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1.
The effect of bed height on CO2 capture was investigated by carbonation/regeneration cyclic operations using a bubbling fluidized bed reactor. We used a potassium-based solid sorbent, SorbKX35T5 which was manufactured by the Korea Electric Power Research Institute. The sorbent consists of 35% K2CO3 for absorption and 65% supporters for mechanical strength. We used a fluidized bed reactor with an inner diameter of 0.05 m and a height of 0.8 m which was made of quartz and placed inside of a furnace. The operating temperatures were fixed at 70 °C and 150 °C for carbonation and regeneration, respectively. The carbonation/regeneration cyclic operations were performed three times at four different L/D (length vs diameter) ratios such as one, two, three, and four. The amount of CO2 captured was the most when L/D ratio was one, while the period of maintaining 100% CO2 removal was the longest as 6 minutes when L/D ratio was three. At each cycle, CO2 sorption capacity (g CO2/g sorbent) was decreased as L/D ratio was increased. The results obtained in this study can be applied to design and operate a large scale CO2 capture process composed of two fluidized bed reactors. This work was presented at the 7 th China-Korea Workshop on Clean Energy Technology held at Taiyuan, Shanxi, China, June 26–28, 2008.  相似文献   

2.
In recent years several processes incorporating a carbonation-calcination loop in an interconnected fluidized bed reactor have been proposed as a way to capture CO2 from flue gases. This paper is a first approximation to the modelling of a fluidized bed carbonator reactor. In this reactor the flue gas comes into contact with an active bed composed of particles with very different activities, depending on their residence time in the bed and in the carbonation-calcination loop. The model combines the residence time distribution functions with existing knowledge about sorbent deactivation rates and sorbent reactivity. The fluid dynamics of the solids (CSTR) and gases (PF) in the carbonator are based on simple assumptions. The carbonation rates are modelled defining a characteristic time for the transition between a fast reaction regime to a regime with a zero reaction rate. On the basis of these assumptions the model is able to predict the CO2 capture efficiency for the flue gas depending on the operating and design conditions. Operating windows with high capture efficiencies are discussed, as well as those conditions where only modest capture efficiencies are possible.  相似文献   

3.
The effects of superficial gas velocity (Ug), wavelength and intensity of ultraviolet (UV) light, oxygen and H2O concentration on the photocatalytic degradation of TCE (Trichloroethylene) over TiO2/SiO2 catalyst have been determined in an annulus fluidized bed photoreactor. The key factor in determining the performance of the annulus fluidized bed photoreactor is found to be an optimum superficial gas velocity (Ug) that provides the optimum UV lighttransmit through the proper size of bubbles in the photoreactor. The degradation efficiency of TCE increases with light intensity but decreases with wavelength of the UV light and H2O concentration in the fluidized bed of TiO2/silica-gel photocatalyst. The optimum concentration of O2 for TCE degradation is found to be approximately 10%. The annulus fluidized bed photoreactor is an effective tool for high TCE degradation with efficient utilization of photon energy. This paper is dedicated to Professor Dong Sup Doh on the occasion of his retirement from Korea University.  相似文献   

4.
To demonstrate process feasibility of in situ CO2 capture from combustion of fossil fuels using Ca-based sorbent looping technology, a flexible atmospheric dual fluidized bed combustion system has been constructed. Both reactors have an ID of 100 mm and can be operated at up to 1000 °C at atmospheric pressure. This paper presents preliminary results for a variety of operating conditions, including sorbent looping rate, flue gas stream volume, CaO/CO2 ratio and combustion mode for supplying heat to the sorbent regenerator, including oxy-fuel combustion of biomass and coal with flue gas recirculation to achieve high-concentration CO2 in the off-gas. It is the authors' belief that this study is the first demonstration of this technology using a pilot-scale dual fluidized bed system, with continuous sorbent looping for in situ CO2 capture, albeit at atmospheric pressure. A multi-cycle test was conducted and a high CO2 capture efficiency (> 90%) was achieved for the first several cycles, which decreased to a still acceptable level (> 75%) even after more than 25 cycles. The cyclic sorbent was sampled on-line and showed general agreement with the features observed using a lab-scale thermogravimetric analysis (TGA) apparatus. CO2 capture efficiency decreased with increasing number of sorbent looping cycles as expected, and sorbent attrition was found to be another significant factor to be limiting sorbent performance.  相似文献   

5.
A two-dimensional (2D) transient model was developed to simulate the local hydrodynamics of a gas (flue gas)–solid (CaO)–solid (CaCO3) three-phase fluidized-bed carbonator using the computational fluid dynamic method, where the chemical reaction model was adopted to determine the molar fraction of CO2 at the exit of carbonator and the partial pressure of CO2 in the carbonator. This investigation was intended to improve an understanding of the chemical reaction effects of CaO with CO2 on the CO2 capture efficiency of combustion flue gases. For this purpose, we had utilized Fluent 6.2 to predict the CO2 capture efficiency for different operation conditions. The adopted model concerning the reaction rate of CaO with CO2 is joined into the CFD software. Model simulation results, such as the local time-averaged CO2 molar fraction and conversion of CaO, were validated by experimental measurements under varied operating conditions, e.g., the fraction of active CaO, chemical reaction temperature, particle size, and cycle number at different locations in a gas–solid–solid three-phase fluidized bed carbonator. Furthermore, the local transient hydrodynamic characteristics, such as gas molar fraction and partial pressure were predicted reasonably by the chemical reaction model adopted for the dynamic behaviors of the gas–solid–solid three-phase fluidized bed carbonator. On the basis of this analysis, capture CO2 strategies to reduce CO2 molar fraction in exit of carbonator reactor can be developed in the future. It is concluded that a fluidized bed of CaO can be a suitable reactor to achieve very effective CO2 capture from combustion flue gases.  相似文献   

6.
A new regenerable alumina-modified sorbent was developed for CO2 capture at temperatures below 200 °C. The CO2 capture capacity of a potassium-based sorbent containing Al2O3 (KAlI) decreased during multiple CO2 sorption (60 °C) and regeneration (200 °C) tests due to the formation of the KAl(CO3)(OH)2 phase, which could be converted into the original K2CO3 phase above 300 °C. However, the new regenerable potassium-based sorbent (Re-KAl(I)) maintained its CO2 capture capacity during multiple tests even at a regeneration temperature of 130 °C. In particular, the CO2 capture capacity of the Re-KAl(I)60 sorbent which was prepared by the impregnation of Al2O3 with 60 wt.% K2CO3 was about 128 mg CO2/g sorbent. This excellent CO2 capture capacity and regeneration property were due to the characteristics of the Re-KAl(I) sorbent producing only a KHCO3 phase during CO2 sorption, unlike the KAlI30 sorbent which formed the KHCO3 and KAl(CO3)(OH)2 phases even at 60 °C. This result was explained through the structural effect of the support containing the KAl(CO3)(OH)2 phase which was prepared by impregnation of Al2O3 with K2CO3 in the presence of CO2.  相似文献   

7.
The effect of the regeneration temperature (150°, 250°, and 350°C) during multiple CO2 cyclic sorption-regeneration cycles of a K2CO3/Al2O3 solid sorbent in a bubbling fluidized bed reactor was evaluated in terms of the CO2 capture capacity and chemical composition of the solid sorbent. The CO2 capture capacity after regeneration at 150° and 250°C decreased with increasing cycle numbers, reaching approximately 57 and 78%, respectively, and 19.0 and 39.3%, respectively, of the original capacity after one and five regeneration cycles. This decline in the CO2 capture capacity was due to the accumulation of KHCO3 (at 150°C) and KAl(CO3)2(OH)2 (150° and 250°C) from their incomplete degradation back to the K2CO3/Al2O3 solid sorbent. When regenerated at 350°C, the CO2 capture capacity remained essentially constant in each cycle number because of complete desorption (no residual KHCO3 and KAl(CO3)2(OH)2). The formation mechanism of complex structure occurred similar to the one in a fixed bed reactor/thermogravimetric analyzer with lower regeneration temperature. The general operation conditions for K2CO3/Al2O3 solid sorbents are summarized.  相似文献   

8.
Potassium-based sorbent was prepared by impregnation with potassium carbonate on activated carbon. The role of water and its effects on pretreatment and CO2 absorption was investigated in a fixed bed reactor. K2CO3 could be easily converted into K2CO3·1.5H2O working as an active species by the absorption of water vapor as the following reaction: K2CO3+3/2 H2O→K2CO3·1.5H2O. One mole of K2CO3·1.5H2O absorbed one mole of CO2 as the following reaction: K2CO3·1.5H2O+CO2ai2KHCO3+0.5 H2O. The K2CO3·1.5H2O phase, however, was easily transformed to the K2CO3 phase by thermal desorption even at low temperature under low relative humidity. To enhance CO2 capture capacity and CO2 absorption rate, it is very important to maintain the K2CO3·1.5H2O phase worked as an active species, as well as to convert the entire K2CO3 to the K2CO3·1.5H2O phase during CO2 absorption at a temperature range between 50 °C and 70 °C. As a result, the relative humidity plays a very important role in preventing the transformation from K2CO3·1.5H2O to the original phase (K2CO3) as well as in producing the K2CO3·1.5H2O from K2CO3, during CO2 absorption between 50 °C and 70 °C.  相似文献   

9.
A novel silica–titania (SiO2–TiO2) nanocomposite has been developed to effectively capture elemental mercury (Hg0) under UV irradiation. Previous studies under room conditions showed over 99% Hg0 removal efficiency using this nanocomposite. In this work, the performance of the nanocomposite on Hg0 removal was tested in simulated coal-fired power plant flue gas, where water vapor concentration is much higher and various acid gases, such as HCl, SO2, and NOx, are present. Experiments were carried out in a fix-bed reactor operated at 135 °C with a baseline gas mixture containing 4% O2, 12% CO2, and 8% H2O balanced with N2. Results of Hg speciation data at the reactor outlet demonstrated that Hg0 was photocatalytically oxidized and captured on the nanocomposite. The removal efficiency of Hg0 was found to be significantly affected by the flue gas components. Increased water vapor concentration inhibited Hg0 capture, due to the competitive adsorption of water vapor. Both HCl and SO2 promoted the oxidation of Hg0 to Hg(II), resulting in higher removal efficiencies. NO was found to have a dramatic inhibitory effect on Hg0 removal, very likely due to the scavenging of hydroxyl radicals by NO. The effect of NO2 was found to be insignificant. Hg removal in flue gases simulating low rank coal combustion products was found to be less than that from high rank coals, possibly due to the higher H2O concentration and lower HCl and SO2 concentrations of the low rank coals. It is essential, however, to minimize the adverse effect of NO to improve the overall performance of the SiO2–TiO2 nanocomposite.  相似文献   

10.
Chemical looping combustion (CLC) is a flameless two-step fuel combustion that produces a pure CO2 stream, ready for compression and sequestration. The process is composed of two interconnected fluidized bed reactors. The air reactor which is a conventional circulating fluidized bed and the fuel reactor which is a bubbling fluidized bed. The basic principle is to avoid the direct contact of air and fuel during the combustion by introducing a highly-reactive metal particle, referred to as oxygen carrier, to transport oxygen from the air to the fuel. In the process, the products from combustion are kept separated from the rest of the flue gases namely nitrogen and excess oxygen. This process eliminates the energy intensive step to separate the CO2 from nitrogen-rich flue gas that reduce the thermal efficiency.Fundamental knowledge of multiphase reactive fluid dynamic behavior of the gas-solid flow is essential for the optimization and operation of a chemical looping combustor.Our recent thorough literature review shows that multiphase CFD-based models have not been adapted to chemical looping combustion processes in the open literature. In this study, we have developed the reaction kinetics model of the fuel reactor and implemented the kinetic model into a multiphase hydrodynamic model, MFIX, developed earlier at the National Energy Technology Laboratory. Simulated fuel reactor flows revealed high weight fraction of unburned methane fuel in the flue gas along with CO2 and H2O. This behavior implies high fuel loss at the exit of the reactor and indicates the necessity to increase the residence time, say by decreasing the fuel flow rate, or to recirculate the unburned methane after condensing and removing CO2.  相似文献   

11.
Sorbent-enhanced/membrane-assisted steam-methane reforming   总被引:1,自引:0,他引:1  
Thermodynamic equilibrium and kinetic reactor models are used to simulate a fluidized bed membrane reactor with in situ or ex situ hydrogen and/or CO2 removal for production of pure hydrogen by steam methane reforming. In the equilibrium model, the membranes and CO2 removal are located in separate vessels downstream of the reformer. As the recycle ratio increases, the overall performance approaches that where membranes are located inside the reactor. Whether located in situ or ex situ, hydrogen removal by membranes and CO2 capture by sorbents both enhance hydrogen production. In the kinetic reactor model, a circulating fluidized bed membrane reformer is coupled with a catalyst/sorbent regenerator. Sorbent enhancement combined with membranes could provide very high hydrogen yields. In addition, since carbonation is exothermic, with its heat of reaction similar in magnitude to the endothermic heat of reaction of the net reforming reactions, sorbent enhancement can provide much of the heat needed in the reformer. The overall heat needed for the process would then be provided in a separate calciner, acting as a sorbent regenerator. While the technology is promising, several practical issues need to be examined.  相似文献   

12.
A kinetic theory based hydrodynamic model with experimentally determined sorption rates for reaction of CO2 with K2CO3 solid sorbent is used to design a compact circulating fluidized bed sorption‐regeneration system for CO2 removal from flue gases. Because of high solids fluxes, the sorber does not require internal or external cooling. The output is verified by computing the granular temperatures, particle viscosities, dispersion, and mass transfer coefficients. These properties agree with reported measurement values except the radial dispersion coefficients, which are much higher due to the larger bed diameter. With the solid sorbent prepared according to published information, the CO2 removal percentage at the riser top is 69.16%. To improve the CO2 removal, an effort is needed to develop a better sorbent or to simply lower the inlet gas velocity to operate in a denser mode, leading to a larger system. Also, the effect of temperature rise on the removal efficiency is investigated. © 2010 American Institute of Chemical Engineers AIChE J, 2010  相似文献   

13.
There is increasing interest in CO2 looping cycles that involve the repeated calcination and carbonation of the sorbent as a way to capture CO2 from flue gases during the carbonation step and the generation of a pure stream of CO2 in the oxyfired calcination step. In particular, attrition of the material in these interconnected fluidized bed reactors is a problem of general concern. Attrition of limestone derived materials has been studied in fluidized bed systems by numerous authors. In this work, we have investigated the attrition of two limestones used in a system of two interconnected circulating fluidized bed reactors operating in continuous mode as carbonation and calciner reactors. We observed a rapid initial attrition of both limestones during the calcination step which was then followed by a highly stable period (up to 140 h of added circulation for one of the limestones) during which particle size changes were negligible. This is consistent with previous observations of attrition in other systems that employ these materials. However, a comparison of the attrition model constants with the data reported in the literature showed the two limestones to be particularly fragile during the initial calcination and the first few hours of circulation. Thus, a careful choice of limestone based on its attrition properties must be taken into account in designing future carbonate looping systems.  相似文献   

14.
Carbonation of fly ash in oxy-fuel CFB combustion   总被引:1,自引:0,他引:1  
Chunbo Wang  Yewen Tan 《Fuel》2008,87(7):1108-1114
Oxy-fuel combustion of fossil fuel is one of the most promising methods to produce a stream of concentrated CO2 ready for sequestration. Oxy-fuel FBC (fluidized bed combustion) can use limestone as a sorbent for in situ capture of sulphur dioxide. Limestone will not calcine to CaO under typical oxy-fuel circulating FBC (CFBC) operating temperatures because of the high CO2 partial pressures. However, for some fuels, such as anthracites and petroleum cokes, the typical combustion temperature is above 900 °C. At CO2 concentrations of 80-85% (typical of oxy-fuel CFBC conditions with flue gas recycle) limestone still calcines, but when the ash cools to the calcination temperature, carbonation of fly ash deposited on cool surfaces may occur. This phenomenon has the potential to cause fouling of the heat transfer surfaces in the back end of the boiler, and to create serious operational difficulties. In this study, fly ash generated in a utility CFBC boiler was carbonated in a thermogravimetric analyzer (TGA) under conditions expected in an oxy-fuel CFBC. The temperature range investigated was from 250 to 800 °C with CO2 concentration set at 80% and H2O concentrations at 0%, 8% and 15%, and the rate and the extent of the carbonation reaction were determined. Both temperature and H2O concentrations played important roles in determining the reaction rate and extent of carbonation. The results also showed that, in different temperature ranges, the carbonation of fly ash displayed different characteristics: in the range 400 °C < T ? 800 °C, the higher the temperature the higher the CaO-to-carbonate conversion ratio. The presence of H2O in the gas phase always resulted in higher CaO conversion ratio than that obtainable without H2O. For T ? 400 °C, no fly ash carbonation occurred without the presence of H2O in the gas phase. However, on water vapour addition, carbonation was observed, even at 250 °C. For T ? 300 °C, small amounts of Ca(OH)2 were found in the final product alongside CaCO3. Here, the carbonation mechanism is discussed and the apparent activation energy for the overall reaction determined.  相似文献   

15.
Sharon Sjostrom  Holly Krutka 《Fuel》2010,89(6):1298-27
Processes based upon solid sorbents are currently under consideration for post-combustion CO2 capture. Twenty-four different sorbent materials were examined on a laboratory scale in a cyclic temperature swing adsorption/regeneration CO2 capture process in simulated coal combustion flue gas. Ten of these materials exhibited significantly lower theoretical regeneration energies compared to the benchmark aqueous monoethanolamine, supporting the hypothesis that CO2 capture processes based upon solids may provide cost benefits over solvent-based processes. The best performing materials were tested on actual coal-fired flue gas. The supported amines exhibited the highest working CO2 capacities, although they can become poisoned by the presence of SO2. The carbon-based materials showed excellent stability but were generally categorized as having low CO2 capacities. The zeolites worked well under dry conditions, but were quickly poisoned by the presence of moisture. Although no one type of material is without concerns, several of the materials tested have theoretical regeneration energies significantly lower than that of the industry benchmark, warranting further development research.  相似文献   

16.
Australia's Commonwealth Scientific and Industrial Research Organization (CSIRO) and Delta Electricity have developed, commissioned and operated an A$7 million aqueous NH3 based post-combustion capture (PCC) pilot plant at the Munmorah black coal fired power station in Australia. The results from the pilot plant trials will be used to address the gap in know-how on application of aqueous NH3 for post-combustion capture of CO2 and other pollutants in the flue gas and explore the potential of the NH3 process for application in the Australia power sector. This paper is one of a series of publications to report and discuss the experimental results obtained from the pilot plant trials and primarily focuses on the absorption section.The pilot plant trials have confirmed the technical feasibility of the NH3 based capture process. CO2 removal efficiency of more than 85% can be achieved even with low NH3 content of up to 6 wt%. The NH3 process is effective for SO2 but not for NO in the flue gas. More than 95% of SO2 in the flue gas is removed in the pre-treatment column using NH3. The mass transfer coefficients for CO2 in the absorber as functions of CO2 loading and NH3 concentration have been obtained based on pilot plant data.  相似文献   

17.
Calcium looping processes for capturing CO2 from large emissions sources are based on the use of CaO particles as sorbent in circulating fluidized‐bed (CFB) reactors. A continuous flow of CaO from an oxyfired calciner is fed into the carbonator and a certain inventory of active CaO is expected to capture the CO2 in the flue gas. The circulation rate and the inventory of CaO determine the CO2 capture efficiency. Other parameters such as the average carrying capacity of the CaO circulating particles, the temperature, and the gas velocity must be taken into account. To investigate the effect of these variables on CO2 capture efficiency, we used a 6.5 m height CFB carbonator connected to a twin CFB calciner. Many stationary operating states were achieved using different operating conditions. The trends of CO2 capture efficiency measured are compared with those from a simple reactor model. This information may contribute to the future scaling up of the technology. © 2010 American Institute of Chemical Engineers AIChE J, 57: 000–000, 2011  相似文献   

18.
Application of new solvents will substantially contribute to the reduction of the energy demand for the post combustion capture of CO2 from power plant flue gases. The present work describes tests of such new solvents in a gas-fired pilot plant, which comprises the complete absorption/desorption process (column diameters 0.125 m, absorber/desorber packing height 4.25/2.55 m, packing type: Sulzer BX 500, flue gas flow 30–100 kg/h, CO2 partial pressure 35–135 mbar). Two new solvents CESAR1 (0.28 g/g 2-amino-2-methyl-1-propanol+0.17 g/g piperazine+0.55 g/g H2O) and CESAR2 (0.32 g/g 1, 2-ethanediamine+0.68 g/g H2O), which were developed in an EU-project, were systematically studied and compared to MEA (0.3 g/g monoethanolamine+0.7 g/g H2O). The two new solvents and MEA were studied in the same way in the pilot plant and detailed results are reported for all solvents. In the present study the structured packing Sulzer BX 500 is used. The measurements are carried out at a constant CO2 removal rate of 90% by an adjustment of the regeneration energy in the desorber for systematically varied solvent flow rates. An optimal solvent flow rate leading to a minimum energy requirement is found from these studies. Direct comparisons of such results can be misleading if there are differences in the kinetics of the different solvent systems. The influence of kinetic effects is experimentally studied by varying the flue gas flow rate at a constant ratio of solvent mass flow to flue gas mass flow and constant CO2 removal rate. Results from these studies indicate similar kinetics for CESAR1, CESAR2 and MEA. The direct comparison of the pilot plant results for these solvents is therefore justified. Both CESAR1 and CESAR2 show improvements compared to MEA. The most promising is CESAR1 with a reduction of about 20% in the regeneration energy and 45% in the solvent flow rate.  相似文献   

19.
A highly efficient technique of contaminant gas reduction, Turbulent Contact Absorber (TCA), is applied to CO2 removal from a typical flue gas. Aqueous K2CO3 sorbent was evaluated as a regenerable sorbent for CO2 from the flue gas. In order to identify the system, momentum and mass balance equations were written for the TCA tower. A flat plate falling film model was employed to simulate the TCA tower and the effect of turbulence was included in mass and momentum transfer coefficients. To check the accuracy of the model, a pilot scale TCA was built and operated. A Testo type gas analyzer was used to detect gas concentrations at the inlet and outlet of the rig. The model was validated successfully with pilot plant data. The effect of velocity and K2CO3 concentration on the TCA performance has also been carried out. It was found that the bed pressure drop increases linearly with gas velocity and then remains constant. An increase in the liquid flow rate increases liquid holdup, which leads to a rise in bed pressure drop. Higher turbulence within the TCA causes a velocity peak to shift from hypothetical gas‐liquid interface towards the falling film plate. An increase of the K2CO3 concentration from 1.0 g mol/L to 2.0 g mol/L was found to give an increase in CO2 removal by about 4 %.  相似文献   

20.
Oxyfuel boiler design in a lignite-fired power plant   总被引:1,自引:0,他引:1  
E. Kakaras  D. Giannakopoulos  I. Vorrias 《Fuel》2007,86(14):2144-2150
In the context of CO2 capture and storage, the oxyfuel technology provides a promising option applicable in centralised power production schemes. This technology is based on combustion with pure oxygen instead of air and the flue gas mainly consists of CO2 and H2O. The work presented in this paper is focused in the application of the oxyfuel technology in a lignite-fired power plant. Significant design issues are the required extended flue gas recirculation in order to provide the ballasting effect of the absent N2 and moderate the furnace temperatures. Therefore, a modified design of heat exchange surfaces of the oxyfuel steam boiler was formulated and was compared to a conventional air-fired boiler. A typical modern Greek air-fired power plant has been used as reference. The dominating factors that affect the dimensioning of the oxyfuel boiler are the higher radiative heat transfer - due to the high concentrations of CO2 and H2O in the flue gas - and the different flue gas mass flow, compared to a conventional air-fired boiler. For the determination of the thermodynamic cycle characteristics, simulations were made with the use of a thermodynamic cycle calculation software [Stamatelopoulos GN. Calculation and optimisation of power plant thermodynamic cycles, VDI-Regulations, Series 6, Nr. 340. Braunchweig, Mechanical Engineering Department; 1996 [in German]].  相似文献   

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