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1.
Significant differences exist in the flue gas composition in hot recycle Oxyfuel conditions as e.g. the high CO2 partial pressure (>90 vol%, dry), the very high SO2 concentration and the high water content (approx. 30 vol%). Therefore certain design and operation criteria have to be observed for the flue gas desulphurization with forced oxidation under Oxyfuel combustion conditions. Several performance tests have been executed at the 30 MWth Oxyfuel pilot plant in Schwarze Pumpe to evaluate the main performance parameters and to assess the influence of the major operation parameters. The results show that there are no fundamental problems for the operation of the flue gas desulphurization unit under Oxyfuel combustion conditions. High removal rates could be reached and no negative impact of the high CO2 partial pressure was observed under the tested operating conditions. No major differences in the gypsum quality have been observed between air firing and Oxyfuel conditions.  相似文献   

2.
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   

3.
Post-combustion CO2 capture and storage (CCS) presents a promising strategy to capture, compress, transport and store CO2 from a high volume–low pressure flue gas stream emitted from a fossil fuel-fired power plant. This work undertakes the simulation of CO2 capture and compression integration into an 800 MWe supercritical coal-fired power plant using chemical process simulators. The focus is not only on the simulation of full load of flue gas stream into the CO2 capture and compression, but also, on the impact of a partial load. The result reveals that the energy penalty of a low capture efficiency, for example, at 50% capture efficiency with 10% flue gas load is higher than for 90% flue gas load at the equivalent capture efficiency by about 440 kWhe/tonne CO2. The study also addresses the effect of CO2 capture performance by different coal ranks. It is found that lignite pulverized coal (PC)-fired power plant has a higher energy requirement than subbituminous and bituminous PC-fired power plants by 40.1 and 98.6 MWe, respectively. In addition to the investigation of energy requirement, other significant parameters including energy penalty, plant efficiency, amine flow rate and extracted steam flow rate, are also presented. The study reveals that operating at partial load, for example at half load with 90% CO2 capture efficiency, as compared with full load, reduces the energy penalty, plant efficiency drop, amine flow rate and extracted steam flow rate by 9.9%, 24.4%, 50.0% and 49.9%, respectively. In addition, the effect of steam extracted from different locations from a series of steam turbine with the objective to achieve the lowest possible energy penalty is evaluated. The simulation shows that a low extracted steam pressure from a series of steam turbines, for example at 300 kPa, minimizes the energy penalty by up to 25.3%.  相似文献   

4.
Oxy-fuel combustion systems have been under development to reduce CO2 emissions from coal-fired power plants. In oxy-fuel combustion system, Hg in the flue gas causes corrosion in CO2 purification and compression units. Also, SO3 in the flue gas corrodes the equipment and ducts of oxy-fuel combustion system. Therefore, Hg and SO3 need to be removed.Babcock-Hitachi conducted tests using a 1.5 MWth Combustion & Air Quality Control System (AQCS) test facility which consists of oxygen supply unit, furnace, Selective Catalytic Reduction (SCR) catalyst, Clean Energy Recuperator (CER), Dry Electrostatic Precipitator (DESP), flue gas recirculation system, Wet Flue Gas Desulfurization (WFGD), and CO2 Compression and Purification Unit (CPU). In both cases of air and oxy-fuel combustion, the Hg removal across the DESP could be improved, and SO3 concentration at the DESP outlet could be reduced to less than 1 ppm by installing a CER upstream of the DESP and reducing the gas temperature at the DESP inlet. Hg was not dissolved in the drain recovered from CO2 compressor, and may be adsorbed at an inner part of CO2 compressor. This indicated that Hg needs to be removed at a location upstream of the CO2 compressor to prevent corrosion of the compressor.  相似文献   

5.
The biogas upgrading by membrane separation process using a highly efficient CO2-selective polyvinylamine/polyvinylalcohol (PVAm/PVA) blend membrane was investigated by experimental study and simulation with respect to process design, operation optimization and economic evaluation. This blend membrane takes advantages of the unique CO2 facilitated transport from PVAm and the robust mechanical properties from PVA, exhibits both high CO2/CH4 separation efficiency and very good stability. CO2 transports through the water swollen membrane matrix in the form of bicarbonate. CO2/CH4 selectivity up to 40 and CO2 permeance up to 0.55 m3(STP)/m2 h bar at 2 bar were documented in lab with synthesized biogas (35% CO2 and 65% CH4). Membrane performances at varying feed pressures were recorded and used as the simulation basis in this work. The process simulation of an on-farm scale biogas upgrading plant (1000 Nm3/h) was conducted. Processes with four different membrane module configurations with or without recycle were evaluated technically and economically, and the 2-stage in cascade with recycle configuration was proven optimal among the four processes. The sensitivity of the process to various operation parameters was analyzed and the operation conditions were optimized.  相似文献   

6.
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   

7.
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   

8.
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   

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.
A post-combustion CO2 capture process intended for offshore operations has been designed and optimised for integration with a natural gas-fired power plant on board a floating structure developed by the Norway-based company Sevan Marine ASA—designated Sevan GTW (gas-to-wire). The concept is constrained by the structure of the floater carrying a SIEMENS modular power system rated at 450 MWe, with a capture rate of 90% and CO2 compression (1.47 Mtpa) for pipeline pressure at 12 MPa. A net efficiency of 45% (based on a lower heating value) is estimated for the system with CO2 capture, thus suggesting that the post-combustion CO2 capture system is accountable for a fuel penalty of nine percentage points.The rationale behind the technology selection is the urgency of replacing the dispersed aero-derivative gas turbines which power the offshore oil and gas production units in Norwegian waters with near-zero emission power.As (inherently) fresh water usually constitutes a limiting factor in sea operations, efforts are made to obtain a neutral water balance to obtain an optimal design. This is primarily achieved by controlling the cleaned flue gas temperature at the top of the absorber column.  相似文献   

11.
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   

12.
The advanced zero emissions power plant (AZEP) project addresses the development of a novel “zero emissions,” gas turbine-based, power generation process to reduce local and global CO2 emissions in a cost-effective way.The key element in AZEP is an integrated MCM-reactor, in which (a) O2 is separated from air by means of a mixed-conducting membrane (MCM), (b) combustion of natural gas occurs in an N2-free environment and (c) the heat of combustion is transferred to air by heat exchange.This paper focuses on the development and testing of the ceramic components of the MCM-reactor (air separation membrane and heat exchangers). For compactness and manufacturability, a module design based on extruded square channel monoliths has been chosen. The manifold design enables gas distribution in a checkerboard pattern. Modules with contact area of >500 m2/m3 have been produced.Results from testing of the modules under close to realistic process conditions agree with model predictions. Extrapolation to AZEP process conditions gives an oxygen production rate of around 37 mol O2/(m3 s), or 15 MW/m3 power density (per net MCM volume). These values correspond to project targets and confirm the feasibility of the AZEP concept.  相似文献   

13.
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   

14.
Chemical-Looping Combustion (CLC) is an emerging technology for CO2 capture because separation of this gas from the other flue gas components is inherent to the process and thus no energy is expended for the separation. Natural or refinery gas can be used as gaseous fuels and they may contain different amounts of light hydrocarbons. This paper presents the combustion results obtained with a Cu-based oxygen carrier using mixtures of CH4 and light hydrocarbons (LHC) (C2H6 and C3H8) as fuel. The effect on combustion efficiency of the fuel reactor temperature, solid circulation flow rate and gas composition was studied in a continuous CLC plant (500 Wth). Full combustions were reached at 1073 and 1153 K working at oxygen to fuel ratios, ? higher than 1.5 and 1.2 respectively. Unburnt hydrocarbons were never detected at any experimental conditions at the fuel reactor outlet. Carbon formation can be avoided working at 1153 K or at ? values higher than 1.5 at 1073 K. After 30 h of continuous operation, the oxygen carrier exhibited an adequate behavior regarding attrition and agglomeration. It can be concluded that no special measures should be taken in a CLC process with Cu-based OC with respect to the presence of LHC in the fuel gas.  相似文献   

15.
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   

16.
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   

17.
This study investigates the possibility of capturing CO2 from flue gas under pressurised conditions, which could prove to be beneficial in comparison to working under atmospheric conditions. Simulations of two hybrid combined cycles with pressurised fluidised bed combustion and CO2 capture are presented. CO2 is captured from pressurised flue gas by means of chemical absorption after the boiler but before expansion. The results show a CO2 capture penalty of approximately 8 percentage points (including 90% CO2 capture rate and compression to 110 bar), which makes the efficiency for the best performing cycle 43.9%. It is 5.2 percentage points higher than the most probable alternative, i.e. using a natural gas fired combined cycle and a pulverised coal fired condensing plant separately with the same fuel split ratio. The largest part of the penalty is associated with the lower mass flow of flue gas after CO2 capture, which leads to a decrease in work output in the expander and potential for feed water heating. The penalty caused by the regeneration of absorbent is quite low, since the high pressure permits the use of potassium carbonate, which requires less regeneration heat than for example the more commonly proposed monoethanolamine. Although the efficiencies of the cycles look promising it will be important to perform a cost estimate to be able to make a fair comparison with other systems. Such a cost estimate has not been done in this study. A significant drawback of these hybrid cycles in that respect is the complex nature of the systems that will have a negative effect on the economy.  相似文献   

18.
Amine volatility is a key screening criterion for amines to be used in CO2 capture. Excessive volatility may result in significant economic losses and environmental impact. It also dictates the capital cost of the water wash. This paper reports measured amine volatility in 7 m MEA (monoethanolamine), 8 m PZ (piperazine), 7 m MDEA (n-methyldiethanolamine)/2 m PZ (piperazine), 12 m EDA (ethylenediamine), and 5 m AMP (2-amino-2-methyl-1-propanol) at 40–60 °C with lean and rich loadings giving CO2 partial pressures of 0.5 and 5 kPa at 40 °C. The amine concentrations were chosen to maximize CO2 capture capacity at acceptable viscosity. At the lean loading condition (where volatility is of greatest interest), the amines are ranked in order of increasing volatility: 7 m MDEA/2 m PZ (6/2 ppm), 8 m PZ (8 ppm), 12 m EDA (9 ppm), 7 m MEA (31 ppm), and 5 m AMP (112 ppm). The apparent amine partial molar excess enthalpies in these systems were estimated to range from ~10 to 87 kJ/mol of amine.  相似文献   

19.
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   

20.
A laboratory-scale reactor system was built and operated to demonstrate the feasibility of catalytically reacting carbon dioxide (CO2) with renewably-generated hydrogen (H2) to produce methane (CH4) according to the Sabatier reaction: CO2 + 4H2  CH4 + 2H2O. A cylindrical reaction vessel packed with a commercial methanation catalyst (Haldor Topsøe PK-7R) was used. Renewable H2 produced by electrolysis of water (from solar- and wind-generated electricity) was fed into the reactor along with a custom blend of 2% CO2 in N2, meant to represent a synthetic exhaust mixture. Reaction conditions of temperature, flow rates, and gas mixing ratios were varied to determine optimum performance. The extent of reaction was monitored by real-time measurement of CO2 and CH4. Maximum conversion of CO2 occurred at 300–350 °C. Approximately 60% conversion of CO2 was realized at a space velocity of about 10,000 h?1 with a molar ratio of H2/CO2 of 4/1. Somewhat higher total CO2 conversion was possible by increasing the H2/CO2 ratio, but the most efficient use of available H2 occurs at a lower H2/CO2 ratio.  相似文献   

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