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1.
In this work, CO2 capture and H2 production during the steam gasification of coal integrated with CO2 capture sorbent were investigated using a horizontal fixed bed reactor at atmospheric pressure. Four different temperatures (650, 675, 700, and 750 °C) and three sorbent-to-carbon ratios ([Ca]/[C] = 0, 1, 2) were studied. In the absence of sorbent, the maximum molar fraction of H2 (64.6%) and conversion of coal (71.3%) were exhibited at the highest temperature (750 °C). The experimental results verified that the presence of sorbent in the steam gasification of coal enhanced the molar fraction of H2 to more than 80%, with almost all CO2 was fixed into the sorbent structure, and carbon monoxide (CO) was converted to H2 and CO2 through the water gas shift reaction. The steam gasification of coal integrated with CO2 capture largely depended on the reaction temperature and exhibited optimal conditions at 675 °C. The maximum molar fraction of H2 (81.7%) and minimum CO2 concentration (almost 0%) were obtained at 675 °C and a sorbent-to-carbon ratio of 2.  相似文献   

2.
In this study, the continuous sorption-enhanced steam reforming of glycerol to high-purity hydrogen production by a simultaneous flow concept of catalyst and sorbent for reaction and regeneration using two moving-bed reactors has been evaluated experimentally. A Ni-based catalyst (NiO/NiAl2O4) and a lime sorbent (CaO) were used for glycerol steam reforming with and without in-situ CO2 removal at 500 °C and 600 °C. The simultaneous regeneration of catalyst and sorbent was carried out with the mixture gas of N2 and steam at 900 °C. The product gases were measured by a GC gas analyzer. It is obvious that the amounts of CO2, CO and CH4 were reduced in the sorption-enhanced steam reforming of glycerol, and the H2 concentration is greatly increased in the pre-CO2 breakthrough periods within 10 min both 500 °C and 600 °C. The extended time of operation for high-purity hydrogen production and CO2 capture was obtained by the continuous sorption-enhanced steam reforming of glycerol. High-purity H2 products of 93.9% and 96.1% were produced at 500 °C and 600 °C and very small amounts of CO2, CH4 and CO were formed. The decay in activity during the continuous reaction-regeneration of catalyst and sorbent was not observed.  相似文献   

3.
This communication reports conversion phenomena in which CO2 and H2O gases are transformed into CO and H2, respectively, when exposed to a mixture of molten CaO-rich metallurgical slag and V2O3-rich gasifier slag. On reaction, CO2 and H2O are thermodynamically driven to become CO and H2, respectively, by giving up oxygen over the formation of calcium orthovanadate in the slag. The concept was experimentally investigated with a synthetic slag heated to 1500 °C (an assumed slag tap-out temperature in the metallurgical industry) in a CO2 saturated atmosphere. On heating, a rapid drop in oxygen partial pressure occurred between 1405 °C and 1460 °C, where 97% of CO2 transformed to CO. Potential industrial applications with the H2O-to-H2 conversion are then explored using detailed process computations. If the process is made economically viable, CO2 and H2O could be converted into products that are environmentally and industrially attractive and that have the potential for energy savings and greenhouse gas reduction in a process.  相似文献   

4.
As generation of carbon dioxide (CO2) greenhouse gas is inherent in the combustion of fossil fuels, effective capture of CO2 from industrial and commercial operations is viewed as an important strategy which has the potential to achieve a significant reduction in atmospheric CO2 levels. At present, there are three basic capture methods, i.e. post combustion capture, pre-combustion capture and oxy-fuel combustion. In pre-combustion, the fossil fuel is reacted with air or oxygen and is partially oxidized to form CO and H2. Then it is reacted with steam to produce a mixture of CO2 and more H2. The H2 can be used as fuel and the carbon dioxide is removed before combustion takes place. Oxy-combustion is when oxygen is used for combustion instead of air, which results in a flue gas that consists mainly of pure CO2 and is potentially suitable for storage. In post combustion capture, CO2 is captured from the flue gas obtained after the combustion of fossil fuel. The post combustion capture (PCC) method eliminates the need for substantial modifications to existing combustion processes and facilities; hence, it provides a means for near-term CO2 capture for new and existing stationary fossil fuel-fired power plants.This paper briefly reviews CO2 capture methods, classifies existing and emerging post combustion CO2 capture technologies and compares their features. The paper goes on to investigate relevant studies on carbon fibre composite adsorbents for CO2 capture, and discusses fabrication parameters of the adsorbents and their CO2 adsorption performance in detail. The paper then addresses possible future system configurations of this process for commercial applications.Finally, while there are many inherent attractive features of flow-through channelled carbon fibre monolithic adsorbents with very high CO2 adsorption capabilities, further work is required for them to be fully evaluated for their potential for large scale CO2 capture from fossil fuel-fired power stations.  相似文献   

5.
Chemical looping combustion (CLC) has been suggested as an energy-efficient method for the capture of carbon dioxide from combustion. It is indirect combustion by the use of an oxygen carrier, which can be used for CO2 capture in power-generating processes. The possibility of CLC using a calcium-based oxygen carrier is investigated in this paper. In the air reactor air is supplied to oxidize CaS to CaSO4, where oxygen is transferred from air to the oxygen carrier; the reduction of CaSO4 to CaS takes place in the fuel reactor. The exit gas from the fuel reactor is CO2 and H2O. After condensation of water, almost pure CO2 could be obtained. The thermodynamic and kinetic problem of the reduction reactions of CaSO4 with CO and H2 and the oxidization reactions of CaS with O2 is discussed in the paper to investigate the technique possibility. To prevent SO2 release from the process of chemical looping combustion using a calcium-based oxygen carrier, thermochemical CaSO4 reduction and CaS oxidation are discussed. Thermal simulation experiments are carried out using a thermogravimetric analyzer (TGA). The properties of the products are characterized by Fourier transform infrared (FT-IR) spectroscopy and X-ray diffractometry (XRD), and the optimal reaction parameters are evaluated. The effects of reaction temperature, reductive gas mixture, and oxygen partial pressure on the composition of flue gas are discussed. The suitable temperature of the air reactor is between 1050 and 1150 °C and the optimal temperature of the fuel reactor between 900 and 950 °C.  相似文献   

6.
Steam methane reforming (SMR) is currently the main hydrogen production process in industry, but it has high emissions of CO2, at almost 7 kg CO2/kg H2 on average, and is responsible for about 3% of global industrial sector CO2 emissions. Here, the results are reported of an investigation of the effect of steam-to-carbon ratio (S/C) on CO2 capture criteria from various locations in the process, i.e. synthesis gas stream (location 1), pressure swing adsorber (PSA) tail gas (location 2), and furnace flue gases (location 3). The CO2 capture criteria considered in this study are CO2 partial pressure, CO2 concentration, and CO2 mass ratio compared to the final exhaust stream, which is furnace flue gases. The CO2 capture number (Ncc) is proposed as measure of capture favourability, defined as the product of the three above capture criteria. A weighting of unity is used for each criterion. The best S/C ratio, in terms of providing better capture option, is determined. CO2 removal from synthesis gas after the shift unit is found to be the best location for CO2 capture due to its high partial pressure of CO2. However, furnace flue gases, containing almost 50% of the CO2 in produced in the process, are of great significance environmentally. Consequently, the effects of oxygen enrichment of the furnace feed are investigated, and it is found that this measure improves the CO2 capture conditions for lower S/C ratios. Consequently, for an S/C ratio of 2.5, CO2 capture from a flue gas stream is competitive with two other locations provided higher weighting factors are considered for the full presence of CO2 in the flue gases stream. Considering carbon removal from flue gases, the ratio of hydrogen production rate and Ncc increases with rising reformer temperature.  相似文献   

7.
This paper investigates the integrated catalytic adsorption (ICA) steam gasification of palm kernel shell for hydrogen rich gas production using pilot scale fluidized bed gasifier under atmospheric condition. The effect of temperature (600–750 °C) and steam to biomass ratio (1.5–2.5 wt/wt) on hydrogen (H2) yield, product gas composition, gas yield, char yield, gasification and carbon conversion efficiency, and lower heating values are studied. The results show that H2 hydrogen composition of 82.11 vol% is achieved at temperature of 675 °C, and negligible carbon dioxide (CO2) composition is observed at 600 °C and 675 °C at a constant steam to biomass ratio of 2.0 wt/wt. In addition, maximum H2 yield of 150 g/kg biomass is observed at 750 °C and at steam to biomass ratio of 2.0 wt/wt. A good heating value of product gas which is 14.37 MJ/Nm3 is obtained at 600 °C and steam to biomass ratio of 2.0 wt/wt. Temperature and steam to biomass ratio both enhanced H2 yield but temperature is the most influential factor. Utilization of adsorbent and catalyst produced higher H2 composition, yield and gas heating values as demonstrated by biomass catalytic steam gasification and steam gasification with in situ CO2 adsorbent.  相似文献   

8.
Steam gasification of a typical Chinese bituminous coal for hydrogen production in a lab-scale pressurized bubbling fluidized bed with CaO as CO2 sorbent was performed over a pressure range of ambient pressure to 4 bar. The compositions of the product gases were analyzed and correlated to the gasification operating variables that affecting H2 production, such as pressure (P), mole ratio of steam to carbon ([H2O]/[C]), mole ratio of CaO to carbon ([CaO]/[C]) and temperature (T). The experimental results indicated that the H2 concentration was enhanced by raising the temperature, pressure and [H2O]/[C] under the circumstances we observed. With the presence of CaO sorbent, CO2 in the production gas was absorbed and converted to solid CaCO3, thus shifting the steam reforming of hydrocarbons and water gas shift reaction beyond the equilibrium restrictions and enhancing the H2 concentration. H2 concentration was up to 78 vol% (dry basis) under a condition of 750 °C, 4 bar, [Ca]/[C] = 1 and [H2O]/[C] = 2, while CO2 (2.7 vol%) was almost in-situ captured by the CaO sorbent. This study demonstrated that CaO could be used as a substantially excellent CO2 sorbent for the pressurized steam gasification of bituminous coal. For the gasification process with the presence of CaO, H2-rich syngas was yielded at far lower temperatures and pressures in comparison to the commercialized coal gasification technologies. SEM/EDX and gas sorption analyses of solid residues sampled after the gasification showed that the pore structure of the sorbent was recovered after the steam gasification process, which was attributed to the formation of Ca(OH)2. Additionally, a coal-CaO–H2O system was simulated with using Aspen Plus software. Calculation results showed that higher temperatures and pressures favor the H2 production within a certain range.  相似文献   

9.
Blast furnace (BF) is a large-scale reactor for producing hot metal where coke and coal are consumed as reducing agent and fuel, respectively. As a result, a large amount of CO2 is liberated into the atmosphere. The blast furnace gas (BFG) and coke oven gas (COG) from the ironmaking process can be used for H2 production in association with carbon capture and storage (CCS), thereby reducing CO2 emissions. In this study thermodynamic analyses are performed to evaluate the feasibility of H2 production from BFG and COG. Through the water gas shift reaction (WGSR) of BFG, almost all CO contained in BFG can be converted for H2 production if the steam/CO (S/C) ratio is no less than unity and the temperature is at 200 °C, regardless of whether CO2 is captured or not. The maximum H2 production from WGSR is around 0.21 Nm3 (Nm3 BFG)−1. Regarding H2 production from COG, a two-stage reaction of partial oxidation (POX) followed by WGSR is carried out. It is found the proper conditions for syngas formation from the POX of COG is at the oxygen/fuel (O/F) ratio of 0.5 and the temperature range of 1000-1750 °C where the maximum syngas yield is 2.83 mol (mol hydrocarbons)−1. When WGSR is subsequently applied, the maximum H2 production from the two-stage reaction can reach 0.83 Nm3 (Nm3 COG)−1.  相似文献   

10.
This paper presents results of thermodynamic analysis and experimental evaluation of hydrogen production by steam reforming of ethanol (SRE) combined with CO2 absorption using a mixture of a solid absorbent (CaO, CaO*MgO and Na2ZrO3) and a Ni/Al2O3 catalyst. Thermodynamic analysis results indicate that a maximum of 69.5% H2 (dry basis) is feasible at 1 atm, H2O/C2H5OH = 6 (molar ratio) and T = 600 °C. whereas, the addition of a CO2 absorbent at 1 atm, T = 600 °C and H2O/C2H5OH/Absorbent = 6:1:2.5, produced a H2 concentration of 96.6, 94.1, and 92.2% using CaO, CaO*MgO, and Na2ZrO3, respectively. SRE experimental evaluation achieved a maximum of 60% H2. While combining SRE and a CO2 absorbent exhibited a concentration of 96, 94, and 90% employing CaO, CaO*MgO, and Na2ZrO3, respectively at 1 atm, T = 600 °C, SV = 414 h−1 and H2O/C2H5OH/absorbent = 6:1:2.5 (molar ratio).  相似文献   

11.
Molten carbonate fuel cells (MCFC) used as carbon dioxide separation units in integrated fuel cell and conventional power generation can potentially reduce carbon emission from fossil fuel power production. The MCFC can utilize CO2 in combustion flue gas at the cathode as oxidant and concentrate it at the anode through the cell reaction and thereby simplifying capture and storage. However, combustion flue gas often contains sulfur dioxide which, if entering the cathode, causes performance degradation by corrosion and by poisoning of the fuel cell. The effect of contaminating an MCFC with low concentrations of both SO2 at the cathode and H2S at the anode was studied. The poisoning mechanism of SO2 is believed to be that of sulfur transfer through the electrolyte and formation of H2S at the anode. By using a small button cell setup in which the anode and cathode behavior can be studied separately, the anodic poisoning from SO2 in oxidant gas can be directly compared to that of H2S in fuel gas. Measurements were performed with SO2 added to oxidant gas in concentrations up to 24 ppm, both for short-term (90 min) and for long-term (100 h) contaminant exposure. The poisoning effect of H2S was studied for gas compositions with high- and low concentration of H2 in fuel gas. The H2S was added to the fuel gas stream in concentrations of 1, 2 and 4 ppm. Results show that the effect of SO2 in oxidant gas was significant after 100 h exposure with 8 ppm, and for short-term exposure above 12 ppm. The effect of SO2 was also seen on the anode side, supporting the theory of a sulfur transfer mechanism and H2S poisoning. The effect on anode polarization of H2S in fuel gas was equivalent to that of SO2 in oxidant gas.  相似文献   

12.
The kinetics of the water-gas shift (WGS) reaction over a novel La0.7Ce0.2FeO3 perovskite-like catalyst is investigated using simulated coal-derived syngas at temperatures of 550 °C and 600 °C which are higher than the maximum operating temperature limit for conventional high temperature WGS catalysts. The influences of CO, CO2, H2O and H2 concentration on WGS reaction rate are determined using selected gas compositions that might be encountered in a coal-based gasification system. An empirical power-law rate model used in this study is found to correlate well with experimental data with good accuracy. Kinetics parameters over La0.7Ce0.2FeO3 obtained in this study are mostly in agreement with those previously measured using Fe-Cr based commercial catalysts in a range of relatively lower temperatures (300-500 °C).  相似文献   

13.
Solid sorbents can be used to capture CO2 from pre-combustion sources at various temperatures. MgO and CaO are typical medium- and high-temperature CO2 sorbents. However, pure MgO is not active toward CO2. The addition of Na2CO3 increases the operating temperature and significantly increases the reactivity of sorbents to capture CO2. Na2CO3-promoted MgO is a promising medium-temperature CO2 sorbent. In this study, the thermodynamic performance of integrated gasification combined cycle (IGCC) systems with Na2CO3–MgO-based warm gas decarbonation (WGDC) and CaO-based hot gas decarbonation (HGDC) is evaluated and compared with that of an IGCC system with methyldiethanolamine (MDEA)-based cold gas decarbonation (CGDC). Assuming that the average CO2 capture capacities of solid sorbents are one-third of their theoretical maxima, we reveal that the IGCC system undergoes approximately 2.8% and 3.6% improvement on net efficiency when switching from CGDC to WGDC and to HGDC, respectively. The net efficiency of the system is increased by improving the CO2 capture capacity of the sorbent. The IGCC with Na2CO3–MgO experiences more significant increase in efficiency than that with CaO along with the improvement of sorbent average CO2 capture capacity. The efficiency of the IGCC systems reaches the same value when the average CO2 capture capacities of both sorbents are 53% of their theoretical levels. The effects of gas turbine combustor fuel gas inlet temperature on IGCC system performance are analyzed. Results show that the efficiency of the IGCC systems with HGDC and WGDC increases by 0.74% and 0.53% respectively as the fuel gas inlet temperature increases from 250 °C to 650 °C.  相似文献   

14.
High- and low- temperature behaviors of La0.6Sr0.4Co0.2Fe0.8O3−δ (LSCF) cathode for solid oxide fuel cells operating under CO2/H2O-containing atmosphere are investigated. LSCF shows different stability against CO2 and H2O at high and low temperature. LSCF has excellent electrochemical performance and high stability against the corrosion of CO2 and H2O at 750 °C due to weak reactivity of LSCF with CO2. LSCF shows a serious degradation at 600 °C under operation with O2–CO2(2.83%)–H2O(2.64%), which is ascribed to the impeded oxygen activation and oxygen surface diffusion by surface carbonates and SrCO3 phases on LSCF surface. Under CO2(5%)–H2O(2.81%)–He, LSCF reacts with CO2 to yield SrCO3 phases in 400–680 °C, and H2O aggravates the chemical reaction between CO2 and LSCF. Taking into account of SrCO3 phase formation on LSCF, LSCF cathode is stable under operation with O2–CO2(2.83%)–H2O(2.64%) in 680–800 °C, whereas it is unstable below 680 °C. LSCF can be subject to degradation caused by CO2 and H2O in air during long-term operation below 680 °C.  相似文献   

15.
AEWGS is a reaction that combines the WGS reaction and CO2 capture by a solid absorbent to produce high purity H2 from synthesis gas in one single step at 600–800 °C. This reactor system, if homogeneous, would not require a catalyst. However, previous research on this concept was not conclusive, since a steel reactor was used and reactor walls were suspected to act as catalyst. Therefore, there is a need to address this issue and to select and evaluate suitable CO2 absorbents for this concept. AEWGS was studied using a quartz-made fixed-bed reactor at; SV = 3000 h−1, feed; 5% CO, 15% H2O, balance He–N2 at 600 °C, 1 atm. CO2 absorbents tested were CaO*MgO, and Na2ZrO3. Empty quartz-reactor tests leaded to conclude that a catalyst is needed for the WGS at temperatures of interest. A 97% H2 product was obtained with calcined dolomite suggesting this last to act as a WGS catalyst.  相似文献   

16.
Nowadays, research aims to produce H2 efficiently through modifying conventional processes by removing CO2 at high temperature (T ≥ 500 °C). The sorption enhanced reforming (SER) is an example of such a process where CO2 capture offers significant energy savings (≈23%). Besides, feedstock to this process may include different sources of biofuels. An essential part of this new reaction system is the use of a solid CO2 absorbent. Among absorbents stands lithium orthosilicate (Li4SiO4) for its high absorption capacity and thermal stability. Therefore, the present research aims to study and model the kinetics of CO2 absorption by Li4SiO4 in a temperature range of 550–650 °C. Results were consistent with a first order reaction dependence with respect to CO2 concentration. Apparent activation energy of the gas–solid reaction (22.5 kcal/mol) is approximately equal the intrinsic activation energy (28.6 kcal/mol), suggesting that the surface reaction resistance determines the overall reaction rate.  相似文献   

17.
MFI zeolite membranes were synthesized on porous α-alumina hollow fibers by in-situ hydrothermal synthesis. The membranes were further modified for H2 separation by on-stream catalytic cracking deposition of methyldiethoxysilane (MDES) in the zeolitic pores. The separation performance of the modified membranes was characterized by separation of H2/CO2 gas mixture at 500 °C. Activation of MFI zeolite membranes by air at 500 °C was found to promote catalytic cracking deposition of silane in the zeolitic pores effectively, which resulted in significant improvement of H2-separating performance. The H2/CO2 separation factor of 45.6 with H2 permeance of 1.0 × 10−8 mol m−2 s−1 Pa−1 was obtained at 500 °C for a modified hollow fiber MFI zeolite membrane. The as-made membranes showed good thermochemical stability for the separation of H2/CO2 gas mixture containing H2O and H2S, respectively.  相似文献   

18.
Numerous furnaces and boilers are extensively used in industrial and commercial facilities to generate thermal energy so that small improvements of the furnace thermal efficiency will amount to tremendous reduction of energy consumption and green gas emission. In this research, the furnace flue damper angle is adjusted to lower the pressure in the furnace for reducing the velocity of hot gas rising in the furnace. This allows more time for the heat to be transferred to the thermal flow that improves the furnace overall thermal efficiency. On the other hand, when the damper angle is adjusted from 45 to 39°, the pressure in the furnace rises from −14.7 to −9.3 mmH2O, the average fuel volumetric flow rate reduces from 751 to 491 m3/h, and the average temperature lowers from 949 to 909 °C in the radiation section and from 756 to 798 °C in the conventional section. Hence, about 1.7 × 106 m3 of fuel gas consumption can be saved, and 1.9 × 103 ton of CO2 emission can be reduced annually. The results confirm that simply by adjusting the flue damper angle of a furnace will achieve significant savings of energy and reduction of carbon dioxide emission.  相似文献   

19.
The synergistic effect of Ca(OH)2 prepared by the wet-mixing method on lignite steam gasification process at different temperatures (700–900 °C) was analyzed in a spout-fluid bed reactor. Firstly, to avoid disturbance of volatile and tar, active carbon was used as a model compound. On the one hand, Ca(OH)2 effectively catalyzed the water-gas shift (WGS) reaction to improve H2 concentration, but the performance was weaker at higher temperature due to the enhancement of boudouard reaction and the weakening of WGS reaction. On the other hand, it was found that the (CO+2CO2)/H2 ratio of syngas produced at 700 °C in the presence of Ca(OH)2 was 0.82, which was much lower than that of the other cases, owning to the absorption of CO2. The synergistic effect was observed at this temperature, for the adsorption of CO2 altered equilibrium of the WGS reaction and further improved H2 concentration. Then two kinds of Chinese lignite (HLH and XM) were selected to further study the performance of Ca(OH)2 on optimizing the lignite steam gasification process. In the presence of Ca(OH)2, tar and char yields greatly reduced at the same reaction temperature, whereas the gas yields significantly increased. As a catalyst, Ca(OH)2 can not only promote solid–gas reaction to decrease char yield, but also accelerate tar decomposition to reduce its yield in syngas. Based on GC–MS data, it can be deduced that Ca(OH)2 has different catalytic activity on the steam reforming of tar with different molecular structures. Contrast to Class 4, tars of aliphatic hydrocarbons, Class 2 and Class 5 were clearly catalytic reformed. Hydrogen-rich gas can be produced at 800 °C and 900 °C owning to the catalytic effect of Ca(OH)2, but the highest H2 concentration was found at 700 °C due to the additional effect of CO2 absorption, which was supported by the results of thermogravity experiments.  相似文献   

20.
The paper presents an experimental investigation of using a Molten Carbonate Fuel Cell (MCFC) to reduce CO2 emission from the flue gas of a lignite fired boiler. The MCFC is placed in the flue gas stream and separates CO2 from the cathode side to the anode side. As a result, a mixture of CO2 and H2O is obtained from which pure CO2 can be obtained through condensation of water and carbon dioxide. The main advantages of this solution are: additional electricity generated, reduced CO2 emissions and higher system efficiency. The results obtained show that the use of an MCFC could reduce CO2 emissions by 90% with over 30% efficiency in additional power generation.  相似文献   

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