首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 875 毫秒
1.
Concentrated, aqueous piperazine (PZ) has been investigated as a novel amine solvent for carbon dioxide (CO2) absorption. The CO2 absorption rate of aqueous PZ is more than double that of 7 m MEA and the amine volatility at 40 °C ranges from 11 to 21 ppm. Thermal degradation is negligible in concentrated, aqueous PZ up to a temperature of 150 °C, a significant advantage over MEA systems. Oxidation of concentrated, aqueous PZ is appreciable in the presence of copper (4 mM), but negligible in the presence of chromium (0.6 mM), nickel (0.25 mM), iron (0.25 mM), and vanadium (0.1 mM). Initial system modeling suggests that 8 m PZ will use 10–20% less energy than 7 m MEA. The fast mass transfer and low degradation rates suggest that concentrated, aqueous PZ has the potential to be a preferred solvent for CO2 capture.  相似文献   

2.
Concentrated, aqueous piperazine (PZ) is a novel solvent for carbon dioxide (CO2) capture by absorption/stripping. One of the major advantages of PZ is its resistance to thermal degradation and oxidation.At 135 and 150 °C, 8 m PZ is up to two orders of magnitude more resistant to thermal degradation than 7 m monoethanolamine (MEA). After 18 weeks at 150 °C, only 6.3% of the initial PZ was degraded, yielding an apparent first order rate constant for amine loss of 6.1 × 10?9 s?1. PZ was the most resistant amine tested, with the other screened amines shown in order of decreasing resistance: 7 m 2-amino-2-methyl-1-propanol, 7 m Diglycolamine®, 7 m N-(2-hydroxyethyl)piperazine, 7 m MEA, 8 m ethylenediamine, and 7 m diethylenetriamine. Thermal resistance allows the use of higher temperatures and pressures in the stripper, potentially leading to overall energy savings.Concentrated PZ solutions demonstrate resistance to oxidation compared to 7 m MEA solutions. Experiments investigating metal-catalyzed oxidation found that PZ solutions were 3–5 times more resistant to oxidation than MEA. Catalysts tested were 1.0 mM iron (II), 4.0–5.0 mM copper (II), and a combination of stainless steel metals (iron (II), nickel (II), and chromium (III)). Inhibitor A reduced PZ degradation catalyzed by iron (II) and copper (II).  相似文献   

3.
The kinetics of the reaction between carbon dioxide (CO2) and mixed solutions of methyldiethanolamine (MDEA) and piperazine (PZ) was investigated experimentally in a laminar jet apparatus. The experimental kinetic data were obtained under no interfacial turbulence and over a temperature range from 313 to 333 K, MDEA/PZ wt% concentration ratios of 27/3, 24/6 and 21/9, and CO2 loadings from 0.0095 to 0.33 mol CO2/mol amine. In addition, a new absorption-rate/kinetics model for the kinetics of the mixed of solvents was developed, which takes into account the coupling between chemical equilibrium, mass transfer, and all possible chemical reactions involved in the CO2 reaction with MDEA/PZ solvent. The partial differential equations of this model were solved by the finite element numerical method (FEM) based on COMSOL software. The obtained experimental kinetics data were used to obtain the kinetic parameters of CO2 absorption into MDEA/PZ solutions. The reaction-rate constant obtained for PZ blended with MDEA was kPZ = 2.572 × 1012 exp(?5211/T). The 2D model for the blended amines MDEA/PZ has revealed the concentration profiles of all the species in both the radial and axial directions of the laminar jet which has enabled a better understanding of the correct sequence in which the reaction steps involved in the reactive absorption of CO2 in aqueous mixed MDEA/PZ solution occur. It also revealed that PZ may be depleted by the time the solvent blend of MDEA/PZ with a loading greater than 0.015 mol/mol amine is exposed to CO2 from the top of the laminar jet absorber.  相似文献   

4.
Use of amines is one of the leading technologies for post-combustion carbon dioxide capture from gas and coal-fired power plants. This study assesses the potential environmental impact of emissions to air that result from use of monoethanol amine (MEA) as an absorption solvent for the capture of carbon dioxide (CO2). Depending on operation conditions and installed reduction technology, emissions of MEA to the air due to solvent volatility losses are expected to be in the range of 0.01–0.8 kg/tonne CO2 captured. Literature data for human and environmental toxicity, together with atmospheric dispersion model calculations, were used to derive maximum tolerable emissions of amines from CO2 capture. To reflect operating conditions with typical and with elevated emissions, we defined a scenario MEA-LOW, with emissions of 40 t/year MEA and 5 t/year diethyl amine (DEYA), and a scenario MEA-HIGH, with emissions of 80 t/year MEA and 15 t/year DEYA. Maximum MEA deposition fluxes would exceed toxicity limits for aquatic organisms by about a factor of 3–7 depending on the scenario. Due to the formation of nitrosamines and nitramines, the estimated emissions of DEYA are close to or exceed safety limits for drinking water and aquatic ecosystems. The “worst case” scenario approach to determine maximum tolerable emissions of MEA and other amines is in particular useful when both expected environmental loads and the toxic effects are associated with high uncertainties.  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.
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   

7.
The carbon dioxide capture and release from aqueous 2,2′-iminodiethanol (DEA) and N-methyl-2,2′-iminodiethanol (MDEA) have been investigated by means of 13C NMR spectroscopy. We have designed two experimental procedures using a gas mixture containing 12% (v/v) CO2 in N2 or air and 0.667 M aqueous solutions of DEA and MDEA. To understand the CO2–amine reaction equilibria, separate experiments of CO2 absorption (at 293, 313 and 333 K) and desorption (at boiling temperature, room pressure) were carried out. The 13C NMR analysis has allowed us to establish: (1) the percentage of CO2 stored in solution as HCO3?, CO32? and DEA carbamate; (2) the formation of DEA carbamate as a function of absorption temperature and time; (3) the slower decomposition of DEA carbamate than that of bicarbonate. In the experiments planned to test the reuse of the regenerated amines, the absorbent solution was continuously circulated in a closed cycle while it was absorbing CO2 in the absorber (set at 293 K) and simultaneously regenerating amine in the desorber (set at 388 K). After the equilibrium has been reached (13 h), the CO2 absorption efficiency is comprised between 84.0% (DEA) and 82.6% (MDEA) and the average amine regeneration efficiency ranges between 69.6% (DEA) and 78.2% (MDEA). Additionally, MDEA is more stable towards thermal degradation than DEA.  相似文献   

8.
While the demand for reduction in CO2 emission is increasing, the cost of the CO2 capture processes remains a limiting factor for large-scale application. Reducing the cost of the capture system by improving the process and the solvent used must have a priority in order to apply this technology in the future. In this paper, a definition of the economic baseline for post-combustion CO2 capture from 600 MWe bituminous coal-fired power plant is described. The baseline capture process is based on 30% (by weight) aqueous solution of monoethanolamine (MEA). A process model has been developed previously using the Aspen Plus simulation programme where the baseline CO2-removal has been chosen to be 90%. The results from the process modelling have provided the required input data to the economic modelling. Depending on the baseline technical and economical results, an economical parameter study for a CO2 capture process based on absorption/desorption with MEA solutions was performed.Major capture cost reductions can be realized by optimizing the lean solvent loading, the amine solvent concentration, as well as the stripper operating pressure. A minimum CO2 avoided cost of € 33 tonne−1 CO2 was found for a lean solvent loading of 0.3 mol CO2/mol MEA, using a 40 wt.% MEA solution and a stripper operating pressure of 210 kPa. At these conditions 3.0 GJ/tonne CO2 of thermal energy was used for the solvent regeneration. This translates to a € 22 MWh−1 increase in the cost of electricity, compared to € 31.4 MWh−1 for the power plant without capture.  相似文献   

9.
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   

10.
This work presents results from a rate-based model of strippers at normal pressure (160 kPa) and vacuum (30 kPa) in Aspen Custom Modeler® (ACM) for the desorption of CO2 from 5 m K+/2.5 m piperazine (PZ). The model solves the material, equilibrium, summation and enthalpy (MESH) equations, the heat and mass transfer rate equations, and computes the reboiler duty and equivalent work for the stripping process. Simulations were performed with IMTP #40 random packing and a temperature approach on the hot side of the cross-exchanger of 5 °C and 10 °C. A “short and fat” stripper requires 7–15% less total equivalent work than a “tall and skinny” one because of the reduced pressure drop. The vacuum and normal pressure strippers require 230 s and 115 s of liquid retention time to get an equivalent work 4% greater than the minimum work. Stripping at 30 kPa was controlled by mass transfer with reaction in the boundary layer and diffusion of reactants and products (88% resistance at the rich end and 71% resistance at the lean end). Stripping at 160 kPa was controlled by mass transfer with equilibrium reactions (84% resistance at the rich end and 74% resistance at the lean end) at 80% flood. The typical predicted energy requirement for stripping and compression to 10 MPa to achieve 90% CO2 removal was 37 kJ/gmol CO2. This is about 25% of the net output of a 500 MW power plant with 90% CO2 removal.  相似文献   

11.
Hilliard completed several thermodynamic models in Aspen Plus® for modeling CO2 removal with amine solvents, including MEA–H2O–CO2. This solvent was selected to make a system model for CO2 removal by absorption/stripping. Both the absorber and the stripper used RateSep? to rigorously calculate mass transfer rates. The accuracy of the new model was assessed using a recent pilot plant run with 35 wt.% (9 m) MEA. Absorber loading and removal were predicted within 6%, and the temperature profile was approached within 5 °C. An average 3.8% difference between measured and calculated values was achieved in the stripper. A three-stage flash configuration which efficiently utilizes solar energy was developed. It reduces energy use by 6% relative to a simple stripper. Intercooling was used to reach 90% removal in the absorber at these optimized conditions.  相似文献   

12.
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   

13.
The carbon dioxide capture potential of amine amino acid salts (AAAS), formed by mixing equinormal amounts of amino acids; e.g. glycine, β-alanine and sarcosine, with an organic base; 3-(methylamino)propylamine (MAPA), was assessed by comparison with monoethanolamine (MEA), and with amino acid salt (AAS) from amino acid neutralized with an inorganic base; potassium hydroxide (KOH). Carbon dioxide absorption and desorption experiments were carried out on the solvent systems at 40 °C and 80 °C respectively. Experimental results showed that amine amino acid salts have similar CO2 absorption properties to MEA of the same concentration. They also showed good signs of stability during the experiments. Amino acid salt from an inorganic base, KOH, showed lower performance in CO2 absorption than the amine amino acid salts (AAAS) mainly due to a lower equilibrium temperature sensitivity. AAAS showed better performance than MEA of same concentration. AAAS from neutralization of sarcosine with MAPA showed the best performance and the performance could be further enhanced when promoted with excess MAPA. The solvent comparison is semi-quantitative since the bubble structure, and thus gas–liquid interfacial area may not be the same for all experiments, however superficial gas velocities were kept constant.  相似文献   

14.
New comprehensive numerically solved 1D and 2D absorption rate/kinetics models have been developed, for the first time, to interpret the experimental kinetic data obtained with a laminar jet apparatus for the absorption of carbon dioxide (CO2) in CO2 loaded mixed solutions of mixed amine system of methyldiethanolamine (MDEA) and monoethanolamine (MEA). Three MDEA/MEA weight ratios ranging from 27/03 to 23/07, over a concentration range of 2.316–1.996 kmol/m3 for MDEA and of 0.490–1.147 kmol/m3 for MEA were studied. The models take into account the coupling between chemical equilibrium, mass transfer, and the chemical kinetics of all possible chemical reactions involved in the CO2 reaction with MDEA/MEA solvent. The partial differential equations of the 1D model were solved by two numerical techniques; the finite difference method (FDM) based on in-house coded Barakat–Clark scheme and the finite element method (FEM) based on COMSOL software. The FEM comprehensive model was then used to solve the set of partial differential equations in the 2D cylindrical coordinate system setting. Both FDM and FEM produced very accurate results for both the 1D and 2D models, which were much better than our previously published simplified model. The reaction rate constant obtained for MEA blended into MDEA at 298–333 K was kMEA = 5.127 × 108 exp(−3373.8/T). In addition, the 2D model, for the first time, has provided the concentration profiles of all the species in both the radial and axial directions of the laminar jet, thereby enabling an understanding of the correct sequence in which the reaction steps involved in the reactive absorption of CO2 in aqueous mixed amines occur.  相似文献   

15.
The present work is a study to evaluate ionic liquids as a potential solvent for post-combustion CO2 capture. In order to enhance the absorption performance of a CO2 capture unit, different ionic liquids have been designed and tested. The main goal was to get a comparison between a reference liquid and selected ionic liquids. As the reference, a solution of 30 w% monoethanolamine (MEA) and water was used. A large range of different pure and diluted ionic liquids was tested with a special screening process to gain general information about the CO2 absorption performance. Based on these results, a 60 w% ionic liquid solution in water was selected and the vapour–liquid equilibrium was measured experimentally between 40 °C and 110 °C. From these curves the enthalpy of absorption for capturing CO2 into the ionic liquid was determined. With these important parameters one is able to calculate the total energy demand for stripping of CO2 from the loaded solvent for comparison of the ionic liquid based solvent with the reference MEA solvent. The energy demand of this 60 w% ionic liquid is slightly lower than that of the reference solution, resulting in possible energy savings between 12 and 16%.  相似文献   

16.
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   

17.
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   

18.
The kinetics of CO2 absorption in unloaded aqueous ammonia solution were measured using a string of discs contactor with the aqueous ammonia concentrations ranging 0.9–5.4 kmol/m3 and temperatures ranging 298.3–321.9 K. The reaction rates strongly increase with the concentration and less strongly with temperature. Both the termolecular and zwitterion models were applied in this study as amine solutions. The parameters for both of the models were interpreted. The kinetic rate constants for CO2 absorption in aqueous ammonia were compared with those for other amines and were found to be around 1/10 that for monoethanolamine. The fitting results for the termolecular mechanism seem more robust than those for the zwitterion mechanism from a statistical perspective.  相似文献   

19.
This work provides the essential information and approaches for integration of carbon dioxide (CO2) capture units into power plants, particularly the supercritical type, so that energy utilization and CO2 emissions can be well managed in the subject power plants. An in-house model, developed at the University of Regina, Canada, was successfully used for simulating a 500 MW supercritical coal-fired power plant with a post-combustion CO2 capture unit. The simulations enabled sensitivity and parametric study of the net efficiency of the power plant, the coal consumption rate, and the amounts of CO2 captured and avoided. The parameters of interest include CO2 capture efficiency, type of coal, flue gas delivery scheme, type of amine used in the capture unit, and steam pressure supplied to the capture unit for solvent regeneration. The results show that the advancement of MEA-based CO2 capture units through uses of blended monoethanolamine–methyldiethanolamine (MEA–MDEA) and split flow configuration can potentially make the integration of power plant and CO2 capture unit less energy intensive. Despite the increase in energy penalty, it may be worth capturing CO2 at a higher efficiency to achieve greater CO2 emissions avoided. The flue gas delivery scheme and the steam pressure drawn from the power plant to the CO2 capture unit should be considered for process integration.  相似文献   

20.
A novel CO2 separation concept is described wherein the enzyme carbonic anhydrase (CA) is used to increase the overall rate of CO2 absorption after which hydrated CO2 reacts with regenerable amine-bearing polyacrylamide buffering beads (PABB). Following saturation of the material's immobilized tertiary amines, CA-bearing carrier water is separated and recycled to the absorption stage while CO2-loaded material is thermally regenerated. Process application of this concept would involve operation of two or more columns in parallel with thermal regeneration with low-pressure steam taking place after the capacity of a column of amine-bearing polymeric material was exceeded. PABB CO2-bearing capacity was evaluated by thermogravimetric analysis (TGA) for beads of three acrylamido buffering monomer ingredient concentrations: 0 mol/kg bead, 0.857 mol/kg bead, and 2 mol/kg bead. TGA results demonstrate that CO2-bearing capacity increases with increasing PABB buffering concentration and that up to 78% of the theoretical CO2-bearing capacity was realized in prepared PABB samples (0.857 mol/kg recipe). The highest observed CO2-bearing capacity of PABB was 1.37 mol of CO2 per kg dry bead. TGA was also used to assess the regenerability of CO2-loaded PABB. Preliminary results suggest that CO2 is partially driven from PABB samples at temperatures as low as 55 °C, with complete regeneration occurring at 100 °C. Other physical characteristics of PABB are discussed. In addition, the effectiveness of bovine carbonic anhydrase for the catalysis of CO2 dissolution is evaluated. Potential benefits and drawbacks of the proposed process are discussed.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号