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1.
Chemical-looping combustion (CLC) is a promising technology for the combustion of gas or solid fuel with efficient use of energy and inherent separation of CO2. The technique involves the use of an oxygen carrier which transfers oxygen from combustion air to the fuel, and hence a direct contact between air and fuel is avoided. A chemical-looping combustion system consists of a fuel reactor and an air reactor. A metal oxide is used as oxygen carrier that circulates between the two reactors. The air reactor is a high velocity fluidized bed where the oxygen carrier particles are transported together with the air stream to the top of the air reactor, where they are then transferred to the fuel reactor using a cyclone. The fuel reactor is a bubbling fluidized bed reactor where oxygen carrier particles react with hydrocarbon fuel and get reduced. The reduced oxygen carrier particles are transported back to the air reactor where they react with oxygen in the air and are oxidized back to metal oxide. The exhaust from the fuel reactor mainly consists of CO2 and water vapor. After condensation of the water in the exit gas from the fuel reactor, the remaining CO2 gas is compressed and cooled to yield liquid CO2, which can be disposed of in various ways.With the improvement of numerical methods and more advanced hardware technology, the time needed to run CFD (Computational fluid dynamics) codes is decreasing. Hence multiphase CFD-based models for dealing with complex gas-solid hydrodynamics and chemical reactions are becoming more accessible. Until now there were a few literatures about mathematical modeling of chemical-looping combustion using CFD approach. In this work, the reaction kinetics model of the fuel reactor (CaSO4 + H2) was developed by means of the commercial code FLUENT. The bubble formation and the relation between bubble formation and molar fraction of products in gas phase were well captured by CFD simulation. Computational results from the simulation also showed low fuel conversion rate. The conversion of H2 was about 34% partially due to fast, large bubbles rising through the reactor, low bed temperature and large particles diameter.  相似文献   

2.
Chemical looping combustion (CLC) is a process in which oxygen required for combustion of a fuel is supplied by the metal oxide. Metal oxide plays the role of an oxygen carrier by providing oxygen for combustion when being reduced and is then re-oxidized by air in a separate reactor. Combustion is thus without any direct contact between air and fuel: as a consequence flue gas does not contain nitrogen of air which simplifies flue gas treatment prior to sequestration. In the present study, biogas combustion was analyzed in a chemical looping combustion fluidized bed reactor. NiAl0.44O1.67 and Cu0.95Fe1.05AlO4 metal oxide particles were used as oxygen carriers. The experiments have shown the feasibility of biogas combustion in chemical looping combustion: CH4 of the biogas was completely converted to CO2 and H2O with a small fraction of CO and H2. The outlet flue gas distribution profile was not affected by ageing during the cycles of reduction and oxidation, indicating the chemical stability of the oxygen carriers. There was limited formation of carbon on the oxygen carriers during reduction.  相似文献   

3.
This paper presents application of the chemical looping combustion (CLC) method in natural gas-fired combined cycles for power generation with CO2 capture. A CLC combined cycle consisting of single CLC-reactor system, an air turbine, a CO2-turbine and a steam cycle has been designated as the base-case cycle. The base-case cycle can achieve net plant efficiency of about 52% at an oxidation temperature of 1200 °C. In order to achieve a reasonable efficiency at lower oxidation temperatures, reheat is introduced into the air turbine by employing multi CLC-reactors. The results show that the single reheat CLC-combined cycle can achieve net plant efficiency of above 51% at oxidation temperature of 1000 °C and above 53% at the oxidation temperature of 1200 °C including CO2 compression to 110 bar. The double reheat cycle results in marginal efficiency improvement as compared to the single reheat cycle. The CLC-cycles are also compared with a conventional combined cycle with and without post-combustion capture in amine solution. All the CLC-cycles show higher net plant efficiencies with close to 100% CO2 capture as compared to a conventional combined cycle with post-combustion capture, which is very promising.  相似文献   

4.
Chemical-looping combustion is a novel combustion technology with inherent separation of the greenhouse gas CO2. The technology uses circulating oxygen carriers to transfer oxygen from the combustion air to the fuel. In this paper, oxygen carriers based on commercially available NiO and α-Al2O3 were prepared using the industrial spray-drying method, and compared with particles prepared by freeze-granulation. The materials were investigated under alternating oxidizing and reducing conditions in a laboratory fluidized bed, thus simulating the cyclic conditions of a chemical-looping combustion system. The particles produced by spray-drying displayed a remarkable similarity to the freeze-granulated oxygen carriers, with high reactivity when the bed was fluidized and similar physical properties when sintered at the same temperature. This is an important result as it shows that the scaling-up from a laboratory production method, i.e. freeze-granulation, to a commercial method suitable for large-scale production, i.e. spray-drying, did not involve any unexpected difficulties. A difference noticed between the spray-dried and freeze-granulated particles was the sphericity. Whereas the freeze-granulated particles showed near perfect sphericity, a large portion of the spray-dried particles had hollow interiors. Defluidization was most likely to occur for highly reduced particles, at low gas velocities. The apparent density and crushing strength of the oxygen carriers could be increased either by increasing the sintering temperature or by increasing the sintering time. However, the fuel conversion was fairly unchanged when the sintering temperature was increased but was clearly improved when the sintering time was increased.  相似文献   

5.
This study presents first operating experience with a 120 kW chemical looping pilot rig. The dual circulating fluidized bed reactor system and its auxiliary units are discussed. Two different oxygen carriers, i.e. ilmenite, which is a natural iron titanium ore, and a designed Ni-based particle, are tested in the CLC unit. The pilot rig is fueled with H2, CO and CH4 respectively at a fuel power of 65–145 kW. High solids circulation, very low solids residence time and low solids inventory are observed during operation. Owing to the scalability of the design concept, these characteristics should be quite similar to those of commercial CLC power plants. Ilmenite shows a high potential for the combustion of H2-rich gases (e.g. from coal gasification with steam). The H2 conversion is quite high but there is still a high potential for further improvement. The Ni-based oxygen carrier achieves the thermodynamic maximum H2 and CO conversion and also very high CH4 conversion. A variation of the air/fuel ratio and the reaction temperature indicates that the Ni/NiO ratio of the particle has an influence on the performance of the chemical looping combustor. Generally, low solids conversion in air and fuel reactors is observed in almost any conditions. Despite a very low H2O/CH4 molar ratio, no carbon formation is observed.  相似文献   

6.
Chemical-looping with oxygen uncoupling (CLOU) is a novel method to burn solid fuels in gas-phase oxygen without the need for an energy intensive air separation unit. The carbon dioxide from the combustion is inherently separated from the rest of the flue gases. CLOU is based on chemical-looping combustion (CLC) and involves three steps in two reactors, one air reactor where a metal oxide captures oxygen from the combustion air (step 1), and a fuel reactor where the metal oxide releases oxygen in the gas-phase (step 2) and where this gas-phase oxygen reacts with a fuel (step 3). In other proposed schemes for using chemical-looping combustion of solid fuels there is a need for an intermediate gasification step of the char with steam or carbon dioxide to form reactive gaseous compounds which then react with the oxygen carrier particles. The gasification of char with H2O and CO2 is inherently slow, resulting in slow overall rates of reaction. This slow gasification is avoided in the proposed process, since there is no intermediate gasification step needed and the char reacts directly with gas-phase oxygen. The process demands an oxygen carrier which has the ability to react with the oxygen in the combustion air in the air reactor but which decomposes to a reduced metal oxide and gas-phase oxygen in the fuel reactor. Three metal oxide systems with suitable thermodynamic properties have been identified, and a thermal analysis has shown that Mn2O3/Mn3O4 and CuO/Cu2O have suitable thermodynamic properties, although Co3O4/CoO may also be a possibility. However, the latter system has the disadvantage of an overall endothermic reaction in the fuel reactor. Results from batch laboratory fluidized bed tests with CuO and a gaseous and solid fuel are presented. The reaction rate of petroleum coke is approximately a factor 50 higher using CLOU in comparison to the reaction rate of the same fuel with an iron-based oxygen carrier in normal CLC.  相似文献   

7.
Nowadays the lab scale feasibility of the chemical looping combustion technology has been proved. This article deals with many of the design requirements that need to be fulfilled to make this technology applicable at industrial scale. A design for a 150 kWth chemical looping combustion reactor system is proposed. In the base case it is supposed to work with gaseous fuels and inexpensive oxygen carriers derived from industrial by-products or natural minerals. More specifically the fuel will be methane and a manganese ore will be the basis for the oxygen carrier. It is a double loop circulating fluidized bed where both the air reactor and the fuel reactor are capable to work in the fast fluidization regime in order to increase the gas solids contact along the reactor body. High operational flexibility is aimed, in this way it will be possible to run with different fuels and oxygen carriers as well as different operating conditions such as variation in air excess. Compactness is a major goal in order to reduce the required solid material and possibly to enclose the reactor body into a pressurized vessel to investigate the chemical looping combustion under pressurized conditions. The mass and heat balance are described, as well as the hydrodynamic investigations performed. Most design solutions presented are taken from industrial standards as one main objective is to meet commercial requirements.  相似文献   

8.
A semi-commercial 10 MWth chemical looping combustion (CLC) plant for power production is proposed as a next scale demonstration plant after successful operation of a 120 kW CLC pilot rig. The design criteria for the CLC boiler are derived from the experience obtained from the CLC pilot rig at Vienna University of Technology. The IPSEpro simulation environment is chosen for implementation of the process flow sheet of the CLC power plant. A single pressure steam cycle is suggested for this small scale demonstration plant. Heat exchangers and a five-stage steam turbine are arranged. Basic design parameters of the power plant are derived from detailed mass and energy investigations and discussed. It turns out that the net electric efficiency of such a small scale plant can be expected to be in the range of 32.5–35.8%. However, a demonstration of CLC at such a scale is necessary in order to gain confidence in more sophisticated CLC power generation concepts at larger scale.  相似文献   

9.
CO2 capture and storage from energy conversion systems is one option for reducing power plant CO2 emissions to the atmosphere and for limiting the impact of fossil-fuel use on climate change. Among existing technologies, chemical looping combustion (CLC), an oxy-fuel approach, appears to be one of the most promising techniques, providing straightforward CO2 capture with low energy requirements.This paper provides an evaluation of CLC technology from an economic and environmental perspective by comparing it with to a reference plant, a combined cycle power plant that includes no CO2 capture. Two exergy-based methods, the exergoeconomic and the exergoenvironmental analyses, are used to determine the economic and environmental impacts, respectively. The applied methods facilitate the iterative optimization of energy conversion systems and lead towards the improvement of the effectiveness of the overall plant while decreasing the cost and the environmental impact of the generated product. For the plant with CLC, a high increase in the cost of electricity is observed, while at the same time the environmental impact decreases.  相似文献   

10.
Fe2O3-containing waste materials from the steel industry are proposed as oxygen carrier for chemical-looping combustion. Three such materials, red iron oxide, brown iron oxide and iron oxide scales, have been examined by oxidation and reduction experiments in a batch fluidized-bed reactor at temperatures between 800 and 950 °C. NiO-based particles have been used as additive, in order to examine if it is possible to utilize the catalytic properties of metallic Ni to facilitate decomposition of hydrocarbons into more reactive combustion intermediates such as CO and H2. The experiments indicated modest reactivity between the waste materials and CH4, which was used as reducing gas. Adding small amounts of NiO-based particles to the sample increased the yield of CO2 in a standard experiment, typically by a factor of 1.5–3.5. The fraction of unconverted fuel typically was reduced by 70–90%. The conversion of CH4 to CO2 was 94% at best, corresponding to a combustion efficiency of 96%. This was achieved using a bed mass corresponding to 57 kg oxygen carrier per MW fuel, of which only 5 wt% was NiO-based synthetic particles. The different materials fared differently well during the experiments. Red iron oxide was fairly stable, while brown iron oxide was soft and subject to considerable erosion. Iron oxide scales experienced increased reactivity and porosity as function of the numbers of reduction cycles.  相似文献   

11.
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 sulphur compounds, such as H2S and COS. This paper presents the combustion results obtained with a Cu-based oxygen carrier using mixtures of CH4 and H2S as fuel. The influence of H2S concentration on the gas product distribution and combustion efficiency, sulphur splitting between the fuel reactor (FR) and the air reactor (AR), oxygen carrier deactivation and material agglomeration was investigated in a continuous CLC plant (500 Wth). The oxygen carrier to fuel ratio, ?, was the main operating parameter affecting the CLC system. Complete fuel combustion were reached at 1073 K working at ? values ≥1.5. The presence of H2S did not produce a decrease in the combustion efficiency even when working with a fuel containing 1300 vppm H2S. At these conditions, the great majority of the sulphur fed into the system was released in the gas outlet of the FR as SO2, affecting to the quality of the CO2 produced. Formation of copper sulphide, Cu2S, and the subsequent reactivity loss was only detected working at low values of ?  1.5, although this fact did not produce any agglomeration problem in the fluidized beds. In addition, the oxygen carrier was fully regenerated in a H2S-free environment. It can be concluded that Cu-based oxygen carriers are adequate materials to be used in a CLC process using fuels containing H2S although quality of the CO2 produced is affected.  相似文献   

12.
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   

13.
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   

14.
A full-scale field study was carried out at two Spanish coal-fired power plants equipped with electrostatic precipitator (ESP) and wet flue gas desulfurisation (FGD) systems to investigate the distribution of boron in coals, solid by-products, wastewater streams and flue gases. The results were obtained from the simultaneous sampling of solid, liquid and gaseous streams and their subsequent analysis in two different laboratories for purposes of comparison. Although the final aim of this study was to evaluate the partitioning of boron in a (co-)combustion power plant, special attention was paid to the analytical procedure for boron determination. A sample preparation procedure was optimised for coal and combustion by-products to overcome some specific shortcomings of the currently used acid digestion methods. In addition boron mass balances and removal efficiencies in ESP and FGD devices were calculated. Mass balance closures between 83 and 149% were obtained. During coal combustion, 95% of the incoming boron was collected in the fly ashes. The use of petroleum coke as co-combustible produced a decrease in the removal efficiency of the ESP (87%). Nevertheless, more than 90% of the remaining gaseous boron was eliminated via the FGD in the wastewater discharged from the scrubber, thereby causing environmental problems.  相似文献   

15.
Chemical-looping combustion, CLC, is a technology with inherent separation of the greenhouse gas CO2. The technique uses an oxygen carrier made up of particulate metal oxide to transfer oxygen from combustion air to fuel. In this work, an oxygen carrier consisting of 60% NiO and 40% NiAl2O4 was used in a 10 kW CLC reactor system for 160 h of operation with fuel. The first 3 h of fuel operation excepted, the test series was accomplished with the same batch of oxygen carrier particles. The fuel used in the experiments was natural gas, and a fuel conversion to CO2 of approximately 99% was accomplished. Combustion conditions were very stable during the test period, except for the operation at sub-stoichiometric conditions. It was shown that the methane fraction in the fuel reactor exit gas was dependent upon the rate of solids circulation, with higher circulation leading to more unconverted methane. The carbon monoxide fraction was found to follow the thermodynamical equilibrium for all investigated fuel reactor temperatures, 660–950 °C. Thermal analysis of the fuel reactor at stable conditions enabled calculation of the particle circulation which was found to be approximately 4 kg/s, MW. The loss of fines, i.e. the amount of elutriated oxygen carrier particles with diameter <45 μm, decreased during the entire test period. After 160 h of operation the fractional loss of fines was 0.00022 h−1, corresponding to a particle life time of 4500 h.  相似文献   

16.
Post-combustion carbonate looping processes are based on the capture of carbon dioxide from the flue gases of an existing power plant in a circulating fluidized bed reactor (CFB) of calcium oxide (the carbonator) particles. The calcination of calcium carbonate in a new oxy-fired CFBC power plant regenerates the sorbent (calcium oxide particles) and obtains high purity carbon dioxide. This communication presents experimental results from a small test facility (30 kWt) operated in continuous mode using two interconnected CFB reactors as carbonator and calciner. Capture efficiencies between 70 and 97% have been obtained under realistic flue gas conditions in the carbonator reactor (temperatures around 650 °C). The similarity between process conditions and those existing in CFBC power plants should allow a rapid scaling up of this technology. The next steps for this process development are also outlined.  相似文献   

17.
Oxy-fuel combustion is considered as one of the most promising technologies for carbon capture and storage (CCS). In this study, a commercial computational fluid dynamics (CFD) code has been employed for the simulation of an air-fired coal combustion and an oxy-fired coal combustion with recycled flue gas in a 1 MWth combustion test facility. Reynolds–averaged Navier–Stokes (RANS) solutions have been obtained for both cases. Results indicate that the CFD code with existing physical sub-models can provide a reasonable prediction for the air-fired combustion. However, the prediction for the oxy-fired case has not been as satisfactory as expected. In order to assess the impact of the turbulence treatment in CFD on the predictions, large eddy simulation (LES) has been performed for oxy-fired case and compared with the results from the RANS simulation and the available experimental data. Although the results suggest that LES can provide a more realistic prediction of the shape and the physical properties of the flame, there has not been significant improvement in the prediction of the temperature. In addition, the complexity of the problem requires more detailed experimental data for the validation of the LES. In order to improve the validity of numerical simulations for design purposes, further modelling improvements for oxy-coal combustion that are necessary for more accurate predictions are addressed. Based on this study, it is envisaged that the complexity in the oxy-coal combustion process requires more detailed analyses of the available physical sub-models.  相似文献   

18.
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   

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.
A stratified sand filter column, operated in recirculation mode and treating synthetic effluent resembling high-strength dairy wastewaters was studied over a 342-d duration. The aim of this paper was to examine the organic, total suspended solids (TSS) and nutrient removal rates of the sand filter, operated in recirculation mode, under incrementally increasing hydraulic and organic loading rates and to propose a field filter-sizing criterion. Best performance was obtained at a system hydraulic loading rate of 10 L m(-2) d(-1); a higher system hydraulic loading rate (of 13.4 L m(-2) d(-1)) caused surface ponding. The system hydraulic loading rate of 10 L m(-2) d(-1) gave a filter chemical oxygen demand (COD), TSS, and total kjeldahl nitrogen (TKN) loading rate of 14, 3.7, and 2.1 g m(-2) d(-1), respectively, and produced consistent COD and TSS removals of greater than 99%, and an effluent NO(3)-N concentration of 42 mg L(-1) (accounting for an 86% reduction in total nitrogen (Tot-N)). As the proportional surface area requirement for the sand filter described in this study is less than the recommended surface area requirement of a free-water surface (FWS) wetland treating an effluent of similar quality, it could provide an economic and sustainable alternative to conventional wetland treatment.  相似文献   

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