首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 46 毫秒
1.
Influence of synthesis parameters; silica sources, relative alkalinity and silicon module, were investigated on preparation of T type zeolite by hydrothermal method, using a two level factorial design. Crystallization time and reaction temperature were held constant at 7 days and 378 K, respectively. The synthesized products were characterized by XRD and SEM techniques. The results showed that increasing silicon module and decreasing relative alkalinity in the synthesis gel improved the product relative crystallinity. It was also observed that using colloidal silica as the silica source improved crystallinity and phase purity of T type zeolites. The prepared zeolite T with the highest relative crystallinity was examined in the batch adsorption experiments at three temperatures of 288, 298 and 308 K and various pressures from 0.1 up to 2 MPa to verify the ability of the material for selective adsorption and separation of CO2 from CH4. The adsorption capacities and isotherms of CO2 and CH4 were determined at the studied temperatures. The results showed that the highest ideal selectivity of CO2/CH4 could be achieved at atmospheric pressure and 308 K. The performance of the adsorbent was confirmed with breakthrough curves and breakthrough times resulted from dynamic adsorption experiments of the mixed gases.  相似文献   

2.
Adsorptive separation of CH4/CO2 mixtures was studied using a fixed-bed packed with MIL-53(Al) MOF pellets. Such pellets of MIL-53(Al) were produced using a polyvinyl alcohol binder. As revealed by N2 adsorption isotherms, the use of polyvinyl alcohol as binder results in a loss in overall capacity of 32%. Separations of binary mixtures in breakthrough experiments were successfully performed at pressures varying between 1 and 8 bar and different mixture compositions. The binary adsorption isotherms reveal a preferential adsorption of CO2 compared to CH4 over the whole pressure and concentration range. The separation selectivity was affected by total pressure; below 5 bar, a constant selectivity, with an average separation factor of about 7 was observed. Above 5 bar, the average separation factor decreases to about 4. The adsorption selectivity is affected by breathing of the framework and specific interaction of CO2 with framework hydroxyl groups. CO2 desorption can be realised by mild thermal treatment.  相似文献   

3.
Abstract

Pure component adsorption equilibrium of CH4 and CO2 on activated carbon have been studied at three different temperatures, 298, 323, and 348?K within a pressure range of 10–2000?kPa. Binary adsorption equilibrium isotherm was described using extended Sips equation and ideal adsorbed solution theory (IAST) model. Experimental breakthrough curves of CO2/CH4 (40:60 in a molar basis) were performed at four different pressures (300, 600, 1200, and 1800?kPa). The experimental results of binary isotherms and breakthrough curves have been compared to the predicted simulation data in order to evaluate the best isotherm model for this scenario. The IAST and Sips models described significantly different results for each adsorbed component when higher pressures are set. These different results cause a significant discrepancy in the estimation of the equilibrium selectivity. Simulated and experimental equilibrium selectivity data provided by IAST presented values of around 4, for CO2/CH4, and extended Sips presented values of around 2. Also, simulated breakthrough curves showed that IAST fits better to the experimental data at higher pressures. According to the simulations, in a binary mixture at total pressure over 800?kPa, extended Sips model underestimated significantly the CO2 adsorbed amount and overestimated the CH4 adsorbed amount.  相似文献   

4.
In this study, the adsorption capacity of single-wall carbon nanotubes (SWCNTs) bundles with regard to the pure CH4, N2, CO and CO2 gases at 298 K and pressure range from 0.01 up to 2.0 MPa has been investigated experimentally and computationally. Experimental work refers to gravimetric surface excess adsorption measurements of each gas studied in this nanomaterial. Commercial samples of pristine SWCNTs, systematically prepared and characterized at first, were used for the evaluation of their adsorption capacity. A Langmuir type equation was adopted to estimate the total adsorption isotherm based on the experimental surface excess adsorption data for each system studied. Computational work refers to Monte Carlo (MC) simulation of each adsorbed gas on a SWCNTs model of the type (9, 9) in the grand canonical (GC) ensemble at the same conditions with experiment using Scienomics’ MAPS platform software simulation packages such as Towhee. The GCMC simulation technique was employed to obtain the uptake wt% of each adsorbed gas by considering a SWCNTs model of arrays with parallel tubes exhibiting open-ended cylindrical structures as in experiment. Both experimental and simulation adsorption data concerning these gases within the examined carbon material are presented and discussed in terms of the adsorbate fluid molecular characteristics and corresponding interactions among adsorbate species and adsorbent material. The adsorption isotherms obtained exhibited type I (Langmuir) behavior, providing enhanced gas-substrate interactions. We found that both the experimental as well as the simulated adsorption uptake of the examined SWCNTs at these conditions with regard to the aforementioned fluids and in comparison with adsorbate H2 on the same material increase similarly and in the following order: H2 ? N2 ≈ CH4 < CO ? CO2. Furthermore, for each adsorbate fluid the calculations exhibit somewhat greater gas uptake with pressure compared to the corresponding experiment. The difference in the absolute uptake values between experiment and simulation has been discussed and ascribed to the following implicit factors: (i) to the employed model calculations, (ii) to the remained carbonaceous impurities in the sample, and (iii) to a proportion of close ended tubes, contained in the experimental sample even after preparation.  相似文献   

5.
The modification of activated carbon fibres prepared from a commercial textile acrylic fibre into materials with monolithic shape using phenolic resin as binder was studied. The molecular sieving properties for the gas separations CO2/CH4 and O2/N2 were evaluated from the gas uptake volume and selectivity at 100 s contact time taken from the kinetic adsorption curves of the individual gases. The pseudo-first order rate constant was also determined by the application of the LDF model. The samples produced show high CO2 and O2 rates of adsorption, in the range 3-35 × 10−3 s−1, and in most cases null or very low adsorption of CH4 and N2 which make them very promising samples to use in PSA systems, or similar. Although the selectivity was very high, the adsorption capacity was low in certain cases. However, the gas uptake in two samples reached 23 cm3 g−1 for CO2 and 5 cm3 g−1 for O2, which can be considered very good. The materials were heat-treated using a microwave furnace, which is a novel and more economic method, when compared with conventional furnaces, to improve the molecular sieves properties.  相似文献   

6.
Adsorption equilibrium capacity of CO2, CH4, N2, H2 and O2 on periodic mesoporous MCM-41 silica was measured gravimetrically at room temperature and pressure up to 25 bar. The ideal adsorption solution theory (IAST) was validated and used for the prediction of CO2/N2, CO2/CH4, CO2/H2 binary mixture adsorption equilibria on MCM-41 using single components adsorption data. In all cases, MCM-41 showed preferential CO2 adsorption in comparison to the other gases, in agreement with CO2/N2, CO2/CH4, CO2/H2 selectivity determined using IAST. In comparison to well known benchmark CO2 adsorbents like activated carbons, zeolites and metal-organic frameworks (MOFs), MCM-41 showed good CO2 separation performances from CO2/N2, CO2/CH4 and CO2/H2 binary mixtures at high pressure, via pressure swing adsorption by utilizing a medium pressure desorption process (PSA-H/M). The working CO2 capacity of MCM-41 in the aforementioned binary mixtures using PSA-H/M is generally higher than 13X zeolite and comparable to different activated carbons.  相似文献   

7.
In this study, fresh water methane-producing bacterium (MPB), strain FJ10, which used H2 as an electron donor and CO2 as an electron acceptor, was isolated and chosen as the primary methanogen for the conversion of CO2 into CH4. Improvements to culture medium to increase methane production were investigated using a fractional factorial design in 32 experiments with six variables under consumption of H2/CO2 at ratios of 4 and 1. The tested nutrient compositions were NaCl, NH4Cl, FeSO4, MgCl2, H2PO4 and yeast extract. Experimental results indicate that yeast extract was essential for the growth of strain FJ10 to impact the conversion of CO2 into CH4. Strain FJ10 generated maximum CH4 production with 5.0 g/l of yeast extract. Moreover, optimal culture conditions for methane production by strain FJ10 were 40 °C and pH 8. Approximately 22-25% of CO2 conversion into CH4 was achieved at an H2/CO2 ratio of 4 and roughly 2.5-6% of CO2 conversion into CH4 was obtained at an H2/CO2 ratio of 1 under different pressurized conditions of 1 atm, 50 atm and 100 atm. Under 100 atm, about 6780 μM CH4 was produced with an H2/CO2 ratio of 4 and 4240 μM CH4 was produced with an H2/CO2 ratio of 1 under the steady state condition. The kinetic model for H2/CO2 utilization and CH4 production under different pressures was verified by experimental data. Model predictions are in good agreement with experimental results. The experimental and modeling approaches in this study can be applied to evaluate the conversion of CO2 into CH4 as an energy source by geo-microorganisms in geological sequestration.  相似文献   

8.
In this study, gas separation properties of Matrimid/MIL-53 mixed matrix membranes with different MOF weight percentages (0–20 wt.%) were investigated. TEM, XRD and DLS analysis were implemented to investigate MIL-53, structure and particles size distribution. SEM, FTIR, DSC and TGA analyses were conducted to characterize the fabricated membranes. The SEM images of these membranes showed good adhesion between polymer and particles, although for 20% MIL-53 loading, particles agglomeration was observed in some areas. Moreover, surface images of the membranes showed adequate dispersion of the particles in the polymer matrix, especially at lower MOF loadings. The permeability of pure CO2 and CH4 gases for all membranes were measured and the ideal CO2/CH4 selectivity was calculated. CH4 permeability of membranes increased slightly as the percentage of loading increased. At 20 wt.% MOF loading, void formation led to a significant increase in CH4 permeability (300% over pure Matrimid). CO2 permeability showed the same trend; there was a 94% increase in permeability compared to pure Matrimid for 15 wt.% MMMs. CO2/CH4 selectivity also increased as MOF loading increased. The highest selectivity was shown for 15 wt.% MOF loading. This membrane had 84% growth in selectivity over pure Matrimid. Although at 20 wt.% MIL-53 loading, membrane separation performance was destroyed.  相似文献   

9.
Pei Shi Tin  Tai-Shung Chung  Ye Liu  Rong Wang 《Carbon》2004,42(15):3123-3131
The separation of CO2/CH4 separation is industrially important especially for natural gas processing. In the past decades, polymeric membranes separation technology has been widely adopted for CO2/CH4 separation. However, polymeric membranes are suffering from plasticization by condensable CO2 molecules. Thus, carbon molecular sieve membranes (CMSMs) with excellent separation performance and stability appear to be a promising candidate for CO2/CH4 separation. A commercially available polyimide, P84 has been chosen as a precursor in preparing carbon membranes for this study. P84 displays a very high selectivity among the polyimides. The carbonization process was carried out at 550–800 °C under vacuum environment. WAXD and density measurements were performed to characterize the morphology of carbon membranes. The permeation properties of single and equimolar binary gas mixture through carbon membranes were measured and analyzed. The highest selectivity was attained by carbon membranes pyrolyzed at 800 °C, where the pyrolysis temperatures significantly affected the permeation properties of carbon membranes. A comparison of permeation properties among carbon membranes derived from four commercially available polyimides showed that the P84 carbon membranes exhibited the highest separation efficiency for CO2/CH4 separation. The pure gas measurement underestimated the separation efficiency of carbon membranes, due to the restricted diffusion of non-adsorbable gas by adsorbable component in binary mixture.  相似文献   

10.
Adsorption and separation of N2, CH4, CO2, H2 and CO mixtures in CMK-5 material at room temperature have been extensively investigated by a hybrid method of grand canonical Monte Carlo (GCMC) simulation and adsorption theory. The GCMC simulations show that the excess uptakes of pure CH4 and CO2 at 6.0 MPa and 298 K can reach 13.18 and 37.56 mmol/g, respectively. The dual-site Langmuir–Freundlich (DSLF) model was also utilized to fit the absolute adsorption isotherms of pure gases from molecular simulations. By using the fitted DSLF model parameters and ideal adsorption solution theory (IAST), we further predicted the adsorption separation of N2–CH4, CH4–CO2, N2–CO2, H2–CO, H2–CH4 and H2–CO2 binary mixtures. The effect of the bulk gas composition on the selectivity of these gases is also studied. To improve the storage and separation performance, we finally tailor the structural parameters of CMK-5 material by using the hybrid method. It is found that the uptakes of pure gases, especially for CO2, can be enhanced with the increase of pore diameter Di, while the separation efficiency is apparently favored in the CMK-5 material with a smaller Di. The selectivity at Di=3.0 nm and 6.0 MPa gives the greatest value of 8.91, 7.28 and 27.52 for SCO2/N2, SCH4/H2 and SCO2/H2, respectively. Our study shows that CMK-5 material is not only a promising candidate for gas storage, but also suitable for gas separation.  相似文献   

11.
Using a manometric experimental setup, high-pressure sorption measurements with CH4 and CO2 were performed on three Chinese coal samples of different rank (VRr = 0.53%, 1.20%, and 3.86%). The experiments were conducted at 35, 45, and 55 °C with pressures up to 25 MPa on the 0.354-1 mm particle fraction in the dry state. The objective of this study was to explore the accuracy and reproducibility of the manometric method in the pressure and temperature range relevant for potential coalbed methane (CBM) and CO2-enhanced CBM (CO2-ECBM) activities (P > 8 MPa, T > 35 °C). Maximum experimental errors were estimated using the Gauss error propagation theorem, and reproducibility tests of the high-pressure sorption measurements for CH4 and CO2 were performed. Further, the experimental data presented here was used to explicitly study the CO2 sorption behaviour of Chinese coal samples in the elevated pressure range (up to 25 MPa) and the effects of temperature on supercritical CO2 sorption isotherms.The experiments provided characteristic excess sorption isotherms which, in the case of CO2 exhibit a maximum around the critical pressure and then decline and level out towards a constant value. The results of these manometric tests are consistent with those of previous gravimetric sorption studies and corroborate a crossover of the 35, 45, and 55 °C CO2 excess sorption isotherms in the high-pressure range. The measurement range could be extended, however, to significantly higher pressures. The excess sorption isotherms tend to converge, indicating that the temperature dependence of CO2 excess sorption on coals at high-pressures (>20 MPa) becomes marginal. Further, all CO2 high-pressure isotherms measured in this study were approximated by a three-parameter excess sorption function with special consideration of the density ratio of the “free” phase and the sorbed phase. This function provided a good representation of the experimental data.The maximum excess sorption capacity of the three coal samples for methane ranged from 0.8 to 1.6 mmol/g (dry, ash-free) and increased from medium volatile bituminous to subbituminous to anthracite. The medium volatile bituminous coal also exhibited the lowest overall excess sorption capacity for CO2. However, the subbituminous coal was found to have the highest CO2 sorption capacity of the three samples. The mass fraction of adsorbed substance as a function of time recorded during the first pressure step was used to analyze the kinetics of CH4 and CO2 sorption on the coal samples. CO2 sorption proceeds more rapidly than CH4 sorption on the anthracite and the medium volatile bituminous coal. For the subbituminous coal, methane sorption is initially faster, but during the final stage of the measurement CO2 sorption approaches the equilibrium value more rapidly than methane.  相似文献   

12.
In order to increase the use of carpet wastes (pre- and/or post-consumer wastes), this work studies for the first time the preparation and characterisation of a microporous material from a commercial carpet (pile fiber content: 80% wool/20% nylon; primary and secondary backings: woven polypropylene; binder: polyethylene) and its application for CO2 capture. The porous material was prepared from an entire carpet material using a standard chemical activation with KOH and then, characterised in terms of their porous structure and surface functional groups. Adsorption of CO2 was studied using a thermogravimetric analyser at several temperatures (25-100 °C) and under different CO2 partial pressures (i.e. pure CO2 flow and a ternary mixture of 15% CO2, 5% O2 and 80% N2). In order to examine the adsorbent regenerability, multiple CO2 adsorption/desorption cycles were also carried out. The surface area and micropore volume of the porous adsorbent were found to be 1910.17 m2 g− 1 and 0.85 cm3 g− 1, respectively. The CO2 adsorption profiles illustrate that the maximum CO2 capture on the sample was reached in less than 10 min. CO2 adsorption capacities up to 8.41 wt.% and 3.37 wt.% were achieved at 25 and 70 °C, respectively. Thermal swing regeneration studies showed that the prepared adsorbent has good cyclic regeneration capacities.  相似文献   

13.
Dong Young Kim 《Carbon》2008,46(4):611-617
Single wall carbon nanotubes (SWCNTs) were treated with a HNO3/H2SO4 mixed solution to increase the number of narrow micropores. The mixed acid treatment increased the micropore volume from 0.13 to 0.35 mL g−1 as measured by N2 adsorption at 77 K. The micropore volume evaluated with CO2 adsorption at 273 K increased from 0.06 to 0.27 mL g−1. This remarkable micropore volume increase was ascribed to the formation of a highly packed and ordered SWCNT assembly with the acid treatment, which was confirmed by field emission scanning electron microscopy. The adsorption amount of supercritical H2 at 77 K under 5 MPa pressure increased twofold as a result of the acid treatment, while the supercritical CH4 adsorption amount at 303 K and 5 MPa pressure increased by 40%. These remarkable increases were caused by increased amount of narrow micropores as a result of the acid treatment.  相似文献   

14.
CO2 and CH4 equilibrium adsorption are predicted by Excess Gibbs energy models based on vacancy solution theory, for single and binary mixture on Multi‐Walled Carbon Nanotubes (MWCNTs) functioned by –NH2 group. The experimental data of single gas adsorption isotherms were obtained at moderate pressures and temperatures using the volumetric method in a static gaseous set up. Firstly, the equilibrium pressures related to the adsorbed amounts, for single gases, were correlated on Wilson and Flory–Huggins activity coefficient equations based on vacancy solution theory and the model parameters were determined by fitting the model on the experimental data. Secondly, the pure component parameters were implemented in extended Wilson and Flory–Huggins equations for CO2 and CH4 mixture to predict the gas–solid phase equilibria. The results showed fairly good agreement between the experiments and both Gibbs models. Finally, the studied models were compared with the popular model of Extended Langmuir. The results revealed more accurately and precisely prediction of Wilson and Flory–Huggins against Langmuir model for mixed gas of CO2 and CH4 on MWCNT–NH2. © 2011 Canadian Society for Chemical Engineering  相似文献   

15.
Nanotubes were coated on the surface of active LiCoO2 particles using electrostatic heterocoagulation to enhance the electrochemical properties of a Li-ion battery. Only 0.5 wt% of multiwalled carbon nanotubes (MWCNTs) was added as a conducting agent into the LiCoO2 cathode, which had a density of 4.0 g cm−3. We found that our electrode that was prepared using heterocoagulation with 0.5 wt% of thin MWCNTs maintained a volumetric capacitance of 403 mAh cm−1 after 40 cycles from the initial 624 mAh cm−1, compared with previous result of 310 mAh cm−1 obtained from simple mixing with 3 wt% MWCNTs. The high volumetric capacity with smaller swelling using less amount of MWCNTs was attributed to the self-assembled nanotube network formed between active particles during coagulation, which was maintained with volume expansion during cycle testing.  相似文献   

16.
Selective synthesis of gasoline-range hydrocarbons (C5-C12) was investigated in a fixed-bed micro reactor using two series of CO2-containing syngas with various mole CO2/(CO + CO2) and H2/(CO + CO2) ratios, where Fischer-Tropsch synthesis(FTS) and in situ hydrocracking/hydroisomerization were performed over bifunctional Co/SiO2/HZSM-5 catalyst. CO2 was converted at 0.15-0.55 of CO2/(CO + CO2) ratio under H2-rich condition (H2/(CO + CO2) = 2.0), highest conversion of 20.3% at 0.42. Further increasing CO2 content decreased CO2 conversion and quite amount of CO2 acted as diluting component. For the syngas with low H2 content or H2/(CO + CO2) ratio(< 1.85, H2/CO = 2.0), the competitive adsorption of CO, H2 and CO2 resulted in low CO, CO2 and total carbon conversion, which was 57.9%, 12.7% and 31.4% respectively at 0.74 of H2/(CO + CO2) ratio(H2/CO/CO2/N2 = 40.8/20.4/34.8/4). FTS results indicated that high H2 content and proper H2/(CO + CO2) ratio were favorable for the conversion of CO2-containing syngas. More than 45% selectivity to gasoline-range hydrocarbons including isoparaffins was obtained under the two series of syngas. It was also tested that the catalytic activity of Co/SiO2/HZSM-5 kept stable under CO2-containing syngas(< 7.5%). And the quick catalytic deactivation under high CO2 containing syngas(H2/CO/CO2/N2 = 45.3/23.2/27.1/3.06) was due to carbon deposition and pore blockage by heavy hydrocarbon, tested by thermal gravimetry, N2 physisorption and scanning electron microscopy(SEM).  相似文献   

17.
Kinetics and selectivity of supercritical carbon dioxide (SC CO2) extraction of Helichrysum italicum flowers were analyzed at pressures in the range of 10-20 MPa and temperatures of 40 °C and 60 °C (density of SC CO2 from 290 to 841 kg/m3) and also at 10 MPa and 40 °C using flowers with different moisture contents (10.5% and 28.4%). Increased moisture content of H. italicum flowers resulted in enchased solubility of solute enabling decrease of SC CO2 consumption necessary for achieving desired extraction yield. The most abundant compounds in the supercritical extracts are sesquiterpenes and waxes while monoterpenes and sesquiterpenes are the main constituents of essential oil obtained by hydrodistillation. The optimal set of working parameters with respect to extraction yield, SC CO2 consumption and chemical composition of extract were defined related to moisture content of raw material and SC CO2 density.  相似文献   

18.
The adsorption isotherms of N2 at 77K, CO2 at 251, 273 and 298K, and SO2 at 262 and 273K have been determined on a series of physically activated carbons with a wide range of micropore size distributions. Since the series includes carbons with very high burn-off, it shows the problems involved in the characterization of microporsity in superactivated carbons. On the other hand, the results show that the carbon surface-adsorbate interactions for SO2 at low relative pressures are weaker than for N2 and CO2, as a result of the strong adsorptive-adsorptive interactions in the bulk gas phase.  相似文献   

19.
Methane and CO2 are the main components of biogas; therefore its direct conversion into a higher added value gas as syn-gas (mixture of CO and H2) is a very interesting alternative for the valorisation of such renewable resource. In this work, firstly a thermodynamic analysis of the decomposition of CH4:CO2 mixtures at different temperatures and CH4:CO2 ratios simulating the biogas composition, has been carried out. Secondly, the decomposition of a mixture with a molar ratio of 1:1 has been studied in a fixed-bed reactor by using a Ni/Al2O3 based catalyst, at the temperature range in which according to the thermodynamic study, carbon formation is favoured. Results obtained have been compared to those of methane decomposition carried out under the same experimental conditions. Co-feeding of CO2 and CH4 avoids catalyst deactivation substantially, allowing to obtain a syn-gas with H2:CO ratio close to 1. Moreover, the carbon obtained from mixtures of CH4 and CO2 is deposited as fishbone carbon nanofibres at 600 °C and ribbon carbon nanofibers at 700 °C, both being materials with high added value which can be used in multiple applications.  相似文献   

20.
Industrial adsorptive separation process for liquids is most successful when the involved species have very close boiling points, making distillation expensive or are thermally sensitive at convenient distillation temperatures. The adsorption process was studied for separating meta-xylene from a feed mixture containing all C8 aromatics on binder-free X and Y zeolites in the liquid phase. Zeolitic adsorbents with different SiO2/Al2O3 were synthesized by the hydrothermal method and ion-exchanged with alkaline metal cations like lithium, sodium and potassium. The adsorption process was carried out in a breakthrough system at temperature of 110–160 °C and pressure of 6–8 atm. The influence of adsorbent moisture content on the separation process was studied. The optimization of adsorption process was also investigated by the changing operation conditions. The isotherms for each isomer of C8 aromatics and the desorbent possess the adsorption characteristics of Langmuir type. The selectivity factor of meta-xylene and the saturation adsorption capacities of adsorbates were determined. It was observed that the selectivity of meta-xylene increased by sodium ion-exchanging of cationic sites in Y zeolite and the selectivity factor of meta-xylene/para-xylene, meta-xylene/ortho-xylene and meta-xylene/ethylbenzene in the optimum conditions was determined to be 2.62, 2.83 and 5.93, respectively.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号