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1.
This study investigates the module configuration for upscaling CO2 capture capacity to a bench-scale in hydrogen selective Pd-based composite membranes. In order to confirm effective upscaling, four plate-type membranes of two inch diameter were stacked in a newly designed plate-and-frame type module, reaching a total membrane surface area of 6.64 × 10−3 m2 (66.4 cm2). A pure gas test carried out using H2 and He confirmed that there were no effects of module configuration in gas permeation behavior, indicating that the upscale of the separation capacity by numbering-up of membranes using our module design was successful. The CO2 enrichment test was conducted using a 40%CO2 + 60%H2 mixture (i.e. a similar composition for the coal gasifier after both the shift reaction and H2O removal), under high feed pressure and flow rate, i.e. 600–2100 kPa and 0.48–0.72 N m3 h−1. The mixture gas test confirmed that the bench-scale membrane module could enrich 40% of the CO2 at a feed flow rate of 0.48 N m3 h−1 up to 93% with a hydrogen recovery ratio of >90% at 673 K and a total feed pressure of 2100 kPa, i.e. ∼4 times CO2 enrichment capacity of one membrane.  相似文献   

2.
The ability of (dimethyl siloxane) (PDMS) and SAPO 34 membrane modules to separate a H2/CO2 gas mixture was investigated in a continuous permeation system in order to decide if they were suitable to be coupled to a biological hydrogen production process. Permeation studies were carried out at relatively low feed pressures ranging from 110 to 180 kPa. The separation ability of SAPO 34 membrane module appeared to be overestimated since the effect concentration polarization phenomena was not taken into consideration in the permeation parameter estimation. On the other hand, the PDMS membrane was the most suitable to separate the binary gas mixture. This membrane reached a maximum CO2/H2 separation selectivity of 6.1 at 120 kPa of feed pressure. The pressure dependence of CO2 and H2 permeability was not considerable and only an apparent slight decrease was observed for CO2 and H2. The mean values of permeability coefficients for CO2 and H2 were 3285 ± 160 and 569 ± 65 Barrer, respectively. The operational feed pressure found to be more adequate to operate initially the PDMS membrane module coupled to the fermentation system was 180 kPa, at 296 K. In these conditions it was possible to achieve an acceptable CO2/H2 separation selectivity of 5.8 and a sufficient recovery of the CO2 in the permeate stream.  相似文献   

3.
CO2/H2 mixtures, such as integrated gasification combined cycle (IGCC) syngas, were separated via hydrate formation in water-in-oil (W/O) emulsions. The oil phase was composed of diesel and cyclopentane (CP). Span 20 was used to disperse the aqueous phase or hydrate in the oil phase, and tetra-n-butyl ammonium bromide (TBAB) was added to produce a synergistic effect with CP. The experimental results show that the presence of TBAB can remarkably increase the separation ability and improve the flow behavior of the hydrate slurry. The most suitable contents of TBAB in the aqueous phase and water in the emulsion were determined to be 0.29 mol% and 35 vol%, respectively. The maximum separation factor of CO2 over H2 was 103, which is much higher than the literature values for separating CO2/H2 gas mixture via hydrate formation. After a two-stage separation, hydrogen was enriched from 53.2 to 97.8 mol%. The influence of temperature, pressure, and the initial gas–liquid volume ratio on the separation ability and hydrate formation rate were investigated in detail. In addition, a criterion for choosing the suitable operation conditions was suggested based on both phase equilibrium and kinetic factors. Based on this criterion, the suitable operation temperature, pressure, and gas–liquid volume ratio for the separation of CO2/H2 are approximately 270.15 K, 3–5 MPa, and 80–100, respectively.  相似文献   

4.
Separation or purification of tritium isotopes is one of the key technologies in ITER. A set of frontal displacement chromatography (FDC) device was designed and constructed for hydrogen isotopes separation using palladium loading on/in alumina (Pd–Al2O3) as the separation material. The hydrogen isotopes separation experiments were carried out. It was found that deuterium abundance of the product was up to 98.5% and the average separation factor was as high as 64, under the condition of 273 K column temperature and 15 mL(NTP)/min flow rate, for a feed gas of 5%H2-5%D2-90%Ar. The deuterium recovery ratio was 42% in this separation test. The results showed that the separation performance of our FDC device was good by using Pd–Al2O3 as separation materials, and it suggested considerable potential for the applicability of FDC in hydrogen isotopes separation.  相似文献   

5.
Using molecular dynamics (MD) simulations, we investigated the performance of graphenylene membrane with functionalized nanopore in the H2/CH4 separation. In the present work, we studied the impact of functionalized nanopore, system temperature (298, 323, and 348 K), applied difference pressure (up to 2 MPa), and feed composition on the H2/CH4 separation performance. The passage of gas molecules across the nanopore was monitored within the simulations, and the permeance was determined under applied conditions. The results revealed that the size of gas molecules and its interaction with the membrane nanopore are two important factors in the separation performance of H2/CH4 gas mixture. It is also found that H2 molecules can easily pass through the studied membranes, whereas no CH4 molecule was seen in the permeate side, which confirms the ultrahigh selectivity of H2 over CH4. Furthermore, the maximum H2 permeance of 1.95 × 105 GPU through the pore 1 was obtained at 1.5 MPa, which was higher than that of 1.93 × 105 GPU through pore 2. The results also demonstrated that the system temperature doesn't have any effect on the membrane performance. To this end, the permeance of H2 molecules through the studied membranes obviously increased with raising the ration of H2 molecules in the feed composition. Due to high selectivity and permeance, the graphenylene membrane with functionalized nanopore is expected to have promising applications in hydrogen separation from H2/CH4 mixed gas.  相似文献   

6.
The conceptual design of a coal gasification system for the production of hydrogen is undertaken here using the PRO-II Simulation program. The operating conditions for the gasifier were tuned to between 1200 °C–1500 °C, 15 atm–30 atm and to a feed molar ratio of C:H2O:O2 = 1:0.5–1:0.25–0.5. The refinery temperature and pressure were kept at 550 °Cand 24.5 atm. The syngas produced goes to water gas shift (WGS) reactors operated at 400 °C, 24 atm (HTS) and 250 °C, 23.5 atm (LTS). The production of hydrogen was found to be independent of the concentration of steam in the feed. However, when other operating conditions are constant, the hydrogen output changes dramatically with changes to the concentration of O2 in the feed. The optimal operating conditions for the production of hydrogen by the gasification of Drayton coal were found to be: 1500 °C, 25 atm and a feed ratio C:H2O:O2 = 1:0.58:0.43.  相似文献   

7.
Supported carbon membranes have been regarded as more competitive than traditional gas separation materials due to the versatile combination of different pyrolyzable polymers and supports which in turn leads to high separation factors and mechanical stability. In order to determine the extent to which supported carbon membranes are more competitive, the transport mechanism of supported carbon membranes was investigated in the range 32–150 °C and 1–2.5 bar. Polyimide (Matrimid 5218) material was coated and pyrolyzed under N2 atmosphere on TiO2-ZrO2 macroporous tubes (Tami) that had not been structurally modified in any way. The supported carbon membrane was studied to determine its permeation for low molecular weight gases such as H2, CH4, CO, N2 and CO2. For these gases, the permeance of the composite supported carbon membranes obtained after pyrolysis at 550 °C increased with inverse square root of molecular weight. The temperature dependence of the permeance was described using an Arrhenius law with the negative activation energies for hydrogen, carbon dioxide and nitrogen providing evidence of a non-activated process. The ideal separation selectivity computed from single gas measurements leads to values slightly lower than the Knudsen because of the influence of viscous flow. The coexistence of more than one transport mechanism in the composite membrane was confirmed. After plugging the possible defects with Polydimethylsiloxane (PDMS), the supported carbon membranes obtained at a pyrolysis temperature of 650 °C showed evidence of a molecular sieving mechanism. This paper shows the separation properties of a crack-free supported carbon membrane obtained using a simple fabrication method that does not require modification of the mesoporous support. The permeance and selectivity values were compared with those of other hydrogen selective materials. Finally, the membranes were applied to methanol steam reforming (MSR).  相似文献   

8.
A parametric study of alkali-promoted hydrogen gas production from by-products from food-based biomass, such as glucose, molasses and rice bran, under hydrothermal conditions has been carried out. Partial oxidation of the biomass samples was aided by the addition of hydrogen peroxide and experiments were carried out in the presence of sodium hydroxide. The effects of reaction temperature, reaction time and feed concentration on the conversion of glucose, molasses and rice bran to gaseous products under hydrothermal conditions were investigated. The reaction time and reaction temperature were investigated in the range of 0–120 min and 330–390 °C, respectively. The results confirmed the positive influence of NaOH in the production of hydrogen gas via the water–gas shift reaction. In the presence of the alkali, no tar/oil and char were observed. The hydrogen gas yield increased when the reaction temperature and reaction time increased. It was observed that higher reaction temperature led to an increase in the amount of methane gas produced. With increasing feed concentration, the yields of other gases such as CO, CO2, CH4 and C2–C4 increased, while hydrogen gas production decreased for all the biomass samples. The generation of gaseous products from the molasses and rice bran showed a similar trend to that of glucose, under identical test conditions.  相似文献   

9.
In this paper we show, for the first time, the feasibility of ammonia exhaust gas reforming as a strategy for hydrogen production used in transportation. The application of the reforming process and the impact of the product on diesel combustion and emissions were evaluated. The research was started with an initial study of ammonia autothermal reforming (NH3 – ATR) that combined selective oxidation of ammonia (into nitrogen and water) and ammonia thermal decomposition over a ruthenium catalyst using air as the oxygen source. The air was later replaced by real diesel engine exhaust gas to provide the oxygen needed for the exothermic reactions to raise the temperature and promote the NH3 decomposition. The main parameters varied in the reforming experiments are O2/NH3 ratios, NH3 concentration in feed gas and gas – hourly – space – velocity (GHSV). The O2/NH3 ratio and NH3 concentration were the key factors that dominated both the hydrogen production and the reforming process efficiencies: by applying an O2/NH3 ratio ranged from 0.04 to 0.175, 2.5–3.2 l/min of gaseous H2 production was achieved using a fixed NH3 feed flow of 3 l/min. The reforming reactor products at different concentrations (H2 and unconverted NH3) were then added into a diesel engine intake. The addition of considerably small amount of carbon – free reformate, i.e. represented by 5% of primary diesel replacement, reduced quite effectively the engine carbon emissions including CO2, CO and total hydrocarbons.  相似文献   

10.
PdCu membranes prepared by sequential electroless plating were integrated into a hydrogen production and purification process. Hydrogen was produced from methane through catalytic partial oxidation and wet catalytic partial oxidation with Ni-based catalysts. Membrane permeance was measured with thermal cycles in an inert and hydrogen atmosphere at 673 and 773 K. Permeability was 1.98·10−3 mol/(smPa0.5) at 673 K and 2.62·10−3 mol/(smPa0.5) at 773 K. The optimum sweep gas flow required in the membrane module when operating with hydrogen-containing mixtures was selected. Peak hydrogen recovery was obtained using 15–20% of the feed to the module as sweep gas flow. Membranes were then placed downstream of the hydrogen production reactor. The CO and H2O percentages fed to the membrane module did not have a major impact on membrane behavior. Around 60–67% of the hydrogen fed to the membrane module was separated, regardless of its composition.  相似文献   

11.
In this paper an ethanol reformer based on catalytic steam reforming with a catalytic honeycomb loaded with RhPd/CeO2 and palladium separation membranes with an area of 30.4 cm2 has been used to generate a pure hydrogen stream of up to 100 ml/min to feed a PEM fuel cell with an active area of 5 cm2. The fuel reformer behavior has been extensively studied under different temperature, ethanol–water flow rate and gas pressure at a fixed S/C ratio of 1.6 (molar). The hydrogen yield has been controlled by acting upon the ethanol–water fuel flow and gas pressure.  相似文献   

12.
In order to investigate the relationship between the type of polyol feed and three-dimensionally mesoporous carbon supports with different mesopore structures and sizes, aqueous phase reforming (APR) reactions of xylitol and glycerol were carried out in a continuous fixed bed reactor. The effect of reaction conditions such as the reaction temperature and pressure on the APR performance were studied in the range of 215–250 °C and 28–45 bar. Three-dimensionally bimodal mesoporous carbon (3D-BMC) with the larger secondary mesopores showed the best catalytic performance in terms of carbon conversion to gas, hydrogen yield, selectivity, and hydrogen production rate due to its unique mesoporous structure, regardless of the kind of polyol feed. In addition, the reaction temperature and pressure significantly affected catalytic performance in the APR of polyols. The product selectivity was dependent on the reaction conditions and the type of polyol feed. The hydrogen selectivity of glycerol was higher than that of xylitol, whereas alkane selectivity was higher for xylitol, and the selectivity increased significantly by promoting the reactions favorable for alkane formation with increased reaction temperature and pressure.  相似文献   

13.
Steel slag, a waste from steelmaking plant, has been proven to be good candidate resources for low-cost calcium-based CO2 sorbent derivation. In this work, a cheap and sintering-resistance CaO-based sorbent (CaO (SS)) was prepared from low cost waste steel slag and was applied to enhance catalytic steam reforming of coke oven gas for production of high-purity hydrogen. This steel slag-derived CaO possessed a high and stable CO2 capture capacity of about 0.48 g CO2/g sorbent after 35 adsorption/desorption cycles, which was mainly ascribed to the mesoporous structure and the presence of MgO and Fe2O3. Product gas containing 95.8 vol% H2 and 1.4 vol% CO, with a CH4 conversion of 91.3% was achieved at 600 °C by steam reforming of COG enhanced by CaO (SS). Although high temperature was beneficial for methane conversion, CH4 conversion was remarkably increased at lower operation temperatures with the promotion effects from CaO (SS), and CO selectivity has been also greatly decreased. Reducing WHSV could increase methane conversion and reduce CO selectivity due to longer reactants residence time. Reducing C/A could increase methane conversion and hydrogen recovery factor, and also decrease CO selectivity. When being mixed with catalyst during SE-SRCOG, CaO (SS) with a uniform size distribution favored methane conversion due to the high utilization efficiency of catalyst. Promising stability of CaO (SS) in cyclic reforming/calcination tests was evidenced with a hydrogen recovery factor >2.1 and CH4 conversion of 82.5% at 600 °C after 10 cycles using CaO (SS) as sorbent.  相似文献   

14.
In this study, we investigate the configuration of a Pd–Au composite membrane on a porous nickel support and membrane modules for withstanding the capture of CO2 from a coal gasifier for a long time. The hydrogen permeation flux, recovery and CO2 capture were experimentally evaluated using two different modules and two conditions. As in our study, the CO2 capturing and durability tests were performed with a 40% CO2/60% H2 feed gas mixture in stainless steel (SS) 316L and 310S membrane modules. As a result, it is achieved the durability tests for more than 1150, 1100 (SS 316L module) and 3150 h (SS 310S module) with pressure cycles from 100 to 2000 kPa at 673 K. The durability of the membranes and membrane modules was demonstrated under pressure cycles from 100 to 2000 kPa at 673 K and the SS 310S module was very stable after 3150 h. The durability test for more than 3000 h demonstrated that there was no significant intermetallic diffusion between the PNS and Pd–Au layer. The CO2 capturing test performed using a 40% CO2/60% H2 mixture confirmed that the CO2 capturing capacity of the membrane and membrane module was 2.0 L/min for a CO2 concentration in the retentate stream of 92.3% and that the hydrogen recovery ratio increased with increasing pressure and reached 93.4%. Furthermore, we suggest that the SS 310S module configuration, CO2 capturing test using Pd–Au/ZrO2/PNS membrane and membrane module is very suitable for application as an Integrated Gasification Combined Cycle (IGCC) system due to very simple numbering-up stackable module design was successful.  相似文献   

15.
In this work continuous hydrogen production by Escherichia coli (XL1-BLUE) and its purification by membrane gas separation were studied. Firstly, a kinetic investigation was performed on formate supplemented broth in order to determine exponential growth phase (5–7 h) while the most intense hydrogen fermentation takes place. Furthermore, important process design parameters such as saturation constant and maximal growth rate were calculated (KS = 0.77 g l−1, μmax = 0.39 h−1). Afterward, based on the kinetic study, continuous hydrogen fermentations using cultures of E. coli (XL1-BLUE) were carried out in a CSTR reactor configuration applying various hydraulic retention times (HRT) related to both exponential and stationary growth period (5 h, 7 h, 9 h). The results indicated that highest hydrogen yield (0.26 mmol H2/mmol formate added) and productivity (5.1 mmol H2 l−1 d−1) could be achieved by applying HRT = 7 h that does not allow the living cells to reach stationary phase. In addition to hydrogen production, the concentration of bioH2 by polyimide membrane under different operational circumstances was investigated using pure and mixed gases, as well. The results of single gas experiments indicated that increasing the temperature has positive effect on separation efficiency. Moreover, the influence of retentate and feed flow ratio (QR/QF) was studied applying binary H2/CO2 gaseous mixture and it was found that polyimide membrane has high potential for H2 purification since 18% increase in H2 concentration and 22% decrease in CO2 content could be attained in the permeate by a one-step separation process.  相似文献   

16.
Pyrolysis fuel oil (PFO) processing by microwave plasma torch was developed for the production of hydrogen. The PFO cracking process was performed at atmospheric pressure in the absence of catalyst and effect of plasma gas on the production rate of hydrogen and light hydrocarbons (C2–C4) was evaluated. In the first step, effect of the applied power and the working gas flow rate was investigated. In the second step, the applied power and working gas rate were set to 650 W and 4000 sccm, respectively, which were provided by combining methane or ethane as 0%, 2.5%, 7.5%, and 20% with argon. By increasing the percentage of the existing methane in argon, production rate of the sum of the light hydrocarbons was increased and that of hydrogen was reduced, but it was more than the case when argon was applied alone. By increasing ethane percentage, hydrogen production and light hydrocarbon rate were increased. The best conditions of the plasma gas for producing hydrogen at the power of 650 W were obtained as 5CC PFO feed, 2500 sccm (80%) argon, and 500 sccm (20%). The hydrogen production rate in optimized conditions was 2343.16SCCM with selectivity of 84.41%. Sum of the obtained hydrocarbons in this test was 434.25 sccm. Another parameter in the present study was the feed volume processed by plasma. In this case, 5 cc, 3 cc, and 1 cc of the feed were tested when the plasma gas was 3000 sccm argon with the power of 650 W. The results showed that, by increasing the feed, the products were increased. In the processing of 5 cc feed with plasma, 896.41 sccm hydrogen and 61 sccm light hydrocarbon were produced.  相似文献   

17.
This work comprises a study of hydrogen separation with a composite Pd-YSZ-PSS membrane from mixtures of H2, N2, CO and CO2, typical of a water gas shift reactor. The Pd layer is extended over a tubular porous stainless steel support (PSS) with an intermediate layer of yttria-stabilized-zirconia (YSZ). YSZ and Pd layers were incorporated over the PSS using Atmospheric Plasma Spraying and Electroless Plating techniques, respectively. The Pd and YSZ thickness values are 13.8 and 100 μm, respectively, and the Pd layer is fully dense. Permeation measurements with pure, binary and ternary gases at different temperatures (350–450 °C), trans-membrane pressures (0–2.5 bar) and gas composition have been carried out. Moreover, thermal stability of the membrane was also checked by repeating permeation measurements after several cycles of heating and cooling the system. Membrane hydrogen permeances were calculated using Sieverts' law, obtaining values in the range of 4·10−5–4·10−4 mol m−2 s−1 Pa−0.5. The activation energy of the permeance was also calculated using Arrhenius' equation, obtaining a value of 16.4 kJ/mol. In spite of hydrogen selectivity being 100% for all experiments, the hydrogen permeability was affected by the composition of feed gas. Thus, a significant depletion in H2 permeate flux was observed when other gases were in the mixture, especially CO, being also more or less significant depending on gas composition.  相似文献   

18.
In this work, highly doped ceria with lanthanum, La0.5Ce0.5O2−δ (LDC), are developed as hydrogen separation membrane material. LDC presents a mixed electronic and protonic conductivity in reducing atmosphere and good stability in moist CO2 environment. LDC separation membranes with asymmetrical structure are fabricated by a cost-saving co-pressing method, using NiO + LDC + corn starch mixture as substrate and LDC as top membrane layer. Hydrogen permeation properties are systemically studied, including the influence of operating temperature, hydrogen partial pressure in feed stream and water vapor in both sides of the membrane on hydrogen permeating fluxes. Hydrogen permeability increases as the increasing of temperature and hydrogen partial pressure in feed gas. Using 20% H2/N2 (with 3% of H2O) as feed gas and dry high purity argon as sweep gas, an acceptable flux of 2.6 × 10−8 mol cm−2 s−1 is achieved at 900 °C. The existing of water in both sides of membrane has significant effect on hydrogen permeation and the corresponding reasons are analyzed and discussed.  相似文献   

19.
In this work, air gasification of sewage sludge was conducted in a lab-scale bubbling fluidized bed gasifier. Further, the gasification process was modeled using artificial neural networks for the product gas composition with varying temperatures and equivalence ratios. Neural network-based prediction will help to predict the hydrogen production from product gas composition at various temperatures and equivalence ratios. The gasification efficiency and lower heating values were also established as a function of temperatures and equivalence ratios. The maximum H2 and CO was recorded as 16.26 vol% and 33.55 vol%. Intraileally at ER 0.2 gas composition H2, CO, and CH4 show high concentrations of 20.56 vol%, 45.91 vol%, and 13.32 vol%, respectively. At the same time, CO2 was lower as 20.20 vol% at ER 0.2. Therefore, optimum values are suggested for maximum H2 and CO yield and lower concentration of CO2 at ER 0.25 and temperature of 850 °C. A predictive model based on an Artificial Neural network is also developed to predict the hydrogen production from product gas composition at various temperatures and equivalence ratios. The network has been trained with different topologies to find the optimal structure for temperature and equivalence ratio. The obtained results showed that the regression coefficients for training, validation, and testing are 0.99999, 0.99998, and 0.99992, respectively, which clearly identifies the training efficiency of the trained model.  相似文献   

20.
Partial oxidation of ethanol with air was carried out in a pulsed discharge plasma reactor at low temperature and atmospheric pressure. Effects of O2:ethanol ratio, ethanol flow rate, and discharge current were investigated. H2 and CO are the major products (>86%). Increases of O2:ethanol ratio promote CO formation at the expense of C2 hydrocarbons. H2 selectivity and H2 + CO selectivity are maximized at O2:ethanol ratios of 0.3 and 0.5, respectively. Increases of feed flow rate accompanied by current increases allow the reactor to operate with high throughput. The LHV energy efficiency is increased with increasing feed flow rate, reaching 85% at high ethanol flow rates, conditions that also increase throughput. In contrast to catalytic and homogenous reactions, not all O2 is consumed at high O2:ethanol ratio for the low temperature plasma reaction. A radical reaction pathway of H abstraction from –OH and the α-H in ethanol to form CH3CHO followed by C–C scission is proposed. The produced hydrogen rich gas can be potentially used in fuel cells and engines.  相似文献   

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