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1.
With thermogravimetric apparatus (TGA), X-ray diffraction (XRD) and barium sulfate gravimetric methods, the carbonation reactivities of K2CO3 and K2CO3/Al2O3 in the simulated flue gases with SO2 are investigated and the reaction equations are inferred. Results show that there are KHCO3 and K2SO3 generated. The generation K2SO3 reduces the utilization ratio of the sorbent. H2O may accelerates the sulfation reaction of AR K2CO3 as K4H2(CO3)3·1.5H2O is generated in the reaction among K2CO3, SO2 and H2O. K2SO3 is directly generated from sulfation reaction of K2CO3/Al2O3, because there are K2CO3·1.5H2O and K2SO3 generated in the reaction among K2CO3/Al2O3, SO2 and H2O. K2CO3·1.5H2O does not react with SO2, and K2CO3·1.5H2O/Al2O3 reacts with SO2 slowly. Compare with the reaction process without H2O pretreatment, the reaction rates of KAl30 increased after H2O pretreatment and the failure ratio is about a half of that without H2O pretreatment. So, K2CO3/Al2O3 shows good carbonation and anti-sulfation characteristic after H2O pretreatment.  相似文献   

2.
Accurate experimental data on the thermo-physical properties of CO2-mixtures are pre-requisites for development of more accurate models and hence, more precise design of CO2 capture and storage (CCS) processes. A literature survey was conducted on both the available experimental data and the theoretical models associated with the transport properties of CO2-mixtures within the operation windows of CCS. Gaps were identified between the available knowledge and requirements of the system design and operation. For the experimental gas-phase measurements, there are no available data about any transport properties of CO2/H2S, CO2/COS and CO2/NH3; and except for CO2/H2O(/NaCl) and CO2/amine/H2O mixtures, there are no available measurements regarding the transport properties of any liquid-phase mixtures. In the prediction of gas-phase viscosities using Chapman–Enskog theory, deviations are typically <2% at atmospheric pressure and moderate temperatures. The deviations increase with increasing temperatures and pressures. Using both the Rigorous Kinetic Theory (RKT) and empirical models in the prediction of gas-phase thermal conductivities, typical deviations are 2.2–9%. Comparison of popular empirical models for estimation of gas-phase diffusion coefficients with newer experimental data for CO2/H2O shows deviations of up to 20%. For many mixtures relevant for CCS, the diffusion coefficient models based on the RKT show predictions within the experimental uncertainty. Typical reported deviations of the CO2/H2O system using empirical models are below 3% for the viscosity and the thermal conductivity and between 5 and 20% for the diffusion coefficients. The research community knows little about the effect of other impurities in liquid CO2 than water, and this is an important area to focus in future work.  相似文献   

3.
In the carbon capture and storage (CCS) chain, transport and storage set different requirements for the composition of the gas stream mainly containing carbon dioxide (CO2). Currently, there is a lack of standards to define the required quality for CO2 pipelines. This study investigates and recommends likely maximum allowable concentrations of impurities in the CO2 for safe transportation in pipelines. The focus is on CO2 streams from pre-combustion processes. Among the issues addressed are safety and toxicity limits, compression work, hydrate formation, corrosion and free water formation, including the cross-effect of H2S and H2O and of H2O and CH4.  相似文献   

4.
Chemical-looping combustion (CLC) has been suggested as an energy efficient method for the capture of carbon dioxide from combustion. Thermodynamics and kinetics of CaSO4 reduction with coal via gasification intermediate in a CLC process were discussed in the paper, with respect to the CO2 generating efficiency, the environmental factor and the surface morphology of oxygen carrier. Tests on the combined process of coal gasification and CaSO4 reduction with coal syngas were conducted in a batch fluidized bed reactor at different reaction temperatures and with different gasification intermediates. The products were characterized by gas chromatograph, gas analyzers and scanning electron microscope. And the results showed that an increase in the reaction temperature aggravated the SO2 emission. The CO2 generating efficiency also increased with the temperature, but it decreased when the temperature exceeded 950 °C due to the sintering of oxygen carrier particles. The use of CO2 as gasification intermediate in the fuel reactor had a positive effect on the sintering-resistant of oxygen carrier particles. However, increasing the steam/CO2 ratio in gasification intermediate evidently enhanced CO2 generating efficiency and reduced SO2 environmental impact.  相似文献   

5.
This work reveals levels of corrosion rate and polarization behavior of carbon steel immersed in aqueous solutions of monoethanolamine (MEA) used in the absorption-based carbon dioxide (CO2) capture process for greenhouse gas reduction from industrial flue gas streams. Such information was obtained from electrochemical-based corrosion experiments under a wide range of the CO2 capture process conditions. The corrosion of carbon steel was evaluated in respect to process parameters including partial pressure of oxygen (O2), CO2 loading in solution, solution velocity, solution temperature, MEA concentration and metal surface condition. Results show that the aqueous MEA solution containing CO2 provides a favorable condition for the corrosion of carbon steel to proceed. Corrosion rate is increased by all tested process parameters. These parametric effects were explained by the electrochemical kinetic data obtained from polarization curves and by the thermodynamic data obtained from Pourbaix diagram.  相似文献   

6.
A numerical study was conducted to predict pCO2 change in the ocean on a continental shelf by the leakage of CO2, which is originally stored in the aquifer under the seabed, in the case that a large fault connects the CO2 reservoir and the seabed by an earthquake or other diastrophism. The leakage rate was set to be 6.025 × 10−4 kg/m2/sec from 2 m × 100 m fault band, which corresponds to 3800 t-CO2/year, referring to the monitored seepage rate from an existing EOR field. The target space in this study was limited to the ocean above the seabed, the depth of which was 200 or 500 m. The computational domain was idealistically rectangular with the seabed fault-band perpendicular to the uniform flow. The CO2 takes a form of bubbles or droplets, depending on the depth of water, and their behaviour and dissolution were numerically simulated during their rise in seawater flow. The advection–diffusion of dissolved CO2 was also simulated. As a result, it was suggested that the leaked CO2 droplets/bubbles all dissolve in the seawater before spouting up to the atmosphere, and that the increase in pCO2 in the seawater was smaller than 500 μ atm.  相似文献   

7.
The goal of this paper is to find methodologies for removing a selection of impurities (H2O, O2, Ar, N2, SOx and NOx) from CO2 present in the flue gas of two oxy-combustion power plants fired with either natural gas (467 MW) or pulverized fuel (596 MW). The resulting purified stream, containing mainly CO2, is assumed to be stored in an aquifer or utilized for enhanced oil recovery (EOR) purposes. Focus has been given to power cycle efficiency i.e.: work and heat requirements for the purification process, CO2 purity and recovery factor (kg of CO2 that is sent to storage per kg of CO2 in the flue gas). Two different methodologies (here called Case I and Case II) for flue gas purification have been developed, both based on phase separation using simple flash units (Case I) or a distillation column (Case II). In both cases purified flue gas is liquefied and its pressure brought to 110 atm prior to storage.Case I: A simple flue gas separation takes place by means of two flash units integrated in the CO2 compression process. Heat in the process is removed by evaporating the purified liquid CO2 streams coming out from both flashes. Case I shows a good performance when dealing with flue gases with low concentration of impurities. CO2 fraction after purification is over 96% with a CO2 recovery factor of 96.2% for the NG-fired flue gas and 88.1% for the PF-fired flue gas. Impurities removal together with flue gas compression and liquefaction reduces power plant output of 4.8% for the NG-fired flue gas and 11.6% for the PF-fired flue gas. The total amount of work requirement per kg stored CO2 is 453 kJ for the NG-fired flue gas and 586 kJ for the PF-fired flue gas.Case II: Impurities are removed from the flue gas in a distillation column. Two refrigeration loops (ethane and propane) have been used in order to partially liquefy the flue gas and for heat removal from a partial condenser. Case II can remove higher amounts of impurities than Case I. CO2 purity prior to storage is over 99%; CO2 recovery factor is somewhat lower than in Case I: 95.4% for the NG-fired flue gas and 86.9% for the PF-fired flue gas, reduction in the power plant output is similar to Case I.Due to the lower CO2 recovery factor the total amount of work per kg stored CO2 is somewhat higher for Case II: 457 kJ for the NG-fired flue gas and 603 kJ for the PF-fired flue gas.  相似文献   

8.
CO2 and SO2 are some of the main polluting gases emitted into atmosphere in combustion processes using fossil fuel for energy production. The former is one of the major contributors to build-up the greenhouse effect implicated in global climate change and the latter produces acid rain. Oxy-fuel combustion is a technology, which consists in burning the fuel with a mix of pure O2 and recirculated CO2. With this technology the CO2 concentration in the flue gas may be enriched up to 95%, becoming possible an easy CO2 recovery. In addition, oxy-fuel combustion in fluidized beds allows in situ desulfurization of combustion gases by supplying calcium based sorbent.In this work, the effect of the principal operation variables affecting the sulfation reaction rate in fluidized bed reactors (temperature, CO2 partial pressure, SO2 concentration and particle size) under typical oxy-fuel combustion conditions have been analyzed in a batch fluidized bed reactor using a limestone as sorbent. It has been observed that sulfur retention can be carried out by direct sulfation of the CaCO3 or by sulfation of the CaO (indirect sulfation) formed by CaCO3 calcination. Direct sulfation and indirect sulfation operating conditions depended on the temperature and CO2 partial pressure. The rate of direct sulfation rose with temperature and the rate of indirect sulfation for long reaction times decreased with temperature. An increase in the CO2 partial pressure had a negative influence on the sulfation conversion reached by the limestone due to a higher temperature was needed to work in conditions of indirect sulfation. Thus, it is expected that the optimum temperature for sulfur retention in oxy-fuel combustion in fluidized bed reactors be about 925–950 °C. Sulfation reaction rate rose with decreasing sorbent particle size and increasing SO2 concentration.  相似文献   

9.
The effect of reaction conditions on the carbonation characteristics of K2CO3 calcined from KHCO3 was investigated with a pressurized thermogravimetric apparatus. Results show that the conversion rate decreased as the reaction temperature and pressure increased, and the effect of CO2 and H2O concentration is little. The mean reaction rate maintained constant of 3%/min. The maximum reaction rate increased as the temperature and H2O concentration increased, and the pressure decreased. The reaction temperature and pressure are the key factors, and it is important to control those carefully for this technique. The optimum reaction condition is 60 °C, 18% CO2, 18% H2O, and 1 atm. K2CO3 calcined from KHCO3 showed excellent CO2 capture capability in this condition.  相似文献   

10.
The degradation of polyacrylamide (PAM) in simulate wastewater was studied in UV/Fenton/C4H4O62? system. The factors such as molecular ratio of H2O2/Fe2+/C4H4O62?, pH, and the dosage of Fenton reagent that could affect the PAM degradation in the UV/Fenton/C4H4O62? system were investigated. The experimental results showed that adding C4H4O62? to UV/Fenton system could form photosensitive ferrous complexes, which led to higher degradation efficiency of PAM. The degradation rate of PAM could be up to 95.2% under the following conditions: the concentration of H2O2, Fe2+, and C4H4O62? were 22.5, 2.25, and 2.25 mmol/L, respectively (i.e., molecular ratio of H2O2/Fe2+/C4H4O62? was 10:1:1), the pH value was 3.0.  相似文献   

11.
ABSTRACT

In this paper, a wet chemical method is used to coat LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode material by Li2O-2B2O3 (LBO) layer for Lithium-ion batteries (LIBs). For performance optimization, the effects of different contents (thicknesses) of LBO coating layers on NCM811 particle surface on the morphologies, structures, compositions, and electrochemical properties of the corresponding LIBs are studied using XRD, SEM, TEM, and electrochemical measurements. Coin LIBs are assembled with such coated NCM811 cathode materials for performance validation. Results show that LBO coating layer does not change the original lattice structure of the bulk material, it can only adhere to the surface of the bulk material. After coating, NCM811 shows a good crystallinity and the ordered layered structure. TEM images show that the thickness of LBO coating is increased with increasing LBO content, and that the appropriate LBO coating thickness and uniform coating state are conducive to the improvement of the electrochemical properties of NCM811 cathode materials. Particularly, NCM811 with LBO coating content of 1000 ppm shows the best performance compared to other coating contents. In this case, the coating thickness is relatively uniform, which is about 40~100 nm, giving a good first charge-discharge capacity of 214.1mAh/g, and a high Coulomb efficiency of 90.06%. After 50 cycles, the capacity retention rate of LIBs still keeps as high as 99.64%. Therefore, LBO coating can improve the performance of NCM811 and then the lithium-ion batteries.  相似文献   

12.
Climate change is being caused by greenhouse gases such as carbon dioxide (CO2). Carbon capture and storage (CCS) is of interest to the scientific community as one way of achieving significant global reductions of atmospheric CO2 emissions in the medium term. CO2 would be captured from large stationary sources such as power plants and transported via pipelines under high pressure conditions to underground storage. If a downward leakage from a surface transportation system module occurs, the CO2 would undergo a large temperature reduction and form a bank of “dry ice” on the ground surface; the sublimation of the gas from this bank represents an area source term for subsequent atmospheric dispersion, with an emission rate dependent on the energy balance at the bank surface. Gaseous CO2 is denser than air and tends to remain close to the surface; it is an asphyxiant, a cerebral vasodilator and at high concentrations causes rapid circulatory insufficiency leading to coma and death. Hence a subliming bank of dry ice represents safety hazard. A model is presented for evaluating the energy balance and sublimation rate at the surface of a solid frozen CO2 bank under different environmental conditions. The results suggest that subliming gas behaves as a proper dense gas (i.e. it remains close to the ground surface) only for low ambient wind speeds.  相似文献   

13.
Global warming is a result of increasing anthropogenic CO2 emissions, and the consequences will be dramatic climate changes if no action is taken. One of the main global challenges in the years to come is therefore to reduce the CO2 emissions.Increasing energy efficiency and a transition to renewable energy as the major energy source can reduce CO2 emissions, but such measures can only lead to significant emission reductions in the long-term. Carbon capture and storage (CCS) is a promising technological option for reducing CO2 emissions on a shorter time scale.A model to calculate the CO2 capture potential has been developed, and it is estimated that 25 billion tonnes CO2 can be captured and stored within the EU by 2050. Globally, 236 billion tonnes CO2 can be captured and stored by 2050. The calculations indicate that wide implementation of CCS can reduce CO2 emissions by 54% in the EU and 33% globally in 2050 compared to emission levels today.Such a reduction in emissions is not sufficient to stabilize the climate. Therefore, the strategy to achieve the necessary CO2 emissions reductions must be a combination of (1) increasing energy efficiency, (2) switching from fossil fuel to renewable energy sources, and (3) wide implementation of CCS.  相似文献   

14.
The prepared different components municipal solid wastes based carbons were used to investigate the adsorption of CO2. The optimum conditions for CO2 adsorption were investigated firstly. And then, the CO2 adsorption performance of different components based carbon adsorbents were compared with each other under the optimum parameters. The results illustrated that the triple components (pinewood, acrylic textile, and tire) based carbon exhibited the best adsorption performance, which is 1.522 mmol/g and its physical prosperity was also conducted to interpret the adsorption mechanism. Besides, to further approach to the actual gas, the influence of additional O2 and SO2 on CO2 adsorption properties of ternary-component-based carbon was investigated. The results illustrate that O2 concentration exerts little effect on adsorption capacity. SO2 plays the dominated role in the competitive adsorption effect.  相似文献   

15.
CO2 storage capacity estimation: Methodology and gaps   总被引:3,自引:0,他引:3  
Implementation of CO2 capture and geological storage (CCGS) technology at the scale needed to achieve a significant and meaningful reduction in CO2 emissions requires knowledge of the available CO2 storage capacity. CO2 storage capacity assessments may be conducted at various scales—in decreasing order of size and increasing order of resolution: country, basin, regional, local and site-specific. Estimation of the CO2 storage capacity in depleted oil and gas reservoirs is straightforward and is based on recoverable reserves, reservoir properties and in situ CO2 characteristics. In the case of CO2-EOR, the CO2 storage capacity can be roughly evaluated on the basis of worldwide field experience or more accurately through numerical simulations. Determination of the theoretical CO2 storage capacity in coal beds is based on coal thickness and CO2 adsorption isotherms, and recovery and completion factors. Evaluation of the CO2 storage capacity in deep saline aquifers is very complex because four trapping mechanisms that act at different rates are involved and, at times, all mechanisms may be operating simultaneously. The level of detail and resolution required in the data make reliable and accurate estimation of CO2 storage capacity in deep saline aquifers practical only at the local and site-specific scales. This paper follows a previous one on issues and development of standards for CO2 storage capacity estimation, and provides a clear set of definitions and methodologies for the assessment of CO2 storage capacity in geological media. Notwithstanding the defined methodologies suggested for estimating CO2 storage capacity, major challenges lie ahead because of lack of data, particularly for coal beds and deep saline aquifers, lack of knowledge about the coefficients that reduce storage capacity from theoretical to effective and to practical, and lack of knowledge about the interplay between various trapping mechanisms at work in deep saline aquifers.  相似文献   

16.
The membrane separation process for CO2 capture can be interfered by the gaseous components and the fine particles in flue gas, especially in desulfurized flue gas. In this work, the pint-sized Polyimide(PI) hollow fiber membrane contactors were self-packed to investigate the membrane CO2 separation from flue gas containing fine particles and gaseous contaminants (SO2,SO3,H2O). First, the effects of SO2, SO3, water vapor, and gypsum particles on the CO2 capture were studied independently and synergistically. The results showed that the effect of SO2 on the membrane separation properties is indistinctive; however, the membrane performance was damaged seriously with the addition of SO3. The high humidity promoted the CO2 separation initially before inhibiting the PI membrane performance. Moreover, the decrease of the CO2/N2 selectivity and the permeation rate were accelerated with the coexistence of SO2. The membrane performance showed an obvious deterioration in the presence of gypsum particles, with a 21% decrease in the CO2/N2 selectivity and 51% decrease in the permeation rate. Furthermore, the gypsum particles exerted dramatic damage. Under the WFGD conditions, the combined effects of SO2, water vapor, and the gypsum particles influenced the stability of the membrane significantly. This tendency is mainly attributed to the deposition of fine particles and aerosol on the membrane surface, which occupied the effective area and enhanced the mass transfer resistance. This study of impurities’ influence could play an important role in further industrial application of membrane CO2 capture.  相似文献   

17.
Effect of oxygenated liquid additives on the urea based SNCR process   总被引:1,自引:0,他引:1  
An experimental investigation was performed to study the effect of oxygenated liquid additives, H2O2, C2H5OH, C2H4(OH)2 and C3H5(OH)3 on NOx removal from flue gases by the selective non-catalytic reduction (SNCR) process using urea as a reducing agent. Experiments were performed with a 150 kW pilot scale reactor in which a simulated flue gas was generated by the combustion of methane operating with 6% excess oxygen in flue gases. The desired levels of initial NOx (500 ppm) were achieved by doping the fuel gas with ammonia. Experiments were performed throughout the temperature range of interest, i.e. from 800 to 1200 °C for the investigation of the effects of the process additives on the performance of aqueous urea DeNOx. With H2O2 addition a downward shift of 150 °C in the peak reduction temperature from 1130 to 980 °C was observed during the experimentation, however, the peak reduction efficiency was reduced from 81 to 63% when no additive was used. The gradual addition of C2H5OH up to a molar ratio of 2.0 further impairs the peak NOx reduction efficiency by reducing it to 50% but this is accompanied by a downward shift of 180 °C in the peak reduction temperature. Further exploration using C2H4(OH)2 suggested that a 50% reduction could be attained for all the temperatures higher than 940 °C. The use of C3H5(OH)3 as a secondary additive has a significant effect on the peak reduction efficiency that decreased to 40% the reductions were achievable at a much lower temperature of 800 °C showing a downward shift of 330 °C.  相似文献   

18.
There is a strong political will to decrease CO2 emissions. Although the steel industry only accounts for some 5% of worldwide CO2 emissions (which totalled 1,200 million tonnes per annum in the late 1990s), it will be strongly affected by this. The EU, for example, is putting up strong economic incentives for reductions. This is taking place at a time when demand for steel products is greater than ever. To radically change existing processes and production routes to decrease the CO2 emissions would be extremely expensive, even if it were possible. Nevertheless, many of the solutions which have been discussed seem to go in this direction. The other alternative discussed seems to be the creation of process solutions and alterations that lead to a focusing of CO2 streams, i.e., much higher CO2 concentrations in flue gases than today, for entrapment of the CO2 so that it is not discharged into the atmosphere. These solutions are feasible, but expensive.

However, there exists today a number of solutions and technologies which, if fully implemented, could substantially decrease CO2 emissions without seriously altering current methods of operation; they are short-term viable solutions. The present paper reviews and discusses such technologies, throughout the steel production paths. If these solutions are fully implemented, the combined impact on CO2 emissions from the steel industry worldwide is estimated to be a reduction of 100–150 million tonnes of CO2 per annum, i.e., current emissions can be reduced by some 8–10% within a relatively short time span.  相似文献   

19.
To test the injection behaviour of CO2 into brine-saturated rock and to evaluate the dependence of geophysical properties on CO2 injection, flow and exposure experiments with brine and CO2 were performed on sandstone samples of the Stuttgart Formation representing potential reservoir rocks for CO2 storage. The sandstone samples studied are generally fine-grained with porosities between 17 and 32% and permeabilities between 1 and 100 mD.Additional batch experiments were performed to predict the long-term behaviour of geological CO2 storage. Reservoir rock samples were exposed over a period of several months to CO2-saturated reservoir fluid in high-pressure vessels under in situ temperature and pressure conditions. Petrophysical parameters, porosity and the pore radius distribution were investigated before and after the experiments by NMR (Nuclear Magnetic Resonance) relaxation and mercury injection. Most of the NMR measurements of the tested samples showed a slight increase of porosity and a higher proportion of large pores.  相似文献   

20.
Acid gas geological disposal is a promising process to reduce CO2 atmospheric emissions and an environment-friendly and economic alternative to the transformation of H2S into sulphur by the Claus process. Acid gas confinement in geological formations is to a large extent controlled by the capillary properties of the water/acid–gas/caprock system, because a significant fraction of the injected gas rises buoyantly and accumulates beneath the caprock. These properties include the water/acid gas interfacial tension (IFT), to which the so-called capillary entry pressure of the gas in the water-saturated caprock is proportional. In this paper we present the first ever systematic water/acid gas IFT measurements carried out by the pendant drop technique under geological storage conditions. We performed IFT measurements for water/H2S systems over a large range of pressure (up to P = 15 MPa) and temperature (up to T = 120 °C). Water/H2S IFT decreases with increasing P and levels off at around 9–10 mN/m at high T (≥70 °C) and P (>12 MPa). The latter values are around 30–40% of water/CO2 IFTs, and around 20% of water/CH4 IFTs at similar T and P conditions. The IFT between water and a CO2 + H2S mixture at T = 77 °C and P > 7.5 MPa is observed to be approximately equal to the molar average IFT of the water/CO2 and water/H2S binary mixtures. Thus, when the H2S content in the stored acid gas increases the capillary entry pressure decreases, together with the maximum height of acid gas column and potential storage capacity of a given geological formation. Hence, considerable attention should be exercised when refilling with a H2S-rich acid gas a depleted gas reservoir, or a depleted oil reservoir with a gas cap: in the case of hydrocarbon reservoirs that were initially (i.e., at the time of their discovery) close to capillary leakage, acid gas leakage through the caprock will inevitably occur if the refilling pressure approaches the initial reservoir pressure.  相似文献   

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