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1.
The effect of impregnation of activated carbon with Cr2O and Fe2O3 and promotion by Zn2+ on its adsorptive properties of carbon dioxide was studied using a volumetric adsorption apparatus at ambient temperature and low pressures. Slurry and solution impregnation methods were used to compare CO2 capture capacity of the impregnated activated carbon promoted by Zinc. The obtained adsorption isotherms showed that amount of CO2 adsorbed on the samples impregnated by Cr2O was increased about 20% in compare to raw activated carbon. The results also showed that Fe2O3 was not an effective impregnating species for activated carbon modification. Moreover slurry impregnation method showed higher CO2 adsorption capacity in comparison with solution impregnation method. Samples prepared by co-impregnation of two metal species showed more adsorption capacity than samples impregnated by just one metal species individually. Washing the impregnated samples by metal oxide resulted in 15% increase in CO2 adsorption capacities of activated carbons which can be attributed to the metal oxides removal covering the adsorption surface. Decreasing impregnation temperature from 95 to 25 °C in solution method showed a significant increase in CO2 adsorption capacity. Sips equation was found a suitable model fitting to the adsorption data in the range studied.  相似文献   

2.
Mesoporous MCM-48 silica was synthesized using a cationic-neutral surfactant mixture as the structure-directing template and rice husk ash (RHA) as the silica source. The MCM-48 samples were characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), N2 physisorption and SEM. X-ray diffraction pattern of the resulting MCM-48 revealed typical pattern of cubic Ia3d mesophase. BET results showed the MCM-48 to have a surface area of 1024 m2/g and FT-IR revealed a silanol functional group at about 3460 cm−1. Breakthrough experiments in the presence of MCM-48 were also carried out to test the material's CO2 adsorption capacity. The breakthrough time for CO2 was found to decrease as the temperature increased from 298 K to 348 K. The steep slopes observed shows the CO2 adsorption occurred very quickly, with only a minimal mass transfer effect and very fast kinetics. In addition, amine grafted MCM-48, APTS-MCM-48 (RHA), was prepared with the 3-aminopropyltriethoxysilane (APTS) to investigate the effect of amine functional group in CO2 separation. An order of magnitude higher CO2 adsorption capacity was obtained in the presence of APTS-MCM-48 (RHA) compared to that with MCM-48 (RHA). These results suggest that MCM-48 synthesized from rice husk ash could be usefully applied for CO2 removal.  相似文献   

3.
Stable carbon isotopes are important tools to assess potential storage sites for CO2, as they allow the quantification of ionic trapping via isotope mass balances. In deep geological formations high p/T conditions need to be considered, because CO2 dissolution, equilibrium constants and isotope fractionation of dissolved inorganic carbon (DIC) depend on temperature, pressure and solute composition. After reviewing different approaches to account for these dependencies, an expanded scheme is presented for speciation and carbon isotope fractionation of DIC and dissolution of CaCO3 for pCO2 up to 100 bar, pH down to 3 and temperatures of up to 200 °C. The scheme evaluates the influence of respective parameters on isotope ratios during CO2 sequestration. The pCO2 and pH are the dominant controlling factors in the DIC/δ13C/pH system. The fugacity of CO2 has major impact on DIC concentrations at temperatures below 100 °C at high pCO2. Temperature dependency of activities and equilibrium dominates at temperatures above 100 °C. Isotope ratios of DIC are expected to be about 1–2‰ more depleted in 13C compared to the free CO2 at pCO2 values above 10 bar. This depletion is controlled by carbon isotope fractionation between CO2 and H2CO3* which is the dominant species of DIC at the resulting pH below 5.  相似文献   

4.
Conversion of leather wastes to useful products   总被引:1,自引:0,他引:1  
The main objective of the present study is to investigate the production of useful materials from different kinds of leather waste. Three different types of tannery wastes (chromium- and vegetable-tanned shavings, and buffing dust) were pyrolyzed in a fixed bed reactor at temperatures of 450 and 600 °C under N2 atmosphere. Gas, oil, ammonium carbonate and carboneous residue were obtained by pyrolysis. The effect of temperature and type of leather waste on product distribution of pyrolysis was investigated. Buffing dust gave the highest yield of oil (ca. 23%), while other wastes recorded yields of ca. 9%. Results of elemental analysis and column chromatography showed that pyrolysis oils could be used as fuel or chemical feedstock after re-treatment. The yields of carboneous residue (chars) were between 37.5% and 48.5% and their calorific value was between 4300 and 6000 kcal kg−1, suitable for use as solid fuel. In addition, these chars were activated by CO2 to obtain the activated carbon. The activated carbon having highest surface area (799.5 m2 g−1) was obtained from chromium-tanned shavings. Activated carbons prepared from chromium-tanned leather were presented as an adsorbant for the adsorption of dyes from aqueous solution.  相似文献   

5.
In this work several Li4SiO4-based sorbents from fly ashes for CO2 capture at high temperatures have been developed. Three fly ash samples were collected and subjected to calcination at 950 °C in the presence of Li2CO3. Both pure Li4SiO4 and fly ash-based sorbents were characterised and tested for CO2 sorption at different temperatures between 400 and 650 °C and adding different amounts of K2CO3 (0–40 mol%). To examine the sorbents performance, multiple CO2 sorption/desorption cycles were carried out. The temperature and the presence of K2CO3 strongly affect the CO2 sorption capacity for the sorbents prepared from fly ashes. When the sorption temperature increases by up to 600 °C both the CO2 sorption capacity and the sorption rate increase significantly. Moreover when the amount of K2CO3 increases, the CO2 sorption capacity also increases. At optimal experimental conditions (600 °C and 40 mol% K2CO3), the maximum CO2 sorption capacity for the sorbent derived from fly ash was 107 mg CO2/g sorbent. The Li4SiO4-based sorbents can maintain its original capacity during 10 cycle processes and reach the plateau of maximum capture capacity in less than 15 min, while pure Li4SiO4 presents a continual upward tendency for the 15 min of the capture step and attains no equilibrium capacity.  相似文献   

6.
In this work, unburnt coal (UC) in bottom ash from coal-fired power plants was soaked in KOH solution and activated for 1 h at 780 °C. The yield of activated carbons varied from 47.8 to 54.8% when the KOH/UC weight ratio changed from 2 to 4. Pore properties of these activated carbons including the BET surface area, pore volume, pore size distribution, and pore diameter were characterized based on N2 adsorption isotherms. It was shown that the isotherms for the adsorption of methylene blue, acid blue 74, and 4-chlorophenol from aqueous solutions on these activated carbons at 30 °C were well fitted by the Langmuir equation (correlation coefficient r2 > 0.9968). The adsorption capacities of methylene blue, acid blue 74, and 4-chlorophenol were obtained to be 2.40–2.88, 0.57–1.29, and 2.34–5.62 mmol/g, respectively. Moreover, the adsorption kinetics could be suitably described by the Elovich equation.  相似文献   

7.
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   

8.
This work presents contact angle measurements for CO2–water–quartz/calcite systems at general sequestration pressure and temperature conditions (200–3000 psig and 77–122 °F). The effect of drop volume, repeated exposure of the substrates to dense water saturated CO2, pressure and temperature on the contact angles is examined. In the 1st measurement cycle, the contact angles for the quartz substrate varied from 46 to 48° and 47 to 46° for gaseous (water saturated) CO2 and liquid (water saturated) CO2 respectively, at 77 °F. For calcite substrate, these values varied from 45 to 48° and 42 to 40°, respectively. Remarkably, this work highlights a characteristic permanent shift in the contact angle data with repeated exposure to dense, water saturated, CO2. The contact angle data trends after repeated exposure to the dense, water saturated CO2 varied from 89 to 91° and 85 to 80° for the quartz substrate for gaseous (water saturated) CO2 and liquid (water saturated) CO2 respectively, at 77 °F. For calcite substrates, these values varied from 60 to 59° and 54 to 48°, respectively. This important observation has serious implications towards the design and safety issues, as a permanent positive contact angle shift indicates lower CO2 retention capabilities of sequestration sites due to a reduction in the capillary pressure. It is further confirmed that the permanent shift in the contact angle is due to surface phenomena. With an increase in temperature (from 77 to 122 °F), the contact angle shift is reduced from about 45° to about 20° for quartz substrates. Other observations in the contact angle data with respect to pressure are in good agreement with the trends reported in the literature.  相似文献   

9.
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   

10.
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   

11.
This study reveals the first analyses of the composition and activity of the microbial community of a saline CO2 storage aquifer. Microbial monitoring during CO2 injection has been reported. By using fluorescence in situ hybridisation (FISH), we have shown that the microbial community was strongly influenced by the CO2 injection. Before CO2 arrival, up to 6 × 106 cells ml−1 were detected by DAPI staining at a depth of 647 m below the surface. The microbial community was dominated by the domain Bacteria that represented approximately 60% to 90% of the total cell number, with Proteobacteria and Firmicutes as the most abundant phyla comprising up to 47% and 45% of the entire population, respectively. Both the total cell counts as well as the counts of the specific physiological groups revealed quantitative and qualitative changes after CO2 arrival. Our study revealed temporal outcompetition of sulphate-reducing bacteria by methanogenic archaea. In addition, an enhanced activity of the microbial population after five months CO2 storage indicated that the bacterial community was able to adapt to the extreme conditions of the deep biosphere and to the extreme changes of these atypical conditions.  相似文献   

12.
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   

13.
In this research, nanoporous zeolite T membranes were synthesized at three levels of synthesis temperature: 100, 120 and 140 °C and synthesis time: 15, 30 and 50 h and characterized by gas permeation. Effects of synthesis parameters on CO2 and CH4 permeances and CO2/CH4 ideal separation factors were studied. All experiments were conducted at 1 bar feed pressure and 30 °C module temperature. Normally, it is anticipated that increasing synthesis temperature and synthesis time increase gas permeances and consequently decrease ideal separation factor. This prediction was not observed in the case of synthesis temperature increase from 100 to 120 °C as well as synthesis time increase from 15 to 30 h, due to the dual effect of increasing synthesis temperature and synthesis time on gas permeances and ideal separation factor. More zeolites are deposited and larger crystals are formed at higher synthesis temperatures and times. Forming the larger crystals accelerates the rate of zeolite layer integration, which is responsible for gas separation, in one hand and reduces the density of deposited zeolite layer on the support, due to the formation of more voids, on the other hand. In terms of maximizing the CO2/CH4 ideal separation factor, medium synthesis temperature and synthesis time (120 °C and 30 h) can be selected, however, maximum gas permeances are obtained at low levels of synthesis temperature and time (100 °C and 15 h). According to the ranges of gas permeances (10−11 to 10−6 mol/m2 s Pa) and CO2/CH4 ideal separation factors (1.4–70.3), it is concluded that the zeolite T membranes synthesized at optimum conditions can be employed for membrane separation of CO2/CH4 mixtures.  相似文献   

14.
In comparison with several other reported inorganic sorbents, Camellia tree leaf and primary sludge obtained from a settling tank as a pretreatment to the activated sludge system in a Hong Kong sewage treatment plant were evaluated for removing Cu(II) from aqueous solutions. Experimental data were modeled by the Langmuir isotherm equation to estimate the maximum sorption capacity (qmax). Results show that, at pH 5.6, biosorbents, Camellia tree leaf and primary sludge in particular, exert higher sorption capacities (qmax > 40 mg g−1) than inorganic sorbents, Na-montmorillonite (qmax = 33.3 mg g−1), fly ash (qmax = 18.8 mg g−1), and goethite powder (10.3 mg g−1). Furthermore, a pseudo second-order kinetic model was found to properly describe the experimental data for both bio- and inorganic sorbents. Sorption of Cu(II) on the Camellia tree leaf and primary sludge were much faster than that on the inorganic sorbents. In addition, desorption tests revealed that the desorption capacities of the two biomaterials are higher than the other selected materials; and much more Cu(II) can be retrieved from the Cu(II)-loaded biosorbents. Finally, increasing solution pH was found to greatly increase qmax and accelerate sorption processes.  相似文献   

15.
Chromium(VI)-containing sorbents in the form of sludge or solid residue from treatment processes are often landfilled or used as fill materials, therefore the long-term stability of metal binding is important. The reduction of Cr(VI)–Cr(III) through heat treatment may be a useful detoxification method. After heating at 500, 900, 1000, and 1100 °C for 4 h, the transformation of chemical states of chromium on 105 °C-dried, 7.9% Cr(VI)-doped TiO2 powders was studied on the basis of surface area measurements, scanning electron microscopy (SEM) images, X-ray diffraction (XRD), and extended X-ray absorption fine structure (EXAFS) spectra. It was shown that Cr(VI) was reduced to Cr(III) in the Cr(VI)-doped samples after heating within 500–900 °C. The present results also suggested that the chromium octahedral was bridged to the titanium tetrahedral and was incorporated in TiO2 minerals formed after 1000 °C treatment.  相似文献   

16.
Mesoporous magnesium oxide (MgO) was synthesized using mesoporous carbon CMK-3 obtained from mesoporous SBA-15 as exotemplate. P123 was used as the structure-directing template and rice husk ash (RHA) as the silica source for the synthesis of SBA-15, which was subsequently treated with sucrose and sulphuric acid to obtain mesoporous carbon (CMK-3). X-ray powder diffraction (XRD) results and the type-IV adsorption isotherm with H1 hysteresis obtained by N2 adsorption/desorption study for SBA-15, CMK-3 and mesoporous MgO suggests its resemblance with materials synthesized using conventional silica sources. Mesoporous MgO was subjected for CO2 adsorption study in TGA; adsorption was 8 and 10 wt% at 25 and 100 °C, respectively. Finally, mesoporous MgO is selective to CO2 gas, thermally stable and regenerable. Thus, this study contributes a better route to enhance CO2 gas adsorption and use ecological waste rice husk for the synthesis of such efficient mesoporous materials.  相似文献   

17.
Calcium oxide (CaO) is a material that is being widely investigated in the context of CO2 capture. One such application is as a CO2 sorbent in the sorption-enhanced steam methane reforming processes (SERP). CO2 is captured in an adsorption mode, where the conversion of CH4 to H2 is also enhanced, and released later in a separate desorption mode. This work presents an analysis of the relation between different process conditions and parameters during both adsorption and desorption modes. The interrelation between these conditions and the sorbent properties as well as the targeted carbon capture ratio is analysed. Conditions relevant for capturing 85% of carbon in the feed on CaO are determined and interlinked. A steam-to-carbon ratio of 4.2 has been determined to be relevant under 600 °C and 17 bar adsorption conditions. Similarly, process conditions relevant for regenerating the sorbent are determined and interlinked. For purge steam-to-CO2 ratio of 1.8 at a desorption pressure of 1 bar, relevant desorption temperature has been calculated to be 820 °C. System simulations under these adsorption and desorption conditions resulted in a system efficiency of 50.8%. Effect of tuning process operating conditions on system efficiency as well as the efficiency penalty associated with the regeneration of the sorbent are investigated by process simulations using Aspen Plus®. Possible system heat integration routes to reduce the efficiency penalty are proposed and the results of the process simulations are presented.  相似文献   

18.
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   

19.
Lignocellulosic materials are good precursors for the production of activated carbon. In this work, coffee residue has been used as raw material in the preparation of powder activated carbon by the method of chemical activation with zinc chloride for the sorption of Pb(II) from dilute aqueous solutions.The influence of impregnation ratio (ZnCl2/coffee residue) on the physical and chemical properties of the prepared carbons was studied in order to optimize this parameter. The optimum experimental condition for preparing predominantly microporous activated carbons with high pore surface area (890 m2/g) and micropore volume (0.772 cm3/g) is an impregnation ratio of 100%. The developed activated carbon shows substantial capability to sorb lead(II) ions from aqueous solutions and for relative impregnation ratios of 75 and 100%, the maximum uptake is practically the same. Thus, 75% represents the optimal impregnation ratio.Batch experiments were conducted to study the effects of the main parameters such as contact time, initial concentration of Pb(II), solution pH, ionic strength and temperature. The maximum uptake of lead(II) at 25 °C was about 63 mg/g of adsorbent at pH 5.8, initial Pb(II) concentration of 10 mg/L, agitation speed of 200 rpm and ionic strength of 0.005 M. The kinetic data were fitted to the models of pseudo-first order and pseudo-second order, and follow closely the pseudo-second order model. Equilibrium sorption isotherms of Pb(II) were analyzed by the Langmuir, Freundlich and Temkin isotherm models. The Freundlich model gives a better fit than the others.Results from this study suggest that activated carbon produced from coffee residue is an effective adsorbent for the removal of lead from aqueous solutions and that ZnCl2 is a suitable activating agent for the preparation of high-porosity carbons.  相似文献   

20.
In general, CO2 sequestration by carbonation is estimated by laboratory experimentation and geochemical simulation. In this study, however, estimation is based on a natural analogue study of the Miocene basalt in the Kuanhsi-Chutung area, Northwestern Taiwan. This region has great potential in terms of geological and geochemical environments for CO2 sequestration. Outcropping Miocene basalt in the study area shows extensive serpentinization and carbonation. The carbon stable isotopes of carbonates lie on the depleted side of the Lohmann meteoric calcite line, which demonstrates that the carbonates most probably precipitate directly from meteoric fluid, and water–rock interaction is less involved in the carbonation process. Oxygen stable isotope examinations also show much depleted ratios, representative of product formation under low temperatures (∼50–90 °C). This translates to a depth of 1–2 km, which is a practical depth for a CO2 sequestration reservoir. According to petrographic observation and electron microprobe analysis, the diopside grains in the basalt are resistant to serpentinization and carbonation; therefore, the fluid causing alteration is likely enriched with calcium and there must be additional sources of calcium for carbon mineralization. These derived geochemical properties of the fluid support the late Miocene sandstone and enclosed basalts as having high potential for being a CO2 sequestration reservoir. Moreover, the existing geochemical environments allow for mineralogical assemblages of ultramafic xenoliths, indicating that forsterite, orthopyroxene and feldspar minerals are readily replaced by carbonates. Based on the mineral transformation in xenoliths, the capacity of CO2 mineral sequestration of the Miocene basalt is semi-quantitatively estimated at 94.15 kg CO2 chemically trapped per 1 m3 basalt. With this value, total CO2 sequestration capacity can be evaluated by a geophysical survey of the amount of viable Miocene basalt at the potential sites. Such a survey is required in the near future.  相似文献   

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