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1.
The gasification reaction of Nantong inferior coal was investigated in a laboratory fixed-bed reactor under CO2 and O2/H2O atmospheres. The effects of the bed temperature and inlet-gas concentration on the yields of CO, H2, and CH4 were studied. The effects of coal ash and particle size on the fixed-carbon conversion were also investigated, and kinetic analysis was conducted with a homogeneous model. The product-gas-heating value and fixed-carbon conversion increased when the temperature was increased from 950 °C to 1100 °C under CO2 atmosphere. When the inlet-CO2 concentration was increased from 50 to 100 vol.%, the low heating value of the product gas and carbon conversion ratio slightly increased. During the gasification of inferior coal under the O2/H2O atmosphere, the CO concentration increased rapidly with increasing temperature. The H2 and CH4 concentrations increased initially and then decreased. The maximum gas heating value of 7934 kJ/m3 was obtained under the O2 concentration of 70 vol.% at a bed temperature of 1050 °C. The cold-gas efficiency increased with increasing temperature and became 40.6% and 86.4% at 1100 °C under the CO2 and O2/H2O atmospheres, respectively. The gasification reaction of the Nantong inferior coal strongly depended on the content of inherent inorganic matter. The gasification rates for both the CO2 and O2/H2O atmospheres were independent of the particle size. The activation energy for the CO2 and O2/H2O gasification reactions were 137 and 81 kJ/mol, respectively. The gasification reactions of the Nantong coal, which was performed under two different atmospheres, were compared and the reaction activity of the gasification reaction under CO2 atmosphere was found to be much lower than that under the O2/H2O atmosphere.  相似文献   

2.
The use of petroleum coke as fuel in a 10 kWth chemical-looping combustor   总被引:1,自引:0,他引:1  
Tests were made in a 10 kWth chemical-looping combustor with a petroleum coke as the solid fuel and the oxygen carrier ilmenite, an iron titanium oxide. The fuel reactor is fluidized by steam and the oxygen carrier reacts with the volatiles released as well as the gasification intermediates CO and H2. A constant fuel flow corresponding to a thermal power of 5.8 kW was introduced into the fuel reactor and a total of 11 h of operation was reached. The effects of particle circulation and carbon stripper operation on solid fuel conversion, conversion of gas from the fuel reactor and CO2 capture were investigated. The actual CO2 capture ranged between 60% and 75% while the solid fuel conversion was in the range of 66–78%. The low values of solid fuel conversion reflect loss of char due to low efficiency of the fuel reactor cyclone. The incomplete conversion of the gas from the fuel reactor is expressed as oxygen demand. The oxygen demand corresponds to the fraction of oxygen lacking to achieve full gas conversion and was typically 25%, due to presence of CH4, CO and H2 from the fuel reactor. Typical ratios of CH4, CO and H2 over the total gaseous carbon from the fuel reactor are respectively 5, 10 and 25%. Low loss of non-combustible fines from the system indicates very low attrition of the oxygen carrier.  相似文献   

3.
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   

4.
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   

5.
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   

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.
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   

8.
Density functional theory (DFT) has been used to investigate the reaction pathways with steam reforming of glycerol under cold plasma conditions. Total energies, energy barriers, and reaction enthalpies at 298.15 K have been calculated at the GGA/PW91/DNP level. The calculation shows that, with the presence of steam, the energy barrier of glycerol conversion is reduced and the conversion from glycerol to H2 and CO is promoted under cold plasma conditions. The formation of syngas was through a multi-step pathway via the conversion of OHCH2CHOH, CH2OH, CH2O, HCO,·and CH3, while the recombination of H generated extra H2. The synthesis of hydrocarbons are from the recombination of·CH3,·CH2, and·CH, which could be primarily generated through glycerol dissociation. The structure of glycerol anion was also studied in this work, and it was less stable than the neutral molecule. The route for the formation of OHCH2CHOH·and CH2OH·from glycerol anion is thermodynamically favorable.  相似文献   

9.
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   

10.
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   

11.
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   

12.
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   

13.
Post-combustion CO2 capture remains one of the most-challenging issue to lower CO2 emissions of existing power plants or heavy industry installations because of strong economy and energy efficiency aspects. The major issue comes from CO2 dilution (4% for NGCC and 14% for PC) and the high flow rates to be treated. Furthermore, CO2 purity has to be higher than 95% with recovery at 90%, to match the transportation/injection requirements.The MEA absorption process remains the reference today but its energy consumption (about 3 MJ/kgCO2) and the amine consumption are still challenging drawbacks.The interest of CO2 capture by indirect TSA (Temperature Swing Adsorption) was demonstrated experimentally in a previous work. The aim of this paper is to present the results of a numerical parametric study. Two main parameters are explored: the desorption temperature (100–200 °C) and the purge flow rate (0.1–0.5 Ndm3 min−1). Four performance indicators are evaluated: CO2 purity, recovery, productivity and specific energy consumption.Results show that purity above 95% can be achieved. Keeping the 95% target, it is possible to achieve recovery at 81% with productivity at 57.7 gCO2/kgads h and a specific energy consumption of 3.23 MJ/kgCO2, which is less than for the reference MEA process.Comparison with other adsorption processes exhibits that this process has good potential especially since some improvements are still expected from further research.  相似文献   

14.
Enhanced oil recovery (EOR) through CO2 flooding has been practiced on a commercial basis for the last 35 years and continues today at several sites, currently injecting in total over 30 million tons of CO2 annually. This practice is currently exclusively for economic gain, but can potentially contribute to the reduction of emissions of greenhouse gases provided it is implemented on a large scale. Optimal operations in distributing CO2 to CO2-EOR or enhanced gas recovery (EGR) projects (referred to here collectively as CO2-EHR) on a large scale and long time span imply that intermediate storage of CO2 in geological formations may be a key component. Intermediate storage is defined as the storage of CO2 in geological media for a limited time span such that the CO2 can be sufficiently reproduced for later use in CO2-EHR. This paper investigates the technical aspects, key individual parameters and possibilities of intermediate storage of CO2 in geological formations aiming at large scale implementation of carbon dioxide capture and storage (CCS) for deep emission reduction. The main parameters are thus the depth of injection and density, CO2 flow and transport processes, storage mechanisms, reservoir heterogeneity, the presence of impurities, the type of the reservoirs and the duration of intermediate storage. Structural traps with no flow of formation water combined with proper injection planning such as gas-phase injection favour intermediate storage in deep saline aquifers. In depleted oil and gas fields, high permeability, homogeneous reservoirs with structural traps (e.g. anticlinal structures) are good candidates for intermediate CO2 storage. Intuitively, depleted natural gas reservoirs can be potential candidates for intermediate storage of carbon dioxide due to similarity in storage characteristics.  相似文献   

15.
Carbon dioxide (CO2) injection into saline aquifers is one of the promising options to sequester large amounts of CO2 in geological formations. During as well as after injection of CO2 into an aquifer, CO2 migrates towards the top of the formation due to density differences between the formation brine and the injected CO2. The time scales of CO2 migration towards the top of an aquifer and the fraction of CO2 that is trapped as residual gas depends strongly on the driving forces that are acting on the injected CO2.When CO2 migrates to the top of an aquifer, brine may be displaced downwards in a counter-current flow setting particularly during the injection period. A majority of the published work on counter-current flow settings have reported significant reductions in the associated relative permeability functions as compared to co-current measurements. However, this phenomenon has not yet been considered in the simulation of CO2 storage into saline aquifers.In this paper we study the impact of changes in mobility for the two-phase brine/CO2 system as a result of transitions between co- and counter-current flow settings. We have included this effect in a simulator and studied the impact of the related mobility reduction on the saturation distribution and residual saturation of CO2 in aquifers over relevant time scales. We demonstrate that the reduction in relative permeability in the vertical direction changes the plume migration pattern and has an impact on the amount of gas that is trapped as a function of time. This is to our best knowledge the first attempt to integrate counter-current relative permeability into the simulation of injection and subsequent migration of CO2 in aquifers. The results and analysis presented in this paper are directly relevant to all ongoing activities related to the design of large-scale CO2 storage in saline aquifers.  相似文献   

16.
Ultrasonic experiments were undertaken on CO2 flooded sandstone core samples, both synthetic sandstones and core plugs from the CRC1 CO2 injection well in the Otway Basin, Victoria, South Eastern. Australia. The aim of these laboratory tests was to investigate the effects of CO2 as a pore fluid on the seismo-acoustic response of the sandstone and ultimately to provide an indication of the sensitivity of time-lapse seismic imaging of the eventual CO2/CH4 plume in the Otway, Waarre C formation.The synthetic sandstones were manufactured using both a proprietary calcium in situ precipitation (CIPS) process and a silica cementing technique. Samples were tested in a computer controlled triaxial pressure cell where pore pressures can be controlled independently of the confining pressures. The pressure cell is equipped with ultrasonic transducers housed in the loading platens. Consequently, effective pressures equivalent to those expected in the reservoir can be applied while ultrasonic testing is undertaken. Both compressional, P and shear waves, S were recorded via a digital oscilloscope at a range of effective pressure steps. Pore pressures were varied from 4 MPa to 17 MPa to represent both the gaseous and liquid phase regions of the CO2 phase diagram. Similar experiments were conducted on core plugs from the Waarre C reservoir horizon obtained from the CRC1 injection well, but with an intervening brine-saturated step and in some cases with a CO2/CH4 mix of 80%/20% molar fraction which is representative of the field situation. However, the pore pressure in these experiments was held at 4 MPa. Finally, acoustic impedances and reflection coefficients were calculated for the reservoir using Gassmann theory and the implications for imaging the CO2 plume is discussed.  相似文献   

17.
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   

18.
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   

19.
Adsorption is one of the most promising technologies for reducing CO2 emissions and at present several different types of sorbents are being investigated. The use of sorbents obtained from low-cost and abundant precursors (i.e. solid wastes) appears an attractive strategy to adopt because it will contribute to a reduction not only in operational costs but also in the amount of waste that is dumped and burned in landfills every year. Following on from previous studies by the authors, in this work several carbon-based adsorbents were developed from different carpet wastes (pre-consumer and post-consumer wastes) by chemical activation with KOH at various activation temperatures (600–900 °C) and KOH:char impregnation ratios (0.5:1 to 4:1). The prepared materials were characterised by chemical analysis and gas adsorption (N2, −196 °C; CO2, 0 °C), and tested for CO2 adsorption at temperatures of 25 and 100 °C. It was found that both the type of precursor and the conditions of activation (i.e. impregnation ratios, and activation temperatures), had a huge influence on the microporosity of the resultant samples and their CO2 capture capacities. The carbon-based adsorbent that presented the maximum CO2 capture capacities at 25 and 100 °C (13.8 wt.% and 3.1 wt.%, respectively), was prepared from a pre-consumer carpet waste and was activated at 700 °C using a KOH:char impregnation ratio of 1:1. This sample showed the highest narrow microporosity volume (0.47 cm3 g−1), thus confirming that only pores of less than 1 nm are effective for CO2 adsorption at atmospheric pressure.  相似文献   

20.
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   

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