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1.
A new apparatus employing a modular, mechanically agitated gas-inducing crystallizer is used to demonstrate the capture of CO2 via hydrate crystallization. The crystallizer enhances the contact of hydrate forming gases with water and thus the rate of hydrate crystallization increases. Flue gas (CO2/N2) and fuel gas (CO2/H2) mixtures were used to represent post- and precombustion capture. A comparison between the rates of hydrate formation in different crystallizers is presented by defining a metric called the normalized rate of hydrate formation. The gas uptake and the separation efficiency for the fuel and flue gas mixtures were found to be greater compared to the results obtained in a smaller scale stirred tank reactor (Kumar et al., 2009c, Linga et al., 2008). The gas uptake and CO2 recovery for flue gas mixture in the presence of THF obtained in this work was higher than that reported in the literature with tetra-n-butyl ammonium bromide and tetra-n-butyl ammonium fluoride (Fan et al., 2009, Li et al., 2009). Although hydrate crystallization is able to capture CO2, the power required for mechanical agitation was found to be very significant. If the hydrate process is to be used industrially then hydrate crystallization must be carried out without mechanical agitation.  相似文献   

2.
This study presents a comparison of different concepts for delivering combined heat and power (CHP) to a refinery in Norway. A reference case of producing high pressure steam from natural gas in boilers and electricity in a combined cycle power plant, is compared to a: (1) natural gas fueled CHP without any CO2 capture; (2) hydrogen fueled CHP with hydrogen produced from steam methane reforming (SMR); (3) hydrogen fueled CHP with hydrogen produced from autothermal reforming (ATR); and finally (4) natural gas fueled CHP with postcombustion CO2 removal. The options are compared on the basis of first law efficiency, emissions of CO2 and a simplified cash flow evaluation. Results show that in terms of efficiency the standard natural gas fueled CHP performs better than the reference case as well as the options with carbon capture. The low carbon options in turn offer lower emissions of greenhouse gases while maintaining the same efficiency as the reference case. The cash flow analysis shows that for any option, a certain mix of prices is required to produce a positive cash flow. As expected, the relationship between natural gas price and electricity price affects all options. Also the value of heat and CO2 emissions plays an important role.  相似文献   

3.
Permeability is one of the most important parameters for CO2 injection in coal to enhance coalbed methane recovery. Laboratory characterization of coal permeability provides useful information for in situ permeability behavior of coal seams when adsorbing gases such as CO2 are injected. In this study, a series of experiments have been conducted for coal samples using both non-adsorbing and adsorbing gases at various confining stresses and pore pressures. Our observations have showed that even under controlled stress conditions, coal permeability decreases with respect to pore pressure during the injection of adsorbing gases. In order to find out the causes of permeability decrease for adsorbing gases, a non-adsorbing gas (helium) is used to determine the effective stress coefficient. In these experiments using helium, the impact of gas sorption can be neglected and any permeability reduction is considered as due to the variation in the effective stress, which is controlled by the effective stress coefficient. The results show that the effective stress coefficient is pore pressure dependent and less than unity for the coal samples studied. The permeability reduction from helium experiments is then used to calibrate the subsequent flow-through experiments using adsorbing gases, CH4 and CO2. Through this calibration, the sole effect of sorption-induced strain on permeability change is obtained for these adsorbing gas flow-through experiments. In this paper, experimental results and analyses are reported including how the impact of effective stress coefficient is separated from that of the sorption-induced strain on the evolution of coal permeability.  相似文献   

4.
Given the dominance of power plant emissions of greenhouse gases, and the growing worldwide interest in CO2 capture and storage (CCS) as a potential climate change mitigation option, the expected future cost of power plants with CO2 capture is of significant interest. Reductions in the cost of technologies as a result of learning-by-doing, R&D investments and other factors have been observed over many decades. This study uses historical experience curves as the basis for estimating future cost trends for four types of electric power plants equipped with CO2 capture systems: pulverized coal (PC) and natural gas combined cycle (NGCC) plants with post-combustion CO2 capture; coal-based integrated gasification combined cycle (IGCC) plants with pre-combustion capture; and coal-fired oxyfuel combustion for new PC plants. We first assess the rates of cost reductions achieved by other energy and environmental process technologies in the past. Then, by analogy with leading capture plant designs, we estimate future cost reductions that might be achieved by power plants employing CO2 capture. Effects of uncertainties in key parameters on projected cost reductions also are evaluated via sensitivity analysis.  相似文献   

5.
The deployment of CCS (carbon capture and storage) at industrial scale implies the development of effective monitoring tools. Noble gases are tracers usually proposed to track CO2. This methodology, combined with the geochemistry of carbon isotopes, has been tested on available analogues.At first, gases from natural analogues were sampled in the Colorado Plateau and in the French carbogaseous provinces, in both well-confined and leaking-sites. Second, we performed a 2-years tracing experience on an underground natural gas storage, sampling gas each month during injection and withdrawal periods.In natural analogues, the geochemical fingerprints are dependent on the containment criterion and on the geological context, giving tools to detect a leakage of deep-CO2 toward surface. This study also provides information on the origin of CO2, as well as residence time of fluids within the crust and clues on the physico-chemical processes occurring during the geological story.The study on the industrial analogue demonstrates the feasibility of using noble gases as tracers of CO2. Withdrawn gases follow geochemical trends coherent with mixing processes between injected gas end-members. Physico-chemical processes revealed by the tracing occur at transient state.These two complementary studies proved the interest of geochemical monitoring to survey the CO2 behaviour, and gave information on its use.  相似文献   

6.
A column of silica gel was employed to contact water with flue gas (CO2/N2) mixture to assess if CO2 can be separated by hydrate crystallization. Three different silica gels were used. One with a pore size of 30 nm (particle size 40–75 μm) and two with a pore size of 100 nm and particle sizes of 40–75 and 75–200 μm respectively. The observed trends indicate that larger pores and particle size increase the gas consumption, CO2 recovery, separation factor and water conversion to hydrate. Thus, the gel (gel #3) with the larger particle size and larger pore size was chosen to carry out experiments with concentrated CO2 mixtures and for experiments in the presence of tetrahydrofuran (THF), which itself is a hydrate forming substance. Addition of THF reduces the operating pressure in the crystallizer but it also reduces the gas uptake. Gel #3 was also used in experiments with a fuel gas (CO2/H2) mixture in order to recover CO2 and H2. It was found that the gel column performs as well as a stirred reactor in separating the gas components from both flue gas and fuel gas mixtures. However, the crystallization rate and hydrate yield are considerably enhanced in the former. Finally the need for stirring is eliminated with the gel column which is enormously beneficial economically.  相似文献   

7.
Laboratory studies and a number of field pilots have demonstrated that CO2 injection into coal seams has the potential to enhance coalbed methane (CBM) recovery with the added advantage that most of the injected CO2 can be stored permanently in coal. The concept of storing CO2 in geologic formations as a safe and effective greenhouse gas mitigation option requires public and regulatory acceptance. In this context it is important to develop a good understanding of the reservoir performance, uncertainties and the risks that are associated with geological storage. The paper presented refers to the sources of uncertainty involved in CO2 storage performance assessment in coalbed methane reservoirs and demonstrates their significance using extensive digital well log data representing the Manville coals in Alberta, Canada. The spatial variability of the reservoir properties was captured through geostatistical analysis, and sequential Gaussian simulations of these provided multiple realisations for the reservoir simulator inputs. A number of CO2 injection scenarios with variable matrix swelling coefficients were evaluated using a 2D reservoir model and spatially distributed realisations of total net thickness and permeability.  相似文献   

8.
Laboratory experiments reported in a companion paper were carried out to examine the chromatographic partitioning of impurities contained in a stream of CO2 injected into a deep saline aquifer. The solubility of the impurity gas in the CO2 stream compared to that of CO2, the in situ conditions of pressure, temperature and water salinity, and the concentration of the impurity gas affect the partitioning of the two gases. For CO2 streams containing H2S, numerical simulations reported here have successfully replicated the laboratory results including the breakthrough of CO2 ahead of H2S. Sensitivity analysis performed with the numerical model has shown that flow conditions, controlled by such parameters as medium permeability, pressure gradient, dispersion, gas mobility and flow direction, affect the breakthrough time and separation of the two gases, leading to delayed or earlier breakthrough, and increasing or decreasing the time lag between the breakthrough of the two gases. Vertical bottom-up flow leads to earlier breakthrough, while top-down flow leads to delayed breakthrough. These results are important in establishing monitoring strategies at CO2 storage sites and in evaluating the risks associated with the possible leakage of injected CO2 that contains impurities.  相似文献   

9.
Coalbeds are an attractive geological environment for storage of carbon dioxide (CO2) because CO2 is retained in the coal as an adsorbed phase and the cost of injection can be offset by enhanced coalbed methane (ECBM) production. This paper presents the findings of a CO2 storage feasibility study on coalbeds in the Wyodak-Anderson coal zone of the Powder River Basin, Wyoming, USA, using reservoir characterization and fluid flow simulations. A 3D numerical model of the Big George coal was constructed using geostatistical techniques, with values of cleat and matrix permeability and porosity constrained through history-matching of production data from coalbed methane (CBM) wells in the field area.Following history-matching, several ECBM and CO2 storage scenarios were investigated: shrinkage and swelling of the coal was either allowed or disallowed, a horizontal hydraulic fracture was either placed at the injection well or removed from the model, the number of model layers was varied between 1 and 24, and the permeability and porosity fields were constructed to be either homogeneous or heterogeneous in accordance with geostatistical models of regional variability. All simulations assumed that the injected gas was 100% CO2 and that the coalbed was overlain by an impermeable caprock. Depending on the scenario, the simulations predicted that after 13 years of CO2 injection, the cumulative methane production would be enhanced by a factor of 1.5–5. Including coal matrix shrinkage and swelling in the model predicted swelling near the injection well, which resulted in a slight reduction (10%) in injection rate. However, including a horizontal hydraulic fracture in the model at the base of the injection well helped mitigate the negative effect of swelling on injection rate. It was also found that six model layers were needed to have sufficient resolution in the vertical direction to account for the buoyancy effects between the gas and resident water, and that capturing the heterogeneous nature of the coal permeability and porosity fields predicted lower estimates of the storage capacity of the Wyodak-Anderson coal zone.After noting that gravity and buoyancy were the major driving forces behind gas flow within the Big George coal, several leakage scenarios were also investigated, in an effort to better understand the interplay between diffusion and flow properties on the transport and storage of CO2. The modeling predicted that the upward migration of gas due to the buoyancy effect was faster than the diffusion of CO2 and therefore the gas rapidly rose to the top of the coalbed and migrated into overlying strata when an impermeable caprock was not included in the model.  相似文献   

10.
Coalbed methane is an important resource of energy. Meanwhile CO2 sequestration in coal is a potential management option for greenhouse gas emissions. An attractive aspect to this process is that CO2 is adsorbed to the coal, reducing the risk of CO2 migration to the surface. Another aspect to this is that the injected CO2 could displace adsorbed methane leading to enhanced coalbed methane recovery. Therefore, in order to understand gas migration within the reservoir, mixed-gas adsorption models are required. Moreover, coal reservoir permeability will be significantly affected by adsorption-induced coal swelling during CO2 injection. Coal swelling is directly related to reservoir pressure and gas content which is calculated by adsorption models in reservoir simulation. Various models have been studied to describe the pure- and mixed-gas adsorption on coal. Nevertheless, only the Langmuir and Extended Langmuir models are usually applied in coal reservoir simulations. This paper presents simulation work using several approaches to representing gas adsorption, implemented into the coal seam gas reservoir simulator SIMED II. The adsorption models are the Extended Langmuir model (ELM), the Ideal Adsorbed Solution (IAS) model and the Two-Dimensional Equation of State (2D EOS). The simulations based on one Australian and one American coal sample demonstrated that (1) the Ideal Adsorbed Solution model, in conjunction with Langmuir model as single-component isotherm, shows similar simulation results as the ELM for both coals, with the IAS model representing the experimental adsorption data more accurately than the ELM for one coal and identically with the ELM for the other coal; (2) simulation results using the 2D EOS, however, are significantly different to the ELM or IAS model for both coal samples. The magnitude of the difference is also dependent on coal swelling and the well operating conditions, such as injection pressure.  相似文献   

11.
Enhanced oil recovery (EOR) through CO2 flooding has been practiced on a commercial basis for the last 35 years and continues today at several sites, currently injecting in total over 30 million tons of CO2 annually. This practice is currently exclusively for economic gain, but can potentially contribute to the reduction of emissions of greenhouse gases provided it is implemented on a large scale. Optimal operations in distributing CO2 to CO2-EOR or enhanced gas recovery (EGR) projects (referred to here collectively as CO2-EHR) on a large scale and long time span imply that intermediate storage of CO2 in geological formations may be a key component. Intermediate storage is defined as the storage of CO2 in geological media for a limited time span such that the CO2 can be sufficiently reproduced for later use in CO2-EHR. This paper investigates the technical aspects, key individual parameters and possibilities of intermediate storage of CO2 in geological formations aiming at large scale implementation of carbon dioxide capture and storage (CCS) for deep emission reduction. The main parameters are thus the depth of injection and density, CO2 flow and transport processes, storage mechanisms, reservoir heterogeneity, the presence of impurities, the type of the reservoirs and the duration of intermediate storage. Structural traps with no flow of formation water combined with proper injection planning such as gas-phase injection favour intermediate storage in deep saline aquifers. In depleted oil and gas fields, high permeability, homogeneous reservoirs with structural traps (e.g. anticlinal structures) are good candidates for intermediate CO2 storage. Intuitively, depleted natural gas reservoirs can be potential candidates for intermediate storage of carbon dioxide due to similarity in storage characteristics.  相似文献   

12.
In order to evaluate the risk of hydrate formation in CO2 transport one has to be able to predict the water content in the fluid phase in equilibrium with the CO2-hydrate. A literature review has identified some knowledge gaps, for example, there are no results available at temperatures lower than 243.15 K (?30 °C); and none of the models found in literature predicts the water content with high accuracy. A model based on equality of water fugacity in fluid and hydrate phase is presented here and used for the predictions of water content in equilibrium with hydrates. Although this model gives better accuracy in the overall temperature and pressure ranges of measurements than the models found in the literature, it is not accurate enough to satisfy the requirements of CO2 transport. The simulation results also show that it is possible to form hydrate at low water content, such as xw = 50 vppm, if temperature is low enough. In order to verify the results and improve the model accuracy further, more experimental data in a larger temperature and pressure region are required.  相似文献   

13.
Carbon dioxide is the major greenhouse gas responsible for global warming. Man-made CO2 emissions contribute approximately 63% of greenhouse gases and the cement industry is responsible for approximately 5% of CO2 emissions emitting nearly 900 kg of CO2 per 1000 kg of cement. CO2 from a cement plant was captured and purified to 98% using the monoethanolamine (MEA) based absorption process. The capture cost was $51 per tonne of CO2 captured, representing approximately 90% of total cost. Steam was the main operating cost representing 39% of the total capture cost. Switching from coal to natural gas reduces CO2 emissions by about 18%. At normal load, about 36 MW of waste heat is available for recovery to satisfy the parasitic heat requirements of MEA process; however, it is very difficult to recover.  相似文献   

14.
Landfills and old waste deposits are some of the major anthropogenic sources of methane (CH4) emissions worldwide. Despite the fact that during the last 15 years the amount of carbon dioxide equivalent (CO2-eq.) emitted from German landfills was reduced by approximately two thirds, estimates show that currently more than 10 Mtonnes are still being emitted annually. As a case study, the in situ aerated former Kuhstedt Landfill (District of Rotenburg (Wümme), Germany) was assessed regarding the possibility of reducing the emitted amounts of greenhouse gases (GHG; here methane). The assessment was based on both a model calculation of the landfill gas emissions that should occur under anaerobic conditions (reference scenario) as well as using monitoring data plus extrapolations to determine the actual emissions from the landfill. It was demonstrated that more than 72% of the total GHG emissions occurring under anaerobic conditions could be avoided by altering the ambient aerobic/oxidizing conditions. By means of subsequent thermal treatment (regenerative thermal oxidation, RTO) of the extracted off-gases during the aeration process, the amount of CO2-eq. savings, as calculated from the amount of emitted methane taking into account secondary emissions for energy production, could be further increased to 96%.  相似文献   

15.
A series of laboratory experiments were carried out to examine the chromatographic partitioning of impurities contained in a stream of CO2 injected into a deep saline aquifer. The experiments were carried out under static (no flow) and dynamic conditions, mainly with H2S as the impurity in the CO2 stream, for 2%, 5% and 30% concentrations, and for in situ conditions of high pressure, temperature and water salinity, and also for pure water at a lower pressure and temperature. In addition, experiments were conducted using CH4, N2 and SO2 at 5% concentration as the ‘Impurity’ in the CO2 stream. The experiments show that gases in an impure stream of CO2 being injected into a deep saline aquifer will chromatographically partition at the leading edge of the gas advancing through the water-saturated porous medium as a result of differential solubility in aquifer water. The solubility of the impurity gas in the CO2 stream compared to that of CO2 is the most dominant factor in regard to the breakthrough time and initial gas concentrations in the effluent. The in situ conditions of pressure, temperature and water salinity also affect the chromatographic partitioning of CO2 and impurities contained in the injection stream through their general effect on the solubility of all gases. The concentration of the impurity gas in the feed gas stream has a secondary effect on the breakthrough and time lag decreasing with increasing concentration of the impurity gas. These experimental findings are significant for understanding the fate of the injected CO2 and associated impurities contained in an injection stream, in devising monitoring procedures and protocols, and in developing emergency response plans in case of leakage of CO2 and associated impurities.  相似文献   

16.
Due to its compatibility with the current energy infrastructures and the potential to reduce CO2 emissions significantly, CO2 capture and geological storage is recognised as one of the main options in the portfolio of greenhouse gas mitigation technologies being developed worldwide. The CO2 capture technologies offer a number of alternatives, which involve different energy consumption rates and subsequent environmental impacts. While the main objective of this technology is to minimise the atmospheric greenhouse gas emissions, it is also important to ensure that CO2 capture and storage does not aggravate other environmental concerns. This requires a holistic and system-wide environmental assessment rather than focusing on the greenhouse gases only. Life Cycle Assessment meets this criteria as it not only tracks energy and non-energy-related greenhouse gas releases but also tracks various other environmental releases, such as solid wastes, toxic substances and common air pollutants, as well as the consumption of other resources, such as water, minerals and land use. This paper presents the principles of the CO2 capture and storage LCA model developed at Imperial College and uses the pulverised coal post-combustion capture example to demonstrate the methodology in detail. At first, the LCA models developed for the coal combustion system and the chemical absorption CO2 capture system are presented together with examples of relevant model applications. Next, the two models are applied to a plant with post-combustion CO2 capture, in order to compare the life cycle environmental performance of systems with and without CO2 capture. The LCA results for the alternative post-combustion CO2 capture methods (including MEA, K+/PZ, and KS-1) have shown that, compared to plants without capture, the alternative CO2 capture methods can achieve approximately 80% reduction in global warming potential without a significant increase in other life cycle impact categories. The results have also shown that, of all the solvent options modelled, KS-1 performed the best in most impact categories.  相似文献   

17.
A 3D numerical model for gas–solid flow was developed and used to study the sorption enhanced steam methane reforming (SE-SMR) and the sorbent regeneration processes with CaO based sorbent in fluidized bed reactors. The SE-SMR process (i.e., SMR and adsorption of CO2) was carried out in a bubbling fluidized bed. The effects of pressure and steam-to-carbon ratio on the reactions are studied. High pressure and low steam-to-carbon ratio will decrease the conversion of methane. But the high pressure makes the adsorption of CO2 faster. The methane conversion and heat utility are enhanced by CO2 adsorption. The produced CO2 in SMR process is adsorbed almost totally in a relative long period of time in the bubbling fluidized bed. It means that the adsorption rate of CO2 is fast enough compared with the SMR rate. The process of sorbent regeneration was carried out in a riser. An unfeasible residence time is required to complete the regeneration process. Higher temperature makes the release of CO2 faster, but the rate is severely restrained by the increased CO2 concentration in gas phase. The temperature distribution is uniform over the whole reactor. Regeneration rate and capacity of sorbents are important factors in selecting the type of reactors for SE-SMR process.  相似文献   

18.
The behavior of natural carbon dioxide (CO2) droplets (8–10 mm in diameter) were observed in a seafloor hydrothermal system at the Okinawa Trough. The natural CO2 droplet contain 95–98% of CO2, 2–3% of H2S, and other gas species. The ascending CO2 droplets were tracked by a remotely operated vehicle (ROV), and depth, temperature, salinity, pH and partial pressure of CO2 (pCO2) in seawater near the CO2 droplets were measured during droplet ascent by a conductivity-temperature-depth sensor (CTD) and in situ pH/pCO2 sensor. The visual images of the rising CO2 droplets were recorded with a high definition television camera on the ROV. A mapping survey (400 m × 400 m; 4 horizontal layers) revealed a dominant distribution of low pH area over the natural CO2 venting site. The size and rise rate of CO2 droplets decreased during their ascent in the water column from depths of 1424 to 679 m (a tracking interval of 745 m). The CO2 droplets dissolved gradually to become small flakes of CO2 hydrate while rising, and these ascending flakes were found to disappear at 679 m depth. Although a pH as low as 5 was detected just above the liquid CO2 venting site on the seafloor, no detectable pH depression in the water column ambient to the rising CO2 droplets was observed. The results of the pH mapping survey showed only localized pH depression over the CO2 venting site.  相似文献   

19.
The objective of this study was to assess the radiative forcing due to Finnish anthropogenic greenhouse gas emissions in three scenarios. All the Kyoto Protocol gases, i.e., CO2, CH4, N2O, and fluorinated gases, were included. The calculations showed that forcing due to Finnish emissions will increase in the case of all gases except methane by the year 2100. In 1990, radiative forcing due to Finland's emission history of all Kyoto Protocol gases was 3.2 mW/m2, of which 71% was due to carbon dioxide, 17% to methane, and the rest to nitrous oxide. In 1990 the share of fluorinated gases was negligible. The share of methane in radiative forcing is decreasing, whereas the shares of carbon dioxide and of fluorinated gases are increasing and that of nitrous oxide remains nearly constant. The nonlinear features concerning additional concentrations in the atmosphere and radiative forcing due to emissions caused by a single country or activity are also considered. Radiative forcing due to Finnish emissions was assessed with two different approaches, the marginal forcing approach and the averaged forcing approach. The impact of the so-called background scenario, i.e., the scenario for concentration caused by global emissions, was also estimated. The difference between different forcing models at its highest was 40%, and the averaged forcing approach appeared to be the more recommendable. The effect of background concentrations in the studied cases was up to 11%. Hence, the choice of forcing model and background scenario should be given particular attention.  相似文献   

20.
Simple models for permeability and selectivity variations of the CO2/CH4 system in 6FDA-2,6-DAT membrane have been derived that include both temperature and pressure effects simultaneously in a single equation. The proposed models were used in MATLAB, for a membrane-based CO2-removal process design for natural gas sweetening. The effects of the following factors on design parameters were examined: feed temperature, feed pressure and permeate pressure. The effect of permeate pressure was found to be very significant in the optimization process. In order to reduce hydrocarbon losses to below 2%, a two-stage membrane process was modeled and simulated in MATLAB, and the extent of desired hydrocarbon recovery was shown to be crucial in the optimization process. It has also been shown that there exist minima for the total required area of the two-stage membrane-based process, and as the CO2 load increases in the feed, the position of these minima shift to higher values of methane loss.  相似文献   

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