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1.
通过溶胶-凝胶法制备了石墨烯水凝胶, 并将其与高氯酸铵(AP)复合, 然后分别采用自然干燥、冷冻干燥和超临界CO2干燥三种干燥方式制备了AP/石墨烯复合材料, 并通过扫描电镜(SEM)、元素分析、X射线衍射(XRD)、差示扫描量热仪(DSC)和热重-红外联用技术(TG-FTIR)研究了不同干燥方式对其结构和热分解行为的影响. 结果表明, 干燥方式对AP/石墨烯复合材料的形貌具有明显影响, 其中通过超临界CO2干燥制备的AP/石墨烯复合材料基本能保持与石墨烯气凝胶相似的外观和多孔结构. 通过自然干燥、冷冻干燥和超临界CO2干燥制备的AP/石墨烯复合材料中AP的质量分数分别为89.97%、92.41%和94.40%, 其中通过超临界CO2干燥制备的复合材料中AP的粒径尺寸为69 nm. DSC测试结果表明, 石墨烯对AP的热分解过程具有明显的促进作用, 能使AP的低温分解过程大大减弱, 高温分解峰温明显降低. 三种干燥方式相比, 通过超临界CO2干燥制备的AP/石墨烯复合材料中石墨烯的促进作用最明显. 与纯AP相比, 其高温分解峰温降低了83.7℃, 表观分解热提高到2110 J·g-1. TG-FTIR分析结果表明, AP/石墨烯复合材料的热分解过程中, AP分解产生的氧化性产物与石墨烯发生了氧化反应, 生成了CO2.  相似文献   

2.
Waste ion-exchange resin was utilized as precursor to produce activated carbon by KOH chemical activation, on which the effects of different activation temperatures, activation times and impregnation ratios were studied in this paper. The CO2 adsorption of the produced activated carbon was tested by TGA at 30 °C and environment pressure. Furthermore, the effects of preparation parameters on CO2 adsorption were investigated. Experimental results show that the produced activated carbons are microporous carbons, which are suitable for CO2 adsorption. The CO2 adsorption capacity increases firstly and then decreases with the increase of activation temperature, activation time and impregnation rate. The maximum adsorption capacity is 81.24 mg/g under the condition of 30 °C and pure CO2. The results also suggest that waste ion-exchange resin-based activated carbons possess great potential as adsorbents for post-combustion CO2 capture.  相似文献   

3.
Environmental concerns and oil price rises and dependency promoted strong research in alternative fuel sources and vectors. Fischer-Tropsch products are considered a valid alternative to oil derivatives having the advantage of being able to share current infrastructures. As a renewable source of energy, synthesis gas obtained from biomass gasification presents itself as a sustainable alternative. However, prior to hydrocarbon conversion, the bio-syngas must be conditioned, which includes the removal of carbon dioxide for subsequent sequestration and capture. A pressure swing adsorption cycle was developed for the removal and concentration of CO2 from the bio-syngas stream. Activated carbon was chosen as adsorbent. The simulation results showed that it was possible to produce a (H2 + CO) product with a H2/CO stoichiometric ratio of 2.14 (suitable as feed stream for the Fischer-Tropsch reactor) and a CO2 product with a purity of 95.18%. A CO2 recovery of 90.3% was obtained. A power consumption of 3.36 MW was achieved, which represents a reduction of about 28% when compared to a Rectisol process with the same recovery.  相似文献   

4.
Potassium-based sorbents using γ-Al2O3 or TiO2 as a support or an additive material have disadvantages in terms of their thermal stability and cyclic CO2 capture. To overcome the shortcomings of these sorbents, a novel potassium-based sorbent (KSnI30) using SnO2 was developed in this study. The KSnI30 sorbent formed only K2CO3 and SnO2 phases without any inactive alloy species even after calcination at high temperatures (500–700 °C), indicating the good thermal stability of the KSnI30 sorbent regardless of the calcination temperature. Furthermore, the KSnI30 sorbent has an excellent regeneration property (above 98 %), as well as high CO2 capture capacities (89–94 mg CO2/g sorbent). Its excellent regeneration property is due to the formation of a KHCO3 phase without by-products during CO2 sorption. These results of the present study demonstrate that the SnO2 shows promise as a new support or an additive material to replace TiO2 and γ-Al2O3 in the preparation of a regenerable potassium-based sorbent for post-combustion CO2 capture with good thermal stability and excellent regeneration property.  相似文献   

5.
Titania–silica composite have been prepared using polyethylene glycol (PEG) with different molecular weights (M w), PEG20000, PEG10000, and PEG2000, as template in supercritical carbon dioxide (SC CO2). The composite precursors were dissolved in SC CO2 and impregnated into PEG templates using SC CO2 as swelling agent and carrier. After removing the template by calcination at suitable temperature, the titania–silica composite were obtained. The composite were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, and nitrogen sorption–desorption experiment. Photocatalytic activity of the samples has been investigated by photodegradation of methyl orange. Results indicate that there are many Si–O–Ti linkages in the TiO2/SiO2 composite; the PEG template has a significant influence on the structure of TiO2/SiO2. In addition, the TiO2/SiO2 prepared with PEG10000 exhibited high photocatalytic efficiency. So this work supplies a clue to control and obtain the TiO2/SiO2 composite with different photocatalytic reactivity with the aid of suitable PEG template in supercritical CO2.  相似文献   

6.
The effect of the H2O/CO2 and EtOH/CO2 media at pressures and temperatures corresponding to the formation of supercritical (sc) carbon dioxide on the structure and mechanical properties of bovine jugular veins was studied for the first time. Treatment of bovine jugular veins in an sc-CO2 + ethanol or sc-CO2 + water medium considerably devitalized the tissue and increased the tissue elasticity, which allows considering the treated veins as promising vascular grafts with expected high capacity to suppress calcification and good hemodynamic properties.  相似文献   

7.
This experimental study of phase equilibria in the K2SO4-K2CO3-H2O system at 385–500°C and pressures up to 100 MPa is directed to determine the sequence of phase transformations that generate heterogeneous supercritical fluids from the homogeneous one; the homogeneous supercritical region spreads into the ternary system from the K2SO4-H2O subsystem. We found that heterogenization of supercritical fluid upon addition of K2CO3 starts with l1=l2 critical phenomena in solid saturated solutions and is attended by amalgamation of the stable immiscibility region that spreads from the K2CO3-H2O system with the metastable immiscibility region that originates from the K2SO4-H2O system. Our experimental results and the topological analysis of phase equilibria at temperatures above the critical point of water gave us the full scenario of the phase behavior of the title ternary system in the regions of fluid equilibria, g=l and l1=l2 critical phenomena, and liquid-liquid phase separation in two-, three-, and four-phase equilibria.  相似文献   

8.
Vacuum pressure swing adsorption (VPSA) for CO2 capture has attracted much research effort with the development of the novel CO2 adsorbent materials. In this work, a new adsorbent, that is, pitch-based activated carbon bead (AC bead), was used to capture CO2 by VPSA process from flue gas. Adsorption equilibrium and kinetics data had been reported in a previous work. Fixed-bed breakthrough experiments were carried out in order to evaluate the effect of feed flowrate, composition as well as the operating pressure and temperature in the adsorption process. A four-step Skarstrom-type cycle, including co-current pressurization with feed stream, feed, counter-current blowdown, and counter-current purge with N2 was employed for CO2 capture to evaluate the performance of AC beads for CO2 capture with the feed compositions from 15–50% CO2 balanced with N2. Various operating conditions such as total feed flowrate, feed composition, feed pressure, temperature and vacuum pressure were studied experimentally. The simulation of the VPSA unit taking into account mass balance, Ergun relation for pressure drop and energy balance was performed in the gPROMS using a bi-LDF approximation for mass transfer and Virial equation for equilibrium. The simulation and experimental results were in good agreement. Furthermore, two-stage VPSA process was adopted and high CO2 purity and recovery were obtained for post-combustion CO2 capture using AC beads.  相似文献   

9.
The effect of sintering on the maximum capture efficiency of CO2 is studied, using a carbonation/calcination cycle for a series of samples with different stoichiometries of dolomite and calcite. For the materials that belong to the categories of limestone and dolomitic limestone, sintering decreases the extent of carbonation significantly at the two different highest temperatures studied. The extent of carbonation for the same maximum heating temperature depends mainly on the percentage of dolomite. Sintering is negligible in the dolomitic rocks, especially at the maximum heating temperature of 1005°C. The composition of the carrier gas does not seem to play a significant role. The reduction of the extent of carbonation at the second heating /cooling cycle in limestone, and the durability after enough successive cycles of calcination/carbonation in the dolomitic rocks, does not seem to be affected by the maximum temperatures of calcination that were used at the experiments.  相似文献   

10.
Bacterial cellulose aerogels overcome the drawback of shrinking during preparation by drying with supercritical CO2. Thus, the pore network of these gels is fully accessible. These materials can be fully rewetted to 100% of its initial water content, without collapsing of the structure due to surface tension of the rewetting solvent. This rehydration property and the high pore volume of these material rendered bacterial cellulose aerogels very interesting as controlled release matrices. Supercritical CO2 drying, the method of choice for aerogel preparation, can simultaneously be used to precipitate solutes within the cellulose matrix and thus to load bacterial cellulose aerogels with active substances. This process, frequently termed supercritical antisolvent precipitation, is able to perform production of the actual aerogel and its loading in one single preparation step. In this work, the loading of a bacterial cellulose aerogel matrix with two model substances, namely dexpanthenol and L-ascorbic acid, and the release behavior from the matrix were studied. A mathematical release model was applied to model the interactions between the solutes and the cellulose matrix. The bacterial cellulose aerogels were easily equipped with the reagents by supercritical antisolvent precipitation. Loading isotherms as well as release kinetics indicated no specific interaction between matrix and loaded substances. Hence, loading and release can be controlled and predicted just by varying the thickness of the gel and the solute concentration in the loading bath.  相似文献   

11.
Electrocatalytic reduction of CO2 is a promising route for energy storage and utilization. Herein we synthesized SnO2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first time. The SnO2 and N-PC in the SnO2@N-PC composites had exellent synergistic effect for electrocatalytic reduction of CO2 to HCOOH. The Faradaic efficiency of HCOOH could be as high as 94.1% with a current density of 28.4 mA cm?2 in ionic liquid-MeCN system. The reaction mechanism was proposed on the basis of some control experiments. This work opens a new way to prepare composite electrode for electrochemical reduction of CO2.  相似文献   

12.
A H3PW12O40/ZrO2 catalyst for effective dimethyl carbonate (DMC) formation via methanol carbonation was prepared using the sol–gel method. X-ray photoelectron spectra showed that reactive and dominant (63%) W(VI) species, in WO3 or H2WO4, enhanced the catalytic performances of the supported ZrO2. The mesoporous structure of H3PW12O40/ZrO2 was identified by nitrogen adsorption–desorption isotherms. In particular, partial sintering of catalyst particles in the duration of methanol carbonation caused a decrease in the Brunauer–Emmett–Teller surface area of the catalyst from 39 to 19 m2/g. The strong acidity of H3PW12O40/ZrO2 was confirmed by the desorption peak observed at 415 °C in NH3 temperature-programmed desorption curve. At various reaction temperatures (T?=?110, 170, and 220 °C) and CO2/N2 volumetric flow rate ratios (CO2/N2?=?1/4, 1/7, and 1/9), the calculated catalytic performances showed that the optimal methanol conversion, DMC selectivity, and DMC yield were 4.45, 89.93, and 4.00%, respectively, when T?=?170 °C and CO2/N2?=?1/7. Furthermore, linear regression of the pseudo-first-order model and Arrhenius equation deduced the optimal rate constant (4.24?×?10?3 min?1) and activation energy (Ea?=?15.54 kJ/mol) at 170 °C with CO2/N2?=?1/7 which were favorable for DMC formation.  相似文献   

13.
The dependent relation between temperature and pressure of supercritical CO2+ ethanol binary system under the pressure range from 5 to 10 MPa with the variety of densities and mole fractions of ethanol that range from 0 to 2% was investigated by the static visual method in a constant volume. The critical temperature and pressure were experimentally determined simultaneously. The PTρ figures at different ethanol contents were described based on the determined pressure and temperature data, from which pressure of supercritical CO2 + ethanol binary system was found to increase linearly with the increasing temperature. P-T lines show certain convergent feature in a specific concentration of ethanol and the convergent points shift to the region of higher temperature and pressure with the increasing ethanol compositions. Furthermore, the effect of density and ethanol concentration on the critical point of CO2 + ethanol binary system was discussed in details. Critical points increase linearly with the increasing mole fraction of ethanol in specific density and critical points change at different densities. The critical compressibility factors Zc of supercritical CO2 + ethanol binary systems at different compositions of ethanol were calculated and Z c figure was obtained accordingly. It was found from Z c figure that critical compressibility factors of supercritical CO2 unitary or binary systems decline linearly with the increasing density, by which the critical point can be predicted precisely.  相似文献   

14.
A comparative analysis of properties of SiO2–TiO2 binary aerogels prepared by supercritical drying using different supercritical fluids (isopropanol, hexafluoroisopropanol, methyl tert-butyl ether, and CO2) has been performed. The use of different supercritical fluids allows preparation of both homogeneous amorphous SiO2–TiO2 binary aerogels (by supercritical drying in hexafluoroisopropanol and CO2) and composite aerogels containing nanocrystalline anatase (by supercritical drying in isopropanol and methyl tert-butyl ether). The thermal treatment of the aerogels at temperatures up to 600°C does not lead to considerable change in the porous structure and phase composition of the aerogels.  相似文献   

15.
Chiu KH  Yak HK  Wai CM  Lang Q 《Talanta》2005,65(1):149-154
Packed in a high-pressure vessel and under calculated conditions, dry ice can be used as a source of carbon dioxide for supercritical CO2 extraction or liquid CO2 of organic compounds from environmental samples. Coupled with a fluid modifier such as toluene, dry ice-originated supercritical CO2 (Sc CO2) achieves quantitative extraction of many volatile organic compounds (VOCs) and semivolatile organic compounds (SOCs) including polycyclic aromatic hydrocarbons (PAHs), n-alkanes, and polychlorinated biphenyls (PCBs) from solid matrices. Compared to contemporary manual or automated supercritical fluid extraction (SFE) technologies, this novel technique simplifies SFE to a minimum requirement by eliminating the need of a high-pressure pump and any electrical peripherals associated with it. This technique is highly suitable to analytical areas where sample preservation is essential but difficult in the sampling field, or where sample collection, sample preparation, and analysis are to be done in the field.  相似文献   

16.
Dry potassium-based sorbents were prepared by impregnation with potassium carbonate on supports such as activated carbon (AC), TiO2, Al2O3, MgO, CaO, SiO2 and various zeolites. The CO2 capture capacity and regeneration property of various sorbents were measured in the presence of H2O in a fixed bed reactor, during multiple cycles at various temperature conditions (CO2 absorption at 50–100 °C and regeneration at 130–400 °C). The KAlI30, KCaI30, and KMgI30 sorbents formed new structures such as KAl(CO3)2(OH)2, K2Ca(CO3)2, K2Mg(CO3)2, and K2Mg(CO3)2·4(H2O), which did not completely convert to the original K2CO3 phase at temperatures below 200 °C, during the CO2 absorption process in the presence of 9 vol.% H2O. In the case of KACI30, KTiI30, and KZrI30, only a KHCO3 crystal structure was formed during CO2 absorption. The formation of active species, K2CO3·1.5H2O, by the pretreatment with water vapor and the formation of the KHCO3 crystal structure after CO2 absorption are important factors for absorption and regeneration, respectively, even at low temperatures (130–150 °C). In particular, the KTiI30 sorbent showed excellent characteristics with respect to CO2 absorption and regeneration in that it satisfies the requirements of a large amount of CO2 absorption (87 mg CO2/g sorbent) without the pretreatment with water vapor, unlike KACI30, and a fast and complete regeneration at a low temperature condition (1 atm, 150 °C). In addition, the higher total CO2 capture capacity of KMgI30 (178.6 mg CO2/g sorbent) than that of the theoretical value (95 mg CO2/g sorbent) was explained through the contribution of the absorption ability of MgO support. In this review, we introduce the CO2 capture capacities and regeneration properties of several potassium-based sorbents, the changes in the physical properties of the sorbents before/after CO2 absorption, and the role of water vapor and its effects on CO2 absorption.  相似文献   

17.
Olivine LiFePO4 is challenged by its poor electronic and ionic conductivities for lithium-ion batteries. Polyethylene glycol (PEG) has been applied for LiFePO4 preparation by different research groups, but there is no consensus on the influence of the mean molecular weight of PEG on the structure and electrochemical performances of LiFePO4/C composites. In this work, LiFePO4/C composites were prepared by using micronsized FePO4·2H2O powder as starting material, PEG (mean molecular weight of 200, 400, 4000 or 10000) and citric acid as complex carbon source. The structure and electrochemical performances of LiFePO4/C composites would be decided considerably by the mean molecular weight of PEG, and the sample using PEG200 exhibited the least inter-particle agglomeration, the smallest charge transfer resistance and the highest discharge capacity. A probable growth mechanism is also proposed based on SEM images and electrochemical results: with the assistance of citric acid, PEG molecule with small molecular weight tends to cover one or only a few micron-sized FePO4·2H2O particles, significantly suppress the agglomeration of primary LiFePO4 particles and thus result in uniform particle-size distribution and carbon coating.  相似文献   

18.
Two series of zeolite X/activated carbon composites with different ratios of zeolite and activated carbon were prepared through a combination process of CO2 activation of the mixtures of elutrilithe and pitch and subsequent hydrothermal crystallization in alkaline solution. An additional surface modification was achieved in diluted NH4Cl solution. CO2 and N2 uptakes on the composites before and after modification were determined for pressures up to 101?kPa at 273 and 298?K, respectively. Langmuir-Freundlich and Toth adsorption models were used to describe the adsorption isotherms of CO2 and the corresponding heats of adsorption were estimated with the Clausius-Clapeyron equation. Both before and after modification, all composites exhibited a remarkable preferential adsorption of CO2 compared to N2, with the modified composites showing a higher adsorption selectivity to CO2 over N2 than the unmodified composites. With an increasing ratio of zeolite in the composites, adsorption capacity and adsorption heat of CO2 on the composites increased simultaneously. Lower adsorption heat was observed both before and after modification especially at the low-loading region and when there was less energetic heterogeneity on the surface of the modified composites. The results may be attributed to the elimination of strong basic sites on the modified composites, which is favorable for desorption of CO2 on the adsorbents and application in pressure swing adsorption processes.  相似文献   

19.
The effects of the sorption and the regeneration temperatures on the performance of a novel rapid thermal swing chemisorption (RTSC) process (Lee and Sircar in AIChE J. 54:2293–2302, 2008) for removal and recovery of CO2 from an industrial flue gas without pre-compression, pre-drying, or pre-cooling of the gas were mathematically simulated. The process directly produced a nearly pure, compressed CO2 by-product stream which will facilitate its subsequent sequestration. Na2O promoted alumina was used as the CO2 selective chemisorbent, and the preferred temperatures were found to be, respectively, 150 and 450 °C for the sorption and regeneration steps of the process. The specific cyclic CO2 production capacity of the process and the pressure of the by-product CO2 gas were substantially increased over those previously achieved by using the sorption and regeneration temperature of, respectively, 200 and 500 °C (Lee and Sircar in AIChE J. 54:2293–2302, 2008). The net compressed CO2 recovery from the flue gas (∼92%) did not change. However, substantially different amounts of high and low pressure steam purges were necessary for comparable degree of desorption of CO2. A first pass estimation of the capital and the operating costs of the RTSC process was carried out for a relatively moderate size application (flue gas clean up and CO2 recovery from a ∼80 MW coal fired power plant). Both costs were substantially lower than those for a conventional absorption process using MEA as the CO2 solvent (Desideri and Paolucci in Energy Convers. Manag. 40:1899–1915, 1999).  相似文献   

20.
During the formation of pastes, mortar and concretes have been used to capture CO2. This work presents a methodology to estimate the carbon dioxide (CO2) sequestered by high strength and sulfate-resistant Portland cement pastes during their early stages of hydration, by Thermogravimetry and Derivative Thermogravimetry. Water to cement ratio equal to 0.50 and 0.70 were evaluated and the captured CO2 amount was determined through TG/DTG curve data on initial cement mass basis, obtained during accelerated carbonation from the fluid state and accelerated carbonation after a first hydration process. The experiments were performed in a controlled chamber, maintaining the CO2 content at 20 vol % and the temperature at 25 °C, at different relative humidity (RH) (60 and 80 %) ambient. The procedure allows one to estimate the amount of CO2 sequestered by the initial cement mass of a given volume of paste, as well as to evaluate the RH and W/C ratio influence on the amount of hydrated formed products, mainly on the Ca(OH)2, important for CO2 fixation.  相似文献   

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