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1.
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   

2.
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   

3.
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   

4.
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   

5.
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   

6.
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   

7.
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   

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.
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   

10.
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   

11.
Gas conditioning is commonly referred to as the required processing for a produced natural gas to achieve transport and sales specifications. In this paper, gas conditioning as the processing required in the interface between CO2 capture and transport is studied for nine different natural gas fired power plant concepts and three different CO2 transport processes. Conditioning processes for both pipeline and ship transport are described and an enhanced process for volatile removal is developed. The energy requirement for the conditioning processes is normally between 90 and 120 kWh/tonne CO2; however, this depends on the pressure and composition of the captured CO2-rich stream. The loss of CO2 in the water purge is small for most capture processes. The waste streams from the gas conditioning processes can contain large amounts of CO2 and should therefore be further processed or reintroduced at an appropriate point upstream in the capture or gas conditioning process if possible. The integration benefit may vary depending on the composition of the CO2-rich stream. It could be particularly interesting for processes with “innovative reactors” (membranes, sorbents, chemical looping) to integrate CO2 capture and gas conditioning.  相似文献   

12.
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   

13.
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   

14.
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   

15.
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   

16.
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   

17.
By analyzing how the largest CO2 emitting electricity-generating region in the United States, the East Central Area Reliability Coordination Agreement (ECAR), responds to hypothetical constraints on greenhouse gas emissions, the authors demonstrate that there is an enduring role for post-combustion CO2 capture technologies. The utilization of pulverized coal generation with carbon dioxide capture and storage (PC + CCS) technologies is particularly significant in a world where there is uncertainty about the future evolution of climate policy and in particular uncertainty about the rate at which the climate policy will become more stringent. The paper's analysis shows that within this one large, heavily coal-dominated electricity-generating region, as much as 20–40 GW of PC + CCS could be operating before the middle of this century. Depending upon the state of PC + CCS technology development and the evolution of future climate policy, the analysis shows that these CCS systems could be mated to either pre-existing PC units or PC units that are currently under construction, announced and planned units, as well as PC units that could continue to be built for a number of decades even in the face of a climate policy. In nearly all the cases analyzed here, these PC + CCS generation units are in addition to a much larger deployment of CCS-enabled coal-fueled integrated gasification combined cycle (IGCC) power plants. The analysis presented here shows that the combined deployment of PC + CCS and IGCC + CCS units within this one region of the U.S. could result in the potential capture and storage of between 3.2 and 4.9 Gt of CO2 before the middle of this century in the region's deep geologic storage formations.  相似文献   

18.
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   

19.
Calcium looping (CaL) is a promising post-combustion CO2 capture technology which is carried out in a dual fluidized bed (DFB) system with continuous looping of CaO, the CO2 carrier, between two beds. The system consists of a carbonator, where flue gas CO2 is adsorbed by CaO and a regenerator, where captured CO2 is released. The CO2-rich regenerator flue gas can be sequestered after gas processing and compression. A parametric study was conducted on the 10 kWth DFB facility at the University of Stuttgart, which consists of a bubbling fluidized bed carbonator and a riser regenerator. The effect of the following parameters on CO2 capture efficiency was investigated: carbonator space time, carbonator temperature and calcium looping ratio. The active space time in the carbonator, which is a function of the space time and the calcium looping ratio, was found to strongly correlate with the CO2 capture efficiency. BET and BJH techniques provided surface area and pore volume distribution data, respectively, for collected sorbent samples. The rate of sorbent attrition was found to be 2 wt.%/h which is below the expected sorbent make-up rate required to maintain sufficient sorbent activity. Steady-state CO2 capture efficiencies greater than 90% were achieved for different combinations of operational parameters. Moreover, the experimental results obtained were briefly compared with results derived from reactor modeling studies. Finally, the implications of the experimental results with respect to commercialization of the CaL process have been assessed.  相似文献   

20.
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   

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