 288, 298, and 308 K and fitted with the Sips and Langmuir isotherm models. The ideal selectivity of CO₂/CH₄ was determined for SAPO-34 and zeolite T at the studied pressures and temperatures, indicating that the molecular sieves can be properly used for CO₂–CH₄ separation or CO₂ capturing from natural gas.  相似文献   

Experiments on Methane Displacement by Carbon Dioxide in Large Coal Specimens     

Weiguo Liang  Yangsheng Zhao  Di Wu  Maurice B. Dusseault 《Rock Mechanics and Rock Engineering》2011,44(5):579-589

Carbon dioxide (CO₂) is considered to be the most important greenhouse gas in terms of overall effect. CO₂ geological storage in coal beds is of academic and industrial interest because of economic synergies between greenhouse gas sequestration and coal bed methane (CH₄) recovery by displacement/adsorption. Previously, most work focused on either theoretical analyses and mathematical simulations or gas adsorption?Cdesorption experiments using coal particles of millimeter size or smaller. Those studies provided basic understanding of CH₄ recovery by CO₂ displacement in coal fragments, but more relevant and realistic investigations are still rare. To study the processes more realistically, we conducted experimental CH₄ displacement by CO₂ and CO₂ sequestration with intact 100?×?100?×?200?mm coal specimens. The coal specimen permeability was measured first, and results show that the permeability of the specimen is different for CH₄ and CO₂; the CO₂ permeability was found to be at least two orders of magnitude greater than that for CH₄. Simultaneously, a negative exponential relationship between the permeability and the applied mean stress on the specimen was found. Under the experimental stress conditions, 17.5?C28.0 volumes CO₂ can be stored in one volume of coal, and the displacement ratio CO₂?CCH₄ is as much as 7.0?C13.9. The process of injection, adsorption and desorption, displacement, and output of gases proceeds smoothly under an applied constant pressure differential, and the CH₄ content in the output gas amounted to 20?C50% at early stages, persisting to 10?C16% during the last stage of the experiments. Production rate and CH₄ fraction are governed by complex factors including initial CH₄ content, the pore and fissure fabric of the coal, the changes in this fabric as the result of differential adsorption of CO₂, the applied stress, and so on. During CO₂ injection and CH₄ displacement, the coal can swell from effects of gas adsorption and desorption, leading to changes in the microstructure of the coal itself. Artificial stimulation (e.g. hydraulic fracturing) to improve coalbed transport properties for either CO₂ sequestration or enhanced coal bed methane recovery will be necessary. The interactions of large-scale induced fractures with the fabric at the scale of observable fissures and fractures in the laboratory specimens, as well as to the pore scale processes associated with adsorption and desorption, remain of profound interest and a great challenge.  相似文献   

Variability in Concentrations and Fluxes of Methane in the Indian Estuaries     

G. D. Rao  V. V. S. S. Sarma 《Estuaries and Coasts》2016,39(6):1639-1650

In order to examine the fluxes of methane (CH₄) from the Indian estuaries, measurements were carried out by collecting samples from 26 estuaries along the Indian coast during high discharge (wet) and low water discharge (dry) periods. The CH₄ concentrations in the estuaries located along the west coast of India were significantly higher (113?±?40 nM) compared to the east coast of India (27?±?6 nM) during wet and dry periods (88?±?15 and 63?±?12 nM, respectively). Supersaturation of CH₄ was observed in the Indian estuaries during both periods ((0.18 to 22.3?×?10³ %). The concentrations of CH₄ showed inverse relation with salinity indicating that freshwater is a significant source. Spatial variations in CH₄ saturation were associated with the organic matter load suggesting that its decomposition may be another source in the Indian estuaries. Fluxes of CH₄ ranged from 0.01 to 298 μmol m^?2 day^?1 (mean 13.4?±?5 μmol m^?2 day^?1) which is ~30 times lower compared to European estuaries (414 μmol m^?2 day^?1). The annual emission from Indian estuaries, including Pulicat and Adyar, amounted to 0.39?×?10¹⁰ g CH₄?year^?1 with the surface area of 0.027?×?10⁶ km² which is significantly lower than that in European estuaries (2.7?±?6.8?×?10¹⁰ g CH₄?year^?1 with the surface area of 0.03?×?10⁶ km²). This study suggests that Indian estuaries are a weak source for atmospheric CH₄ than European estuaries and such low fluxes were attributed to low residence time of water and low decomposition of organic matter within the estuary. The CH₄ fluxes from the Indian estuaries are higher than those from Indian mangroves (0.01?×?10¹⁰ g CH₄?year^?1) but lower than those from Indian inland waters (210?×?10¹⁰ g CH₄?year^?1).  相似文献   

Geochemical and isotopic characteristics of fluids in the Niutuozhen geothermal field,North China     

Jumei Pang  Zhonghe Pang  Min Lv  Jiao Tian  Yanlong Kong 《Environmental Earth Sciences》2018,77(1):12

Niutuozhen geothermal field is located in the Jizhong graben, belonging to the northern part of Bohai Bay Basin in North China. Chemical and isotopic analyses were carried out on 14 samples of the geothermal fluids discharged from Neogene Minghuazhen (Nm), Guantao (Ng), and Jixianian Wumishan (Jxw) formations. The δ²H and δ¹⁸O in water, δ¹³C in CH₄, δ¹³C in CO₂, and ³He/⁴He ratio in the gases were analyzed in combination with chemical analyses on the fluids in the Niutuozhen geothermal field. The chemical and isotopic compositions indicate a meteoric origin of the thermal waters. The reservoir temperatures estimated by chemical geothermometry are in the range between 60 and 108 °C. The results show that the gases are made up mainly by N₂ (18.20–97.42 vol%), CH₄ (0.02–60.95 vol%), and CO₂ (0.17–25.14 vol%), with relatively high He composition (up to 0.52 vol%). The chemical and isotopic compositions of the gas samples suggest the meteoric origin of N₂, predominant crustal origins of CH₄, CO₂, and He. The mantle-derived He contributions are calculated to be from 5 to 8% based on a crust–mantle binary mixing model. The deep temperatures in the Jxw reservoir were evaluated based on gas isotope geothermometry to be in the range from 141 to 165 °C. The mantle-derived heat fraction in the surface heat flow is estimated to be in the range of 48–51% based on ³He/⁴He ratios.  相似文献   

Milestones in the evolution of the atmosphere with reference to climate change     

A. Y. Glikson 《Australian Journal of Earth Sciences》2013,60(2):125-139

The history of life on Earth is critically dependent on the carbon, sulfur and oxygen cycles of the lithosphere – hydrosphere – atmosphere – biosphere system. An Archean oxygen-poor greenhouse atmosphere developed through: (i) accumulation of CO₂ and CH₄ from episodic injections of CO₂ from volcanic activity, volatilised crust impacted by asteroids and comets, metamorphic devolatilisation processes and release of methane from sediments; and (ii) little CO₂ weathering-capture due to both high temperatures of the hydrosphere (low CO₂ solubility) and a low ratio of exposed continents to oceans. In the wake of the Sturtian glaciation, enrichment in oxygen and appearance of multicellular eukaryotes heralded the onset of the Phanerozoic where greenhouse conditions were interrupted by periods of strong CO₂-sequestration through intensified capture of CO₂ by marine plants, onset of land plants and burial of carbonaceous shale and coal (Late Ordovician; Carboniferous – Permian; Late Jurassic; Late Tertiary – Quaternary). The progression from Late Mesozoic and Early Tertiary greenhouse conditions to Late Tertiary – Quaternary ice ages was related to the sequestration of CO₂ by rapid weathering of the emerging Alpine and Himalayan mountain chains. A number of peak warming and sea-level-rise events include the Late Oligocene, mid-Miocene, mid-Pliocene and Pleistocene glacial terminations. The Late Tertiary – Quaternary ice ages were dominated by cyclic orbital-forcing-triggered terminations which involved CO₂-feedback effects from warming seas and the biosphere and albedo flips due to ice-sheet melting. Since ca AD 1750 human emissions were ～305 Gt of carbon, as compared with ～750 Gt C in the atmosphere. The emissions constitute ～12% of the terrestrial biosphere and ～10% of the known global fossil fuel reserve of ～4000 Gt C, whose combustion would compare to the ～ 4600 Gt C released to the atmosphere during the K – T impact event 65 million years ago, with associated ～65% mass extinction of species. The current growth rate of atmospheric greenhouse gases and global mean temperatures exceed those of Pleistocene glacial terminations by one to two orders of magnitude. The relationship between temperatures and sea-levels for the last few million years project future sea-level rises toward time-averaged values of at least 5 m per 1°C. The instability of ice sheets suggested by the Dansgaard – Oeschinger glacial cycles during 50 – 20 ka, observed ice melt lag effects of glacial terminations, spring ice collapse dynamics and the doubling per-decade of Greenland and west Antarctic ice melt suggest that the Intergovernmental Panel on Climate Change's projected sea-level rises (<59 cm) for the 21st century may be exceeded. The biological and philosophical rationale underlying climate change and mass extinction perpetrated by an intelligent carbon-emitting mammal species may never be known.  相似文献   

Experimental study of pure and mixtures of CO<Subscript>2</Subscript> and CH<Subscript>4</Subscript> adsorption on modified carbon nanotubes     

E. Molyanyan  S. Aghamiri  M. R. Talaie  N. Iraji 《International Journal of Environmental Science and Technology》2016,13(8):2001-2010

In this work 3-[2-(2-aminoethylamino)ethylamino]propyl trimethoxysilane (TRI) was employed to functionalize MWCNT containing hydroxyl groups (OH-MWCNT), and the XRD, FTIR, TGA and CHNS elemental analysis techniques were used to characterize the resulted adsorbents. The characterization results for amine-MWCNT showed amine groups effectively attached to the surface of the MWCNT. The equilibrium adsorption capacity of pure CO₂ and CH₄ and their binary mixture on the pristine MWCNT, OH-MWCNT and amine-MWCNT was measured through a set of equilibrium adsorption experiments at 303.2 and 318.2 K. Capacities of all three types of adsorbents for CO₂ adsorption were higher than those for methane adsorption. Also, amine-MWCNT demonstrated better performance on CO₂ adsorption than the other two adsorbents, especially at low partial pressures. The capacity of amine-MWCNT for pure CO₂ adsorption was 2.5 and 4 times as much as those for pristine MWCNT and OH-MWCNT, respectively, at the temperature of 303.2 K and the pressure of 0.2 bar. The binary adsorption experiment revealed that CO₂/CH₄ selectivity for pristine MWCNT and amine-MWCNT in all molar fractions of CO₂ is about 1.77 and 7, respectively.  相似文献