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1.
The adsorption properties of N2 and CO2 of MCM-41 and derived alkali-containing samples were analyzed over a wide range of pressures (up to ~4500 kPa) and temperatures (between 30 and 300 °C). The high-pressure and high-temperature experiments were carried out on pure MCM-41 and K- and Na-impregnated derived samples. It was analyzed the influence of pressure and temperature on the CO2 capture capacity on pure and impregnated samples. The adsorption performance was correlated to the structure and textural properties of the materials using X-ray diffraction and N2 adsorption–desorption measurements. The addition of an alkaline element changes the textural properties of the material increasing the pore size, which positively affected the CO2 adsorption capacity of these materials at high pressure. In addition, the isosteric heats of adsorption gave information about the chemical affinity between the impregnated materials and CO2. The CO2 adsorption at ~ 4500 kPa for the samples with 5 wt% Na at 100 and 200 °C were 77.98 and 9.79 mmol g?1, respectively, while the pure MCM-41 adsorbs only 8.92 mmol g?1.  相似文献   

2.
Amine-modified SiO2 aerogel was prepared using 3-(aminopropyl)triethoxysilane (APTES) as the modification agent and rice husk ash as silicon source, its CO2 adsorption performance was investigated. The amine-modified SiO2 aerogel remains porous, the specific surface area is 654.24 m2/g, the pore volume is 2.72 cm3/g and the pore diameter is 12.38 nm. The amine-modified aerogel, whose N content is up to 3.02 mmol/g, can stay stable below the temperature of 300 °C. In the static adsorption experiment, amine-modified SiO2 aerogel (AMSA) showed the highest CO2 adsorption capacity of 52.40 cm3/g. A simulation was promoted to distinguish the adsorption between the physical process and chemical process. It is observed that the chemical adsorption mainly occurs at the beginning, while the physical adsorption affects the entire adsorption process. Meanwhile, AMSA also exhibits excellent CO2 adsorption–desorption performance. The CO2 adsorption capacity dropped less than 10 % after ten times of adsorption–desorption cycles. As a result, AMSA with rice husk ash as raw material is a promising CO2 sorbent with high adsorption capacity and stable recycle performance and will have a broad application prospect for exhaust emission in higher temperature.  相似文献   

3.
Hierarchical porous nitrogen-doped carbon (HPNC) materials are synthesized through one-step carbonization of polyimide using triblock copolymer P123 as mesoporous template. The microstructure, chemical composition and CO2 adsorption behaviors are investigated in detail. The results show that HPNC materials have hierarchical micro-/mesopore structures, high specific surface area of 579 m2/g, large pore volume of 0.34 cm3/g, and nitrogen functional groups (5.2 %). HPNC materials exhibit high CO2 uptake of 5.56 mmol/g at 25 °C and 1 bar, which is higher than those of previously reported nitrogen-doped porous carbon materials. After 5 cycles the value of CO2 adsorption uptakes is 5.28 mmol/g, which is approximately 95 % of the original adsorption capacity. The estimated CO2/N2 selectivity of HPNC materials is 17, revealing great promise for practical CO2 adsorption and separation applications. The efficient CO2 uptake and enhanced CO2/N2 selectivity are due to the combination of nitrogen-doped and hierarchical porous structures of HPNC materials.  相似文献   

4.
MIL-101@g-C3N4 nanocomposite was prepared by solvothermal synthesis and used for CO2 adsorption. The parent materials (MIL-101 and g-C3N4) and the MIL-101@g-C3N4 were characterized by X-ray diffraction, argon adsorption/desorption, Fourier transform infrared spectroscopy, thermal analysis (TG/DTA), transmission electronic microscopy, and Energy-dispersive X-ray spectroscopy. The results confirmed the formation of well-defined MIL-101@g-C3N4 with interesting surface area and pore volume. Furthermore, both MIL-101 and MIL-101@g-C3N4 were accomplished in carbon dioxide capture at different temperatures (280, 288, 273 and 298 K) at lower pressure. The adsorption isotherms show that the nanocomposite has a good CO2 adsorption affinity compared to MIL-101. The best adsorption capacity is about 1.6 mmol g?1 obtained for the nanocomposite material which is two times higher than that of MIL-101, indicating strong interactions between CO2 and MIL-101@g-C3N4. This difference in efficacy is mainly due to the presence of the amine groups dispersed in the nanocomposite. Finally, we have developed a simple route for the preparation of an effective and new adsorbent for the removal of CO2, which can be used as an excellent candidate for gas storage, catalysis, and adsorption.  相似文献   

5.
Ordered mesoporous carbons (OMC), were synthesized by nanocasting using ordered mesoporous silica as hard templates. Ordered mesoporous carbons CMK-1 and CMK-3 were prepared from MCM-48 and SBA-15 materials with pore diameters of 3.4 nm and 4.2 nm, respectively. Mesoporous carbons can be effectively modified for CO2 adsorption with amine functional groups due to their high affinity for CO2. Polyaniline (PANI)/mesoporous carbon nanocomposites were synthesized from in-situ polymerization by dissolving OMC in aniline monomer. The polymerization of aniline molecules inside the mesochannels of mesoporous carbons has been performed by ammonium persulfate. The nanocomposition, morphology, and structure of the nanocomposite were investigated by nitrogen adsorption-desorption isotherms, Fourier Transform Infrared (FT–IR), X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM) and thermo gravimetric analysis (TGA). CO2 uptake capacity of the mesoporous carbon materials was obtained by a gravimetric adsorption apparatus for the pressure range from 1 to 5 bar and in the temperature range of 298 to 348 K. CMK-3/PANI exhibited higher CO2 capture capacity than CMK-1/PANI owing to its larger pore size that accommodates more amine groups inside the pore structure, and the mesoporosity also can facilitate dispersion of PANI molecules inside the pore channels. Moreover, the mechanism of CO2 adsorption involving amine groups is investigated. The results show that at elevated temperature, PANI/mesoporous carbon nanocomposites have a negligible CO2 adsorption capacity due to weak chemical interactions with the carbon nanocomposite surface.  相似文献   

6.
CO2 methanation over supported ruthenium catalysts is considered to be a promising process for carbon capture and utilization and power-to-gas technologies. In this work 4% Ru/Al2O3 catalyst was synthesized by impregnation of the support with an aqueous solution of Ru(OH)Cl3, followed by liquid phase reduction using NaBH4 and gas phase activation using the stoichiometric mixture of CO2 and H2 (1:4). Kinetics of CO2 methanation reaction over the Ru/Al2O3 catalyst was studied in a perfectly mixed reactor at temperatures from 200 to 300 °C. The results showed that dependence of the specific activity of the catalyst on temperature followed the Arrhenius law. CO2 conversion to methane was shown to depend on temperature, water vapor pressure and CO2:H2 ratio in the gas mixture. The Ru/Al2O3 catalyst was later tested together with the K2CO3/Al2O3 composite sorbent in the novel direct air capture/methanation process, which combined in one reactor consecutive steps of CO2 adsorption from the air at room temperature and CO2 desorption/methanation in H2 flow at 300 or 350 °C. It was demonstrated that the amount of desorbed CO2 was practically the same for both temperatures used, while the total conversion of carbon dioxide to methane was 94.2–94.6% at 300 °C and 96.1–96.5% at 350 °C.  相似文献   

7.
The adsorption characteristics of CO2 and N2 in 13X zeolites have been studied by the molecular simulation and N2 adsorption experiment. It is found that the simulation results by Dreiding force fields are in an agreement with the published data. The influence of the σ and ε parameters of OZ and Na+ on the adsorption performance is discussed. Then the optimized force field parameters are obtained. Specific surface area (S B ) is calculated by simulation and experiment. Its relative error is just only 4.3 %. Therefore, it is feasible that S B of 13X zeolites is obtained by the simulation methods. Finally, the impacts of pressure and temperature on adsorption characteristics are investigated. At low pressure, CO2 adsorption in 13X zeolites belongs to the surface adsorption. As the pressure increase, the partial multilayer adsorption appears along with the surface adsorption. N2 adsorption in 13X zeolites is different from that of CO2. At low temperature of 77 K, two primary peaks are caused by the surface adsorption and multilayer adsorption respectively regardless of pressure variation. When the temperature is 273 K, the energy distribution curve appears undulate at low pressures. Then it becomes stable with the pressure increase. The surface adsorption plays an important role at the relative high pressures. The results will help to provide the theory guide for the optimization of force field parameters of adsorbents, and it is very important significance to understand the adsorption performance of zeolites.  相似文献   

8.
Nano CuO-Fe2O3/TiO2 adsorbents were made with different compositions of metal oxides using precipitation- desorption method. The adsorbents were applied for adsorption of SO2 at high concentrations ranging from 10,000 to 30,000 ppm and temperatures between 523 and 627 K. Adsorption experiments were applied for adsorbents in a laboratory fixed bed adsorption column. The adsorption capacity was measured by calculating the area under the adsorption curve using the integral method. The results showed that temperature is the most affecting factor on the adsorption capacity. The highest adsorption capacity was obtained by using 17, 8 and 75 wt% of CuO, Fe2O3 and nano TiO2, respectively. Characteristics of the best sorbent were determined by using Fe-SEM, XRD and nitrogen adsorption-desorption analyses.  相似文献   

9.
Copolymers based on glassy and rubbery units have been developed to take advantage of both domains to enhance solubility and diffusivity. In this study, a series of gas separation membranes from polysulfone (PSF) containing ethylene glycol were synthesized via nucleophilic substitution polycondensation. The structures of copolymers were characterized by nuclear magnetic resonance spectra, Fourier transform infrared spectra, and thermal gravity analysis. The permeability and selectivity of the membranes were studied at different temperatures of 25–55 °C and pressures of 0.5–1.5 atm using single gases CO2 and CH4. Gas permeation measurements showed that copolymers with different contents of poly(ethylene glycol) exhibited different separation performances. For example, the membrane from PSF-PEG2000-20 containing 20 wt% poly(ethylene glycol) showed better performance in terms of ideal selectivity over the other seven copolymer membranes. The highest ideal CO2/CH4 selectivity was 43.0 with CO2 permeability of 6.4 Barrer at 1.5 atm and 25 °C.  相似文献   

10.
Adsorption of CO2 and CO at 25 °C has been conducted using commercially-available (Y, ZSM-5) and laboratory-synthesized (SSZ-13, SAPO-34) H-zeolites with different framework topologies and chemical compositions, and their textual and surface properties have been characterized by N2 sorption and NH3 adsorption techniques. All the zeolites were microporous, although ZSM-5 and SSZ-13 apparently showed a mesoporous sorption behavior due to the interparticle spaces. The zeolites had Si/Al values in the order of SSZ-13 (16.44) > ZSM-5 (16.08) ? Y (2.82) ? SAPO-34 (0.19). Regardless, high CO2 adsorption capacity was obtained for SSZ-13 and SAPO-34 with a CHA framework. The FAU zeolite Y with the highest micropore volume showed less CO2 adsorption than the CHA zeolites and the MFI-type ZSM-5 yielded the poorest performance. Probing acid sites in the H-form zeolites using NH3 disclosed that these all contain both weak and strong acid sites with significant dependence of their strengths and amounts on the topology. The acid strength of the weak acid sites in the CHA zeolites was the weakest, which might allow a stronger interaction with CO2. The H-zeolites gave CO2/CO selectivity factors that were in the range of 4.61–11.0, depending on the framework topology.  相似文献   

11.
0.1 Fe/Ti mole ratio of Fe-TiO2 catalysts were synthesized via solvothermal method and calcined at various temperatures: 300, 400, and 500 °C. The calcined catalysts were characterized by XRD, N2-adsorption-desorption, UV-DRS, XRF, and Zeta potential and tested for photocatalytic degradation of alachlor under visible light. The calcined catalysts consisted only of anatase phase. The BET specific surface area decreased with the calcination temperatures. The doping Fe ion induced a red shift of absorption capacity from UV to the visible region. The Fe-TiO2 calcined at 400 °C showed the highest photocatalytic activity on degradation of alachlor with assistance of 30 mM H2O2 at pH 3 under visible light irradiation. The degradation fitted well with Langmuir-Hinshelwood model that gave adsorption coefficient and the reaction rate constant of 0.683 L mg−1 and 0.136 mg/L·min, respectively.  相似文献   

12.
Nanoporous silica membrane without any pinholes and cracks was synthesized by organic templating method. The tetrapropylammoniumbromide (TPABr)-templating silica sols were coated on tubular alumina composite support ( γ-Al2O3/ α-Al2O3 composite) by dip coating and then heat-treated at 550 °C. By using the prepared TPABr templating silica/alumina composite membrane, adsorption and membrane transport experiments were performed on the CO2/N2, CO2/H2 and CH4/H2 systems. Adsorption and permeation by using single gas and binary mixtures were measured in order to examine the transport mechanism in the membrane. In the single gas systems, adsorption characteristics on the α-Al2O3 support and nanoporous unsupport (TPABr templating SiO2/ γ-Al2O3 composite layer without α-Al2O3 support) were investigated at 20–40 °C conditions and 0.0–1.0 atm pressure range. The experimental adsorption equilibrium was well fitted with Langmuir or/and Langmuir-Freundlich isotherm models. The α-Al2O3 support had a little adsorption capacity compared to the unsupport which had relatively larger adsorption capacity for CO2 and CH4. While the adsorption rates in the unsupport showed in the order of H2> CO2> N2> CH4 at low pressure range, the permeate flux in the membrane was in the order of H2≫N2> CH4> CO2. Separation properties of the unsupport could be confirmed by the separation experiments of adsorbable/non-adsorbable mixed gases, such as CO2/H2 and CH4/H2 systems. Although light and non-adsorbable molecules, such as H2, showed the highest permeation in the single gas permeate experiments, heavier and strongly adsorbable molecules, such as CO2 and CH4, showed a higher separation factor (CO2/H2=5-7, CH4/H2=4-9). These results might be caused by the surface diffusion or/and blocking effects of adsorbed molecules in the unsupport. And these results could be explained by surface diffusion. This paper is dedicated to Professor Hyun-Ku Rhee on the occasion of his retirement from Seoul National University.  相似文献   

13.
A sulfonic acid functionalized titanium dioxide quasi-superparamagnetic nanocatalyst Fe3O4@SiO2@TiO2-OSO3H with average size of 61 nm and semispherical shape with surface area about 97 m2 g?1 with saturation magnetization 17.7 emu g?1 and the coercivity 9.84 Oe was successfully synthesized. The structure and morphology of the nanocatalyst was characterized by Fourier transform infrared spectroscopy (FT-IR), energy-dispersive X-ray spectroscopy, X-ray diffraction pattern, transmission electron microscopy, field-emission scanning electron microscopy, vibrating sample magnetometer and Brunauer–Emmett–Teller surface area analysis. The catalytic usage of the nanocatalyst was exemplified in synthesis of 2,3-dihydroquinazolin-4(1H)-one and spiroquinazolin-4(3H)-one derivatives in deep eutectic solvents (DESs) based on choline chloride and urea. We suggest that the synergistic effects in catalytic activities of titanium dioxide, organic acid and the CO2 capture property of DES are the main reasons for the improvement of catalytic activity. The synthesized spiroquinazolinones and dihydroquinazolinones derivatives were characterized by FT-IR, 1H and 13C nuclear magnetic resonance spectroscopy. The magnetic nanocatalyst exhibit high catalytic activity and can be simply separated from reaction media by an external magnet in a few seconds and could be reused for six cycles without significant loos in activity, which indicates the good immobilization of sulfonic acid on the magnetic titanium dioxide support. Furthermore, the solvent which has been used in this work can be readily isolated and reused for several times.  相似文献   

14.
In this work, TiO2 has been modified by treating it thermally together with different proportions (0.5–15 wt%) of La2O3. The resulting materials have been extensively characterized by XRD, TEM, N2 adsorption isotherms, temperature-programmed CO2 desorption, Raman, UV–Vis photoluminescence and X-ray photoelectron spectroscopies. The activity tests of these materials for the gas-phase photocatalytic reduction of carbon dioxide show that the main products of the reaction are in all cases CO and CH4, together with H2 from the parallel reduction of water. After the preparation procedure, La phases are best described as oxycarbonates, and lead to improved activity with respect to TiO2 with La contents up to 5 wt%. Higher loadings do not, however, lead to further enhanced activity. Retarded electron–hole recombination and enhanced CO2 adsorption are invoked as the key factors contributing to this activity improvement, which is optimized in the case of 0.5 wt% La leading to higher productions of CO and CH4 and increased quantum efficiency with respect to titania.  相似文献   

15.
A lithium insertion material having the composition LiNi0.3Co0.3Mn0.3Fe0.1O2 was synthesized by simple sol-gel method. The structural and electrochemical properties of the sample were investigated using X-ray diffraction spectroscopy (XRD) and the galvanostatic charge-discharge method. Rietvelt analysis of the XRD patterns shows that this compound can be classified as α-NaFeO2 structure type (R3m; a=2.8689(5) Å and 14.296(5) Å in hexagonal setting). Rietvelt fitting shows that a relatively large amount of Fe and Ni ion occupy the Li layer (3a site) and a relatively large amount of Li occupies the transition metal layer (3b site). LiNi0.3Co0.3Mn0.3Fe0.1O2 when cycled in the voltage range 4.3–2.8 V gives an initial discharge capacity of 120 mAh/g, and stable cycling performance. LiNi0.3Co0.3Mn0.3Fe0.1O2 in the voltage range 2.8–4.5 V has a discharge capacity of 140 mAh/g, and exhibits a significant loss in capacity during cycling. Ex-situ XRD measurements were performed to study the structure changes of the samples after cycling between 2.8–4.3 V and 2.8–4.5 V for 20 cycles. The XRD and electrochemical results suggested that cation mixing in this layered structure oxide could be causing degradation of the cell capacity.  相似文献   

16.
An amine functional MIL-53(Al) material was prepared through a clean, rapid, energy-efficient method of microwave and ultrasound irradiation. The pure phase NH2-MIL-53(Al) can be formed in 25 min, utilizing the synergistic effect of microwave and ultrasound irradiation. The dramatic acceleration in reaction rates suggested that the removal of a passivation coating on the substrate particles and the resultant enhancement in mass and heat transfer. The porous MOFs exhibited a high thermal and chemical stability, decomposing at temperatures above 410 °C in air. The NH2-MIL-53(Al) performed an excellent adsorption for CO2. The CO2 capacities up to 33.86 cm3 g?1 at 298 K at low pressures, which suggests chemisorption between CO2 and pendan amine groups. Measurement of CO2 adsorption cycles proved that the functionalized materials show good regenerability and stability.  相似文献   

17.
The conditions for the formation of a spinel structure from a NiO–CuO–Fe2O3–Cr2O3 oxide mixture using several technological approaches have been examined. Addition of KCl is accompanied with the formation of two spinel-like phases, whereas in the absence of KCl just one solid solution of nickel–copper ferrite–chromite with the structure of a cubic spinel is formed. At the temperature of thermal treatment of 900°C, the presence of an admixture phase of the delafossite (CuCrO2) type was established. The conditions for the fabrication of samples containing two spinel phases (cubic and tetragonal) characterized with the most developed surface and manifesting = increased catalytic activity in the reaction of the decomposition of an organic substance by hydrogen peroxide have been formulated. The studied features of spinel synthesis can be of interest for developing materials with an active surface promising for application as adsorbents of catalysts and sensors.  相似文献   

18.
The following investigation reports the synthesis of novel complex [Fe(opd)3]2[Ba(CN)8] and preparation of BaFe2O4 nanoparticles through thermal decomposition without using any surfactant. The complex was characterized via Furrier transform infrared spectroscopy (FT-IR), ultra violet-visible spectroscopy (UV–vis), conductivity measurement and elemental analysis. The synthesized crystals of inorganic precursor complex was transferred to furnace, where they were calcined under normal atmosphere condition at 900 °C for 4 h. Formation of BaFe2O4 was supported by FT-IR and energy-dispersive X-ray analysis. Hexagonal structure of nano-oxide was confirmed on powder X-ray diffraction. Furthermore, uniform morphology of nanocrystals were reported by scanning electron microscopy. The saturation magnetization (22 emu/g), remanent magnetization (6 emu/g) and coercivity (400 Oe) reported on vibrating sample magnetometer curve illustrates the promising industrial and medicinal applications of prepared mixed oxide.  相似文献   

19.
LaBO3/attapulgite (ATP) (B=Mn, Fe, Co, Ni) composites were prepared by sol–gel method using citric acid as complex agent. The products were characterized by X-ray diffraction transmission electron microscopy, energy-dispersive spectroscopy, Battett–Emmett–Teller, fourier-transform infrared, H2 temperature-programmed reduction and temperature-programmed desorption of NH3 measurements. The catalytic activity of LaBO3/ATP nanocomposites was evaluated via selective catalytic reduction of NO with NH3 by fixed bed denitration equipment at low-temperature. The impact of the various B-site elements on the NO conversion was investigated. Results showed that the adsorption capacity of NH3 played significant role in the low temperature denitrification process, and Mn was the best B-site element where LaMnO3/ATP achieves 81% conversion of NO at 250 °C.  相似文献   

20.
Aluminum terephthalate, MIL-53(Al), metal–organic framework synthesized hydrothermally and purified by solvent extraction method was used as an adsorbent for gas adsorption studies. The synthesized MIL-53(Al) was characterized by powder X-Ray diffraction analysis, surface area measurement using N2 adsorption–desorption at 77 K, FTIR spectroscopy and thermo gravimetric analysis. Adsorption isotherms of CO2, CH4, CO, N2, O2 and Ar were measured at 288 and 303 K. The absolute adsorption capacity was found in the order CO2>CH4>CO>N2>Ar>O2. Henry’s constants, heat of adsorption in the low pressure region and adsorption selectivities for the adsorbate gases were calculated from their adsorption isotherms. The high selectivity and low heat of adsorption for CO2 suggests that MIL-53(Al) is a potential adsorbent material for the separation of CO2 from gas mixtures. The high selectivity for CH4 over O2 and its low heat of adsorption suggests that MIL-53(Al) could also be a compatible adsorbent for the separation of methane from methane–oxygen gas mixtures.  相似文献   

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