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1.
Studies of the kinetics of sulfur dioxide (SO2)- and oxygen (O2)-induced degradation of aqueous monoethanolamine (MEA) during the absorption of carbon dioxide (CO2) from flue gases derived from coal- or natural gas-fired power plants were conducted as a function of temperature and the liquid phase concentrations of MEA, O2, SO2 and CO2. The kinetic data were based on the initial rate which shows the propensity for amine degradation and obtained under a range of conditions typical of the CO2 absorption process (3–7 kmol/m3 MEA, 6% O2, 0–196 ppm SO2, 0–0.55 CO2 loading, and 328–393 K temperature). The results showed that an increase in temperature and the concentrations of MEA, O2 and SO2 resulted in a higher MEA degradation rate. An increase in CO2 concentration gave the opposite effect. A semi-empirical model based on the initial rate, ?rMEA = {6.74 × 109 e?(29,403/RT)[MEA]0.02([O]2.91 + [SO2]3.52)}/{1 + 1.18[CO2]0.18} was developed to fit the experimental data. With the higher order of reaction, SO2 has a higher propensity to cause MEA to degrade than O2. Unlike previous models, this model shows an improvement in that any of the parameters (i.e. O2, SO2, and CO2) can be removed without affecting the usability of the model.  相似文献   

2.
Basic research on the corrosive effect of flue gases has been performed at the BAM Federal Institute for Materials Research and Testing (Germany). Conditions at both high and low temperatures were simulated in specially designed experiments. Carburization occured in flue gases with high CO2 content and temperatures higher than 500 °C. In SO2 containing flue gases sulphur was detected in the oxide scale. At lower temperatures no corrosion was observed when gases with low humidity were investigated. Humidity higher than 1500 ppm was corrosive and all steels with Cr contents lower than 12% revealed corroded surfaces. At low temperatures below 10 °C a mixture of sulphuric and nitric acid condensed on metal surfaces. Acid condensation caused severe corrosion. Humidity, CO2, O2, and SO2 contents are the important factors determining corrosion. Below 300 °C acid condensation is the primary reason for corrosion. Low humidity and low temperatures are conditions which can be expected in the CO2 separation and treatment process. This work includes major conditions of the flue gas and CO2 stream in CCS plants and CCS technology.  相似文献   

3.
Methodology is presented for a first-order regional-scale estimation of CO2 storage capacity in coals under sub-critical conditions, which is subsequently applied to Cretaceous-Tertiary coal beds in Alberta, Canada. Regions suitable for CO2 storage have been defined on the basis of groundwater depth and CO2 phase at in situ conditions. The theoretical CO2 storage capacity was estimated on the basis of CO2 adsorption isotherms measured on coal samples, and it varies between ∼20 kt CO2/km2 and 1260 kt CO2/km2, for a total of approximately 20 Gt CO2. This represents the theoretical storage capacity limit that would be attained if there would be no other gases present in the coals or they would be 100% replaced by CO2, and if all the coals will be accessed by CO2. A recovery factor of less than 100% and a completion factor less than 50% reduce the theoretical storage capacity to an effective storage capacity of only 6.4 Gt CO2. Not all the effective CO2 storage capacity will be utilized because it is uneconomic to build the necessary infrastructure for areas with low storage capacity per unit surface. Assuming that the economic threshold to develop the necessary infrastructure is 200 kt CO2/km2, then the CO2 storage capacity in coal beds in Alberta is greatly reduced further to a practical capacity of only ∼800 Mt CO2.  相似文献   

4.
The purpose of this article is to study the energy and carbon dioxide intensities of Thailand's steel industry and to propose greenhouse gas emission trends from the year 2011 to 2050 under plausible scenarios. The amount of CO2 emission from iron and steel production was calculated using the 2006 Intergovernmental Panel on Climate Change (IPCC) guidelines in the boundary of production process (gate to gate). The results showed that energy intensity of semi-finished steel product was 2.84 GJ/t semi-finished steel and CO2 intensity was 0.37 tCO2eq/t semi-finished steel. Energy intensity of steel finishing process was 1.86 GJ/t finished steel and CO2 intensity was 0.16 tCO2eq/t finished steel. Using three plausible scenarios from Thailand's steel industry, S1: without integrated steel plant (baseline scenario), S2: with a traditional integrated BF–BOF route and S3: with an alternative integrated DR-EAF route; the Greenhouse Gas emissions from the year 2011 to 2050 were projected. In 2050, the CO2 emission from S1 (baseline scenario) was 4.84 million tonnes, S2 was 21.96 million tonnes increasing 4.54 times from baseline scenario. The CO2 emission from S3 was 7.12 million tonnes increasing 1.47 times from baseline scenario.  相似文献   

5.
The capture of CO2 from a hot stove gas in steel making process containing 30 vol% CO2 by chemical absorption in a rotating packed bed (RPB) was studied. The RPB had an inner diameter of 7.6 cm, an outer diameter of 16 cm, and a height of 2 cm. The aqueous solutions containing 30 wt% of single and mixed monoethanolamine (MEA), 2-(2-aminoethylamino)ethanol (AEEA), and piperazine (PZ) were used. The CO2 capture efficiency was found to increase with increasing temperature in a range of 303–333 K. It was also found to be more dependent on gas and liquid flow rates but less dependent on rotating speed when the speed was higher than 700 rpm. The obtained results indicated that the mixed alkanolamine solutions containing PZ were more effective than the single alkanolamine solutions. This was attributed to the highest reaction rate of PZ with CO2. A higher portion of PZ in the mixture was more favorable to CO2 capture. The highest gas flow rates allowed to achieve a desired CO2 capture efficiency and the correspondent height of transfer unit (HTU) were determined at different aqueous solution flow rates. Because all the 30 wt% single and mixed alkanolamine solutions could result in a HTU less than 5.0 cm at a liquid flow rate of 100 mL/min, chemical absorption in a RPB instead of a packed bed adsorber is therefore suggested to capture CO2 from the flue gases in steel making processes.  相似文献   

6.
A reaction calorimeter was used to determine the enthalpies of absorption of CO2 in aqueous ammonia and in aqueous solutions of ammonium carbonate at temperatures of 35–80 °C. The heat of absorption of CO2 with 2.5 wt% aqueous ammonia solution was found to be about 70 kJ/mol CO2, which is lower than that with MEA (around 85 kJ/mol) at 35 and 40 °C. The value decreases with increased loading, but not to as low a value as expected by the carbonate–bicarbonate reaction (26.88 kJ/mol). The enthalpy of absorption of CO2 in aqueous ammonia at 60 and 80 °C decreases with loadings at first, then increases between 0.2 mol CO2/mol NH3 and 0.6 mol CO2/mol NH3, and then decreases again. The behavior of the heat of absorption of CO2 in 10 wt% ammonium carbonate solution was found to be the same as that of aqueous ammonia at loadings above 0.6 mol CO2/mol NH3. The heat of absorption increases with increasing temperature. The heats of absorption are directly related to the extent of the various reactions with CO2 and can be assessed from the species variation in the liquid phase.  相似文献   

7.
The effect of impregnation of activated carbon with Cr2O and Fe2O3 and promotion by Zn2+ on its adsorptive properties of carbon dioxide was studied using a volumetric adsorption apparatus at ambient temperature and low pressures. Slurry and solution impregnation methods were used to compare CO2 capture capacity of the impregnated activated carbon promoted by Zinc. The obtained adsorption isotherms showed that amount of CO2 adsorbed on the samples impregnated by Cr2O was increased about 20% in compare to raw activated carbon. The results also showed that Fe2O3 was not an effective impregnating species for activated carbon modification. Moreover slurry impregnation method showed higher CO2 adsorption capacity in comparison with solution impregnation method. Samples prepared by co-impregnation of two metal species showed more adsorption capacity than samples impregnated by just one metal species individually. Washing the impregnated samples by metal oxide resulted in 15% increase in CO2 adsorption capacities of activated carbons which can be attributed to the metal oxides removal covering the adsorption surface. Decreasing impregnation temperature from 95 to 25 °C in solution method showed a significant increase in CO2 adsorption capacity. Sips equation was found a suitable model fitting to the adsorption data in the range studied.  相似文献   

8.
We sketch four possible pathways how carbon dioxide capture and storage (CCS) (r)evolution may occur in the Netherlands, after which the implications in terms of CO2 stored and avoided, costs and infrastructural requirements are quantified. CCS may play a significant role in decarbonising the Dutch energy and industrial sector, which currently emits nearly 100 Mt CO2/year. We found that 15 Mt CO2 could be avoided annually by 2020, provided some of the larger gas fields that become available the coming decade could be used for CO2 storage. Halfway this century, the mitigation potential of CCS in the power sector, industry and transport fuel production is estimated at maximally 80–110 Mt CO2/year, of which 60–80 Mt CO2/year may be avoided at costs between 15 and 40 €/t CO2, including transport and storage. Avoiding 30–60 Mt CO2/year by means of CCS is considered realistic given the storage potential represented by Dutch gas fields, although it requires planning to assure that domestic storage capacity could be used for CO2 storage. In an aggressive climate policy, avoiding another 50 Mt CO2/year may be possible provided that nearly all capture opportunities that occur are taken. Storing such large amounts of CO2 would only be possible if the Groningen gas field or large reservoirs in the British or Norwegian part of the North Sea will become available.  相似文献   

9.
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   

10.
In order to develop subsurface CO2 storage as a viable engineered mechanism to reduce the emission of CO2 into the atmosphere, any potential leakage of injected supercritical CO2 (SC-CO2) from the deep subsurface to the atmosphere must be reduced. Here, we investigate the utility of biofilms, which are microorganism assemblages firmly attached to a surface, as a means of reducing the permeability of deep subsurface porous geological matrices under high pressure and in the presence of SC-CO2, using a unique high pressure (8.9 MPa), moderate temperature (32 °C) flow reactor containing 40 millidarcy Berea sandstone cores. The flow reactor containing the sandstone core was inoculated with the biofilm forming organism Shewanella fridgidimarina. Electron microscopy of the rock core revealed substantial biofilm growth and accumulation under high-pressure conditions in the rock pore space which caused >95% reduction in core permeability. Permeability increased only slightly in response to SC-CO2 challenges of up to 71 h and starvation for up to 363 h in length. Viable population assays of microorganisms in the effluent indicated survival of the cells following SC-CO2 challenges and starvation, although S. fridgidimarina was succeeded by Bacillus mojavensis and Citrobacter sp. which were native in the core. These observations suggest that engineered biofilm barriers may be used to enhance the geologic sequestration of atmospheric CO2.  相似文献   

11.
In this work several Li4SiO4-based sorbents from fly ashes for CO2 capture at high temperatures have been developed. Three fly ash samples were collected and subjected to calcination at 950 °C in the presence of Li2CO3. Both pure Li4SiO4 and fly ash-based sorbents were characterised and tested for CO2 sorption at different temperatures between 400 and 650 °C and adding different amounts of K2CO3 (0–40 mol%). To examine the sorbents performance, multiple CO2 sorption/desorption cycles were carried out. The temperature and the presence of K2CO3 strongly affect the CO2 sorption capacity for the sorbents prepared from fly ashes. When the sorption temperature increases by up to 600 °C both the CO2 sorption capacity and the sorption rate increase significantly. Moreover when the amount of K2CO3 increases, the CO2 sorption capacity also increases. At optimal experimental conditions (600 °C and 40 mol% K2CO3), the maximum CO2 sorption capacity for the sorbent derived from fly ash was 107 mg CO2/g sorbent. The Li4SiO4-based sorbents can maintain its original capacity during 10 cycle processes and reach the plateau of maximum capture capacity in less than 15 min, while pure Li4SiO4 presents a continual upward tendency for the 15 min of the capture step and attains no equilibrium capacity.  相似文献   

12.
Using a combination of experimental (petrophysical and mineralogical) methods, the effects of high-pressure CO2 exposure on fluid transport properties and mineralogical composition of two pelitic caprocks, a limestone and a clay-rich marl lithotype have been studied. Single and multiphase permeability tests, gas breakthrough and diffusion experiments were conducted under in situ p/T conditions on cylindrical plugs (28.5 mm diameter, 10–20 mm thickness).The capillary CO2 sealing efficiency of the initially water-saturated sample plugs was found to decrease in repetitive gas breakthrough experiments on the same sample from 0.74 to 0.41 MPa for the limestone and from 0.64 to 0.43 MPa for the marl. Helium breakthrough experiments before and after the CO2 tests showed a decrease in capillary threshold (snap-off) pressure from 1.81 to 0.62 MPa for the limestone.Repetitive CO2 diffusion experiments on the marlstone revealed an increase in the effective diffusion coefficient from 7.8 × 10?11 to 1.2 × 10?10 m2.Single-phase (water) permeability coefficients derived from steady-state permeability tests ranged between 7 and 56 nano-Darcy and showed a consistent increase after each CO2 test cycle. Effective gas permeabilities were generally one order of magnitude lower than water permeabilities and exhibit the same trend. XRD measurements performed before and after exposure to CO2 did not reveal any distinct change in the mineral composition for both samples. Similarly, no significant changes were observed in specific surface areas (determined by BET) and pore-size distributions (determined by mercury injection porosimetry). High-pressure CO2 sorption experiments on powdered samples revealed significant CO2 sorption capacities of 0.27 and 0.14 mmol/g for the marlstone and the limestone, respectively.The changes in transport parameters in the absence of detectable mineral alterations may be explained by carbonate dissolution and further precipitation along a pH profile across the sample plug which would not be subject to quantitative mineral alteration.  相似文献   

13.
The feasibility of the sorption enhanced water gas shift (SEWGS) process under sour conditions is shown. The sour-SEWGS process constitutes a second generation pre-combustion carbon capture technology for the application in an IGCC. As a first critical step, the suitability of a K2CO3 promoted hydrotalcite-based CO2 sorbent is demonstrated by means of adsorption and regeneration experiments in the presence of 2000 ppm H2S. In multiple cycle experiments at 400 °C and 5 bar, the sorbent displays reversible co-adsorption of CO2 and H2S. The CO2 sorption capacity is not significantly affected compared to sulphur-free conditions. A mechanistic model assuming two different sites for H2S interaction explains qualitatively the interactions of CO2 and H2S with the sorbent. On the type A sites, CO2 and H2S display competitive sorption where CO2 is favoured. The type B sites only allow H2S uptake and may involve the formation of metal sulphides. This material behaviour means that the sour-SEWGS process likely eliminates CO2 and H2S simultaneously from the syngas and that an almost CO2 and H2S-free H2 stream and a CO2 + H2S stream can be produced.  相似文献   

14.
Ash deposition is still an unresolved problem when retrofitting existing air-fired coal power plants to oxy-fuel combustion. Experimental data are quite necessary for mechanism validation and model development. This work was designed to obtain laboratory combustor data on ash and deposits from oxy-coal combustion, and to explore the effects of oxy-firing on their formation. Two bituminous coals (Utah coal and Illinois coal) and one sub-bituminous coal (PRB coal) were burned on a down-fired combustor under both oxy- and air-firing. Two oxy-fired cases, i.e., 27 vol% O2/73 vol% CO2 and 32 vol% O2/68 vol% CO2, were selected to match the radiation flux and the adiabatic flame temperature of air combustion, respectively. Once-through CO2 was used to simulate fully cleaned recycled flue gas. The flue gas excess oxygen was fixed at 3 vol%. For each case, both size-segregated fly ash and bulk fly ash samples were obtained. Simultaneously, ash deposits were collected on an especially designed un-cooled deposition probe. Ash particle size distributions and chemical composition of all samples were characterized. Data showed that oxy-firing had insignificant impacts on the tri-modal ash particle size distributions and composition size distributions in the size range studied. Bulk ash compositions also showed no significant differences between oxy- and air-firing, except for slightly higher sulfur contents in some oxy-fired ashes. The oxy-fired deposits were thicker than those from air-firing, suggesting enhanced ash deposition rates in oxy-firing. Oxy-firing also had apparent impacts on the deposit composition, especially for those components (e.g., CaO, Fe2O3, SO3, etc.) that could contribute significantly to ash deposition. Based on these results, aerodynamic changes in gas flow and changes in combustion temperature seemed more important than chemical changes of ash particles in determining deposit behavior during oxy-coal combustion.  相似文献   

15.
Capture and storage of CO2 from fossil fuel fired power plants is drawing increasing interest as a potential method for the control of greenhouse gas emissions. An optimization and technical parameter study for a CO2 capture process from flue gas of a 600 MWe bituminous coal fired power plant, based on absorption/desorption process with MEA solutions, using ASPEN Plus with the RADFRAC subroutine, was performed. This optimization aimed to reduce the energy requirement for solvent regeneration, by investigating the effects of CO2 removal percentage, MEA concentration, lean solvent loading, stripper operating pressure and lean solvent temperature.Major energy savings can be realized by optimizing the lean solvent loading, the amine solvent concentration as well as the stripper operating pressure. A minimum thermal energy requirement was found at a lean MEA loading of 0.3, using a 40 wt.% MEA solution and a stripper operating pressure of 210 kPa, resulting in a thermal energy requirement of 3.0 GJ/ton CO2, which is 23% lower than the base case of 3.9 GJ/ton CO2. Although the solvent process conditions might not be realisable for MEA due to constraints imposed by corrosion and solvent degradation, the results show that a parametric study will point towards possibilities for process optimisation.  相似文献   

16.
The oxyfuel process is one of the most promising options to capture CO2 from coal fired power plants. The combustion takes place in an atmosphere of almost pure oxygen, delivered from an air separation unit (ASU), and recirculated flue gas. This provides a flue gas containing 80–90 vol% CO2 on a dry basis. Impurities are caused by the purity of the oxygen from the ASU, the combustion process and air ingress. Via liquefaction a CO2 stream with purity in the range from 85 to 99.5 vol% can be separated and stored geologically. Impurities like O2, NOX, SOX, and CO may negatively influence the transport infrastructure or the geological storage site by causing geochemical reactions. Therefore the maximum acceptable concentrations of the impurities in the separated CO2 stream must be defined regarding the requirements from transportation and storage. The main objective of the research project COORAL therefore is to define the required CO2 purity for capture and storage.  相似文献   

17.
Fe2O3-containing waste materials from the steel industry are proposed as oxygen carrier for chemical-looping combustion. Three such materials, red iron oxide, brown iron oxide and iron oxide scales, have been examined by oxidation and reduction experiments in a batch fluidized-bed reactor at temperatures between 800 and 950 °C. NiO-based particles have been used as additive, in order to examine if it is possible to utilize the catalytic properties of metallic Ni to facilitate decomposition of hydrocarbons into more reactive combustion intermediates such as CO and H2. The experiments indicated modest reactivity between the waste materials and CH4, which was used as reducing gas. Adding small amounts of NiO-based particles to the sample increased the yield of CO2 in a standard experiment, typically by a factor of 1.5–3.5. The fraction of unconverted fuel typically was reduced by 70–90%. The conversion of CH4 to CO2 was 94% at best, corresponding to a combustion efficiency of 96%. This was achieved using a bed mass corresponding to 57 kg oxygen carrier per MW fuel, of which only 5 wt% was NiO-based synthetic particles. The different materials fared differently well during the experiments. Red iron oxide was fairly stable, while brown iron oxide was soft and subject to considerable erosion. Iron oxide scales experienced increased reactivity and porosity as function of the numbers of reduction cycles.  相似文献   

18.
Industrial Combined Heat and Power plants (CHPs) are often operated at partial load conditions. If CO2 is captured from a CHP, additional energy requirements can be fully or partly met by increasing the load. Load increase improves plant efficiency and, consequently, part of the additional energy consumption would be offset. If this advantage is large enough, industrial CHPs may become an attractive option for CO2 capture and storage CCS. We therefore investigated the techno-economic performance of post-combustion CO2 capture from small-to-medium-scale (50–200 MWe maximum electrical capacity) industrial Natural Gas Combined Cycle- (NGCC-) CHPs in comparison with large-scale (400 MWe) NGCCs in the short term (2010) and the mid-term future (2020–2025). The analyzed system encompasses NGCC, CO2 capture, compression, and branch CO2 pipeline.The technical results showed that CO2 capture energy requirement for industrial NGCC-CHPs is significantly lower than that for 400 MWe NGCCs: up to 16% in the short term and up to 12% in the mid-term future. The economic results showed that at low heat-to-power ratio operations, CO2 capture from industrial NGCC-CHPs at 100 MWe in the short term (41–44 €/tCO2 avoided) and 200 MWe in the mid-term future (33–36 €/tCO2 avoided) may compete with 400 MWe NGCCs (46–50 €/tCO2 avoided short term, 30–35 €/tCO2 avoided mid-term).  相似文献   

19.
The objective of this study is to investigate the potential process for the removal of carbon dioxide (CO2) from flue gas using fundamental membrane contactor, which is a membrane gas absorption (MGA) system. The experiments consisted of microporous polyvinylidenefluoride (PVDF) flat sheet membrane with 0.1 μm (as module I) and 0.45 μm (as module II) pore size. 2-Amino-2-methyl-1-propanol (AMP) solution was employed as the liquid absorbent. The effect of AMP concentration was studied with variation in the range 1–5 M. In addition, the experiments were carried out with 10%, 20%, 30% and 40% gas ratio of CO2 to N2 and pure CO2 as well. Through contact angle measurement, membranes for module I and module II were obtained with CA values of around 130.25° and 127.77°, respectively. The mass transfer coefficients for module II are lower than those of module I for 1–5 M of AMP. Furthermore, the increase in CO2 concentration in the feed gas stream enhanced the CO2 flux as the driving force of the system was increased in sequence from 1 M to 5 M of AMP. However, after the particular percentage (40%) of CO2 inlet concentration, the CO2 fluxes seem saturated. The combination of AMP as liquid absorbent and PVDF microporous membrane in MGA system has shown the potential to remove the CO2 from flue gas. In addition, the higher AMP concentration gave higher mass transfer coefficient at low liquid flow rates.  相似文献   

20.
This paper explores the integration and evaluation of a power plant with a CaO-based CO2 capture system. There is a great amount of recoverable heat in the CaO-based CO2 capture process. Five cases for the possible integration of a 600 MW power plant with CaO-based CO2 capture process are considered in this paper. When the system is configured so that recovered heat is used to replace part of the boiler heat load (Case 2), modelling not only shows that this is the system recovering the most heat of 1008.8 MW but also results in the system with the lowest net power output of 446 MW and the second lowest of efficiency of 34.1%. It is indicated that system performance depends both on the amount of heat recovery and the type of heat utilization. When the system is configured so that a 400 MW power plant is built using the recovered heat (Case 4), modelling shows that this is the system with the most net power output of 846 MW, the highest efficiency of 36.8%, the lowest cost of electricity of 54.3 €/MWh and the lowest cost of CO2 avoided of 28.9 €/tCO2. This new built steam cycle will not affect the operation of the reference plant which vents its CO2 to the atmosphere, highly reducing the connection between the CO2 capture process and the reference plant which vents its CO2 to the atmosphere. The average cost of electricity and the cost of CO2 avoided of the five cases are about 58.9 €/kWh and 35.9 €/tCO2, respectively.  相似文献   

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