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1.
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   

2.
The carbon molecular sieves (CMSs) prepared by carbonaceous materials as precursors are effective in CO2/N2 separation. However, selectivity of these materials is too low, since hydrocarbon cracking for developing the desired microporosity in carbonaceous materials has not been done effectively. Hence, in this study, cobalt and nickel impregnation on the precursor was conducted to introduce catalysts for hydrocarbon cracking. Cobalt and nickel impregnation, carbonization under N2 atmosphere, and chemical vapor deposition (CVD) by benzene were conducted on the extruded mixtures of activated carbon and coal tar pitch under different conditions to prepare CMSs. The best CMS prepared by carbon deposition on the cobalt-impregnated samples exhibited CO2 adsorption capacity of 54.79 mg/g and uptake ratio of 28.9 at 0 °C and 1 bar. In terms of CO2 adsorption capacity and uptake ratio, CMSs prepared by carbon deposition on non-impregnated and cobalt-impregnated samples presented the best results, respectively. As benzene concentration and CVD time increased, equilibrium adsorption capacity of CO2 decreased, and uptake ratio increased. Cobalt was found to be the best catalyst for benzene cracking in the CVD process.  相似文献   

3.
In this work, rice husk ash was used as silica source to synthesize NaX zeolite potentially suitable for CO2 adsorption. The produced material, denoted NaX-RHA, was characterized employing X-ray diffraction, scanning electron microscopy and gas adsorption porosimetry, in order to verify the occurred production of well-crystallized NaX zeolite with a significant degree of purity. CO2 adsorption isotherms on NaX-RHA were volumetrically evaluated in the 298–348 K temperature range up to standard pressure, revealing performances that are higher than those reported for commercial similar substrates. The experimental data regarding CO2 adsorption on NaX-RHA were very satisfyingly fitted by the semiempirical Sips model. Analyzing the best fitting values of model parameters allowed to conclude that the synthesized adsorbent could be quite suitable for applications like CO2 capture from flue gas.  相似文献   

4.
Amine post-combustion carbon capture technology is based on washing the flue gas with a solvent that captures CO2. Thus, a small fraction of this solvent can be released together with the cleaned flue gas. This release may cause environmental concerns, both directly and indirectly through subsequent solvent degradation into other substances in the atmosphere. The paper presents the ammonia emission from CO2 capture pilot plant (1 tonne CO2 per day) using 40 wt% aminoethylethanolamine solvent, along with the efficiency of the water wash unit. In addition, the temperature effect of lean amine entering the absorber on ammonia emission was studied. Furthermore, the concentrations of other compounds such as SO2, SO3, NO2, CS2 and formaldehyde were monitored. The literature review on the NH3 emission from a pilot plant using aminoethylethanolamine solvent has not been published. The results show that the main source of ammonia emission is the absorber and that emission (in the range 27–50 ppm) corresponds to typical NH3 release from CO2 capture pilot plant using an amine solvent. The emission of amines and amine degradation products is a complex phenomenon which is difficult to predict in novel solvents, and for this reason the significance of new solvents testing in a pilot scale has been highlighted.  相似文献   

5.
Geologic storage of CO2 is expected to produce plumes of large areal extent, and some leakage may occur along fractures, fault zones, or improperly plugged pre-existing wellbores. A review of physical and chemical processes accompanying leakage suggests a potential for self-enhancement. The numerical simulations presented here confirm this expectation, but reveal self-limiting features as well. It seems unlikely that CO2 leakage could trigger a high-energy run-away discharge, a so-called “pneumatic eruption,” but present understanding is insufficient to rule out this possibility. The most promising avenue for increasing understanding of CO2 leakage behavior is the study of natural analogues.  相似文献   

6.
The efficiency and sustainability of carbon dioxide (CO2) storage in deep geological formations crucially depends on the integrity of the overlying cap-rocks. Existing oil and gas wells, which penetrate the formations, are potential leakage pathways. This problem has been discussed in the literature, and a number of investigations using semi-analytical mathematical approaches have been carried out by other authors to quantify leakage rates. The semi-analytical results are based on a number of simplifying assumptions. Thus, it is of great interest to assess the influence of these assumptions. We use a numerical model to compare the results with those of the semi-analytical model. Then we ease the simplifying restrictions and include more complex thermodynamic processes including sub- and supercritical fluid properties of CO2 and non-isothermal as well as compositional effects. The aim is to set up problem-oriented benchmark examples that allow a comparison of different modeling approaches to the problem of CO2 leakage.  相似文献   

7.
Careful site characterization is critical for successful geologic storage of carbon dioxide (CO2) because of the many physical and chemical processes impacting CO2 movement and containment under field conditions. Traditional site characterization techniques such as geological mapping, geophysical imaging, well logging, core analyses, and hydraulic well testing provide the basis for judging whether or not a site is suitable for CO2 storage. However, only through the injection and monitoring of CO2 itself can the coupling between buoyancy flow, geologic heterogeneity, and history-dependent multi-phase flow effects be observed and quantified. CO2 injection and monitoring can therefore provide a valuable addition to the site-characterization process. Additionally, careful monitoring and verification of CO2 plume development during the early stages of commercial operation should be performed to assess storage potential and demonstrate permanence. The Frio brine pilot, a research project located in Dayton, Texas (USA) is used as a case study to illustrate the concept of an iterative sequence in which traditional site characterization is used to prepare for CO2 injection and then CO2 injection itself is used to further site-characterization efforts, constrain geologic storage potential, and validate understanding of geochemical and hydrological processes. At the Frio brine pilot, in addition to traditional site-characterization techniques, CO2 movement in the subsurface is monitored by sampling fluid at an observation well, running CO2-saturation-sensitive well logs periodically in both injection and observation wells, imaging with crosswell seismic in the plane between the injection and observation wells, and obtaining vertical seismic profiles to monitor the CO2 plume as it migrates beyond the immediate vicinity of the wells. Numerical modeling plays a central role in integrating geological, geophysical, and hydrological field observations.  相似文献   

8.
The CO2 migrated from deeper to shallower layers may change its phase state from supercritical state to gaseous state (called phase transition). This phase transition makes both viscosity and density of CO2 experience a sharp variation, which may induce the CO2 further penetration into shallow layers. This is a critical and dangerous situation for the security of CO2 geological storage. However, the assessment of caprock sealing efficiency with a fully coupled multi-physical model is still missing on this phase transition effect. This study extends our previous fully coupled multi-physical model to include this phase transition effect. The dramatic changes of CO2 viscosity and density are incorporated into the model. The impacts of temperature and pressure on caprock sealing efficiency (expressed by CO2 penetration depth) are then numerically investigated for a caprock layer at the depth of 800 m. The changes of CO2 physical properties with gas partial pressure and formation temperature in the phase transition zone are explored. It is observed that phase transition revises the linear relationship of CO2 penetration depth and time square root as well as penetration depth. The real physical properties of CO2 in the phase transition zone are critical to the safety of CO2 sequestration. Pressure and temperature have different impact mechanisms on the security of CO2 geological storage.  相似文献   

9.
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   

10.
One of the uncertainties in the field of carbon dioxide capture and storage (CCS) is caused by the parameterization of geochemical models. The application of geochemical models contributes significantly to calculate the fate of the CO2 after its injection. The choice of the thermodynamic database used, the selection of the secondary mineral assemblage as well as the option to calculate pressure dependent equilibrium constants influence the CO2 trapping potential and trapping mechanism. Scenario analyses were conducted applying a geochemical batch equilibrium model for a virtual CO2 injection into a saline Keuper aquifer. The amount of CO2 which could be trapped in the formation water and in the form of carbonates was calculated using the model code PHREEQC. Thereby, four thermodynamic datasets were used to calculate the thermodynamic equilibria. Furthermore, the equilibrium constants were re-calculated with the code SUPCRT92, which also applied a pressure correction to the equilibrium constants. Varying the thermodynamic database caused a range of 61% in the amount of trapped CO2 calculated. Simultaneously, the assemblage of secondary minerals was varied, and the potential secondary minerals dawsonite and K-mica were included in several scenarios. The selection of the secondary mineral assemblage caused a range of 74% in the calculated amount of trapped CO2. Correcting the equilibrium constants with respect to a pressure of 125 bars had an influence of 11% on the amount of trapped CO2. This illustrates the need for incorporating sensitivity analyses into reaction pathway modeling.  相似文献   

11.
Modeling geological carbon storage represents a new and substantial challenge for the subsurface geosciences. To increase understanding and make good engineering decisions, containment processes and large-scale storage operations must be simulated in a thousand-year perspective. Large differences in spatial and temporal scales make it prohibitively expensive to compute the fate of injected CO2 using traditional 3D simulators. Instead, accurate forecast can be computed using simplified models that are adapted to the specific setting of the bouyancy-driven migration of the light fluid phase. This paper presents a family of vertically integrated models for studying the combined large-scale and long-term effects of structural, residual, and solubility trapping of CO2. The models are based on an assumption of a sharp interface separating CO2 and brine and can provide a detailed inventory of the injected CO2 volumes over periods of thousands of years within reasonable computational time. To be compatible with simulation tools used in industry, the models are formulated in a black-oil framework. The models are implemented in MRST-co2lab, which is an open community software developed especially to study and optimize large-scale, long-term geological storage of CO2. The resulting simulators are fully implicit and handle input from standard geomodeling tools.  相似文献   

12.
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13.
The present analysis adjusts previous estimates of global ocean CaCO3 production rates substantially upward, to 133 × 1012 mol yr?1 plankton production and 42 × 1012 mol yr?1 shelf benthos production. The plankton adjustment is consistent with recent satellite-based estimates; the benthos adjustment includes primarily an upward adjustment of CaCO3 production on so-called carbonate-poor sedimentary shelves and secondarily pays greater attention to high CaCO3 mass (calcimass) and turnover of shelf communities on temperate and polar shelves. Estimated CaCO3 sediment accumulation rates remain about the same as they have been for some years: ~20 × 1012 mol yr?1 on shelves and 11 × 1012 mol yr?1 in the deep ocean. The differences between production and accumulation of calcareous materials call for dissolution of ~22 × 1012 mol yr?1 (~50 %) of shelf benthonic carbonate production and 122 × 1012 mol yr?1 (>90 %) of planktonic production. Most CaCO3 production, whether planktonic or benthonic, is assumed to take place in water depths of <100 m, while most dissolution is assumed to occur below this depth. The molar ratio of CO2 release to CaCO3 precipitation (CO2↑/CaCO3↓) is <1.0 and varies with depth. This ratio, Ψ, is presently about 0.66 in surface seawater and 0.85 in ocean waters deeper than about 1000 m. The net flux of CO2 associated with CaCO3 reactions in the global ocean in late preindustrial time is estimated to be an apparent influx from the atmosphere to the ocean, of +7 × 1012 mol C yr?1, at a time scale of 102–103 years. The CaCO3-mediated influx of CO2 is approximately offset by CO2 release from organic C oxidation in the water column. Continuing ocean acidification will have effects on CaCO3 and organic C metabolic responses to the oceanic inorganic C cycle, although those responses remain poorly quantified.  相似文献   

14.
This study assesses the ability of two low-cost adsorbents made from waste of Rapanea ferruginea treated with ethanol (WRf) and its H2SO4-treated analog (WRf/H2SO4) for the removal of two cationic dyes methylene blue (MB) and crystal violet (CV) from aqueous solutions. The adsorbent was characterized by scanning electron microscopy, Fourier transform infrared spectrometry, thermogravimetric analysis, point of zero charge (pHpzc), specific surface, and functional groups. The adsorption of dye onto the adsorbents was studied as a function of pH solution (2–12), contact time (up to 120 min) and initial concentration (20–120 mg/L), and temperature (25, 35, and 55 °C). The influence of these parameters on adsorption capacity was studied using the batch process. The response surface methodology (RSM) was used in the experimental design, modeling of the process, and optimizing of the variables and was optimized by the response involving Box–Behnken factorial design (15 runs). The results show that the data correlated well with the Sips isotherm. The maximum adsorption capacities of MB and CV onto WRf were found to be 69 and 106 mg/g, and onto WRf/H2SO4, the adsorption capacities were 33 and 125 mg/g, respectively. The kinetic data revealed that adsorption of cationic dyes onto the adsorbents closely follows the pseudo-second-order kinetic model. Regression analysis showed good fit of the experimental data to the second-order polynomial model, with coefficient of determination (R2) values for MB (R2?=?0.9685) and MB (R2?=?0.9832) for WRf and CV (R2?=?0.9685) and CV (R2?=?0.9832) for WRf/H2SO4 indicated that regression analysis is able to give a good prediction of response for the adsorption process in the range studied. The results revealed that waste from R. ferruginea is potentially an efficient and low-cost adsorbent for adsorption of MB and CV.  相似文献   

15.
CO2 geological storage is a transitional technology for the mitigation of climate change. In the vicinity of potential CO2 reservoirs in Hungary, protected freshwater aquifers used for drinking water supplies exist. Effects of disaster events of CO2 escape and brine displacement to one of these aquifers have been studied by kinetic 1D reactive transport modelling in PHREEQC. Besides verifying that ion concentrations in the freshwater may increase up to drinking water limit values in both scenarios (CO2 or brine leakage), total porosity of the rock is estimated. Pore volume is expected to increase at the entry point of CO2 and to decrease at further distances, whereas it shows minor increase along the flow path for the effect of brine inflow. Additionally, electrical conductivity of water is estimated and suggested to be the best parameter to measure for cost-effective monitoring of both worst-case leakage scenarios.  相似文献   

16.
Miller field of the North Sea has had high concentrations of natural CO2 for ~70 Ma. It is an ideal analog for the long-term fate of CO2 during engineered storage, particularly for formation of carbonate minerals that permanently lock up CO2 in solid form. The Brae Formation reservoir sandstone contains an unusually high quantity of calcite concretions; however, C and O stable isotopic signatures suggest that these are not related to the present-day CO2 charge. Margins of the concretions are corroded, probably because of reduced pH due to CO2 influx. Dispersed calcite cements are also present, some of which postdate the CO2 charge and, therefore, are the products of mineral trapping. It is calculated that only a minority of the reservoired CO2 in Miller (6–24%) has been sequestrated in carbonates, even after 70 Ma of CO2 emplacement. Most of the CO2 accumulation is dissolved in pore fluids. Therefore, in a reservoir similar to the Brae Formation, engineered CO2 storage must rely on physical retention mechanisms because mineral trapping is both incomplete and slow.  相似文献   

17.
Documenting geographic distribution and spatial linkages between CO2 sources and potential sinks in areas with significant levels of CO2 emissions is important when considering carbon-management strategies such as geologic sequestration or enhanced oil recovery (EOR). For example, the US Gulf Coast overlies a thick succession (>6,000 m [>20,000 ft]) of highly porous and permeable sandstone formations separated by thick, regionally extensive shale aquitards. The Gulf Coast and Permian Basin also have a large potential for EOR, in which CO2 injected into suitable oil reservoirs could be followed by long-term storage of CO2 in nonproductive formations below reservoir intervals. For example, >6 billion barrels (Bbbl) of oil from 182 large reservoirs is technically recoverable in the Permian Basin as a result of miscible-CO2 flooding. The Gulf Coast also contains an additional 4.5 Bbbl of oil that could be produced by using miscible CO2. Although the CO2 pipeline infrastructure is well-developed in the Permian Basin, east Texas and the Texas Gulf Coast may have a greater long-term potential for deep, permanent storage of CO2 because of thick brine-bearing formations near both major subsurface and point sources of CO2.  相似文献   

18.
A field facility located in Bozeman, Montana provides the opportunity to test methods to detect, locate, and quantify potential CO2 leakage from geologic storage sites. From 9 July to 7 August 2008, 0.3 t CO2 day−1 were injected from a 100-m long, ~2.5-m deep horizontal well. Repeated measurements of soil CO2 fluxes on a grid characterized the spatio-temporal evolution of the surface leakage signal and quantified the surface leakage rate. Infrared CO2 concentration sensors installed in the soil at 30 cm depth at 0–10 m from the well and at 4 cm above the ground at 0 and 5 m from the well recorded surface breakthrough of CO2 leakage and migration of CO2 leakage through the soil. Temporal variations in CO2 concentrations were correlated with atmospheric and soil temperature, wind speed, atmospheric pressure, rainfall, and CO2 injection rate.  相似文献   

19.
Capture and geological sequestration of CO2 from energy production is proposed to help mitigate climate change caused by anthropogenic emissions of CO2 and other greenhouse gases. Performance goals set by the US Department of Energy for CO2 storage permanence include retention of at least 99% of injected CO2 which requires detailed assessments of each potential storage site’s geologic system, including reservoir(s) and seal(s). The objective of this study was to review relevant basin-wide physical and chemical characteristics of geological seals considered for saline reservoir CO2 sequestration in the United States. Results showed that the seal strata can exhibit substantial heterogeneity in the composition, structural, and fluid transport characteristics on a basin scale. Analysis of available field and wellbore core data reveal several common inter-basin features of the seals, including the occurrence of quartz, dolomite, illite, calcite, and glauconite minerals along with structural features containing fractures, faults, and salt structures. In certain localities within the examined basins, some seal strata also serve as source rock for oil and gas production and can be subject to salt intrusions. The regional features identified in this study can help guide modeling, laboratory, and field studies needed to assess local seal performances within the examined basins.  相似文献   

20.
Geological storage of CO2 in the offshore Gippsland Basin, Australia, is being investigated by the Cooperative Research Centre for Greenhouse Gas Technologies (CO2CRC) as a possible method for storing the very large volumes of CO2 emissions from the nearby Latrobe Valley area. A storage capacity of about 50 million tonnes of CO2 per annum for a 40-year injection period is required, which will necessitate several individual storage sites to be used both sequentially and simultaneously, but timed such that existing hydrocarbon assets will not be compromised. Detailed characterisation focussed on the Kingfish Field area as the first site to be potentially used, in the anticipation that this oil field will be depleted within the period 2015–2025. The potential injection targets are the interbedded sandstones of the Paleocene-Eocene upper Latrobe Group, regionally sealed by the Lakes Entrance Formation. The research identified several features to the offshore Gippsland Basin that make it particularly favourable for CO2 storage. These include: a complex stratigraphic architecture that provides baffles which slow vertical migration and increase residual gas trapping and dissolution; non-reactive reservoir units that have high injectivity; a thin, suitably reactive, lower permeability marginal reservoir just below the regional seal providing mineral trapping; several depleted oil fields that provide storage capacity coupled with a transient production-induced flow regime that enhances containment; and long migration pathways beneath a competent regional seal. This study has shown that the Gippsland Basin has sufficient capacity to store very large volumes of CO2. It may provide a solution to the problem of substantially reducing greenhouse gas emissions from future coal developments in the Latrobe Valley.  相似文献   

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