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1.
Novel low-temperature swing adsorbents that preferably adsorb CO2 were synthesized by varying loading of heteropolyacid Fe1.5PMo12O40 (Fe–PMA) supporting on mesoporous cellular foams (MCFs) by wetting impregnation. The synthesized materials were characterized by various physicochemical, thermal and spectral techniques and the CO2 adsorption capacity of the materials were evaluated. Solid adsorbents showed a significantly high adsorption capacity toward CO2 due to the chemisorptions of CO2. The CO2 adsorption capacities of the materials decreased as the temperature increased. The results showed that the adsorption capacity reached a level of 81.8 mg CO2/g-adsorbent at 25 °C for the 20 wt% Fe–PMA–MCFs. These results indicated that the iron (Fe2+) complexes acted as efficient catalysts for the separation of CO2. The as-synthesized adsorbents were selective, thermally stable, long-lived, and could be recycled at a temperature of 110 °C.  相似文献   

2.
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   

3.
Herein, we studied the influence of calcination temperature (500–800 °C) of Ni/CeO2 and Ni/Ce0.8Zr0.2O2 catalysts on the specific surface area, pore volume, crystalline size, lattice parameter, chemical bonding and oxidation states, nickel dispersion and CH4/CO production rate in CO2 methanation. In general, the catalytic performance revealed that Zr doping catalysts could increase the CH4 production rate. Combined with the production rate and the characterizations results, we found that the combination of nickel dispersion, peak area of CO2–TPD and OII/(OII + OI)) play the critical role in increasing the CH4 production rate. It is well to be mentioned that the CO production rate is strongly influenced by the nickel dispersion. Furthermore, the in-situ DRIFTS confirmed that the CO originates from the decomposition of H-assisted formate species.  相似文献   

4.
The electrochemical route is a promising and environmentally friendly technique for fabrication of metal organic frameworks (MOFs) due to mild synthesis condition, short time for crystal growth and ease of scale up. A microstructure Cu3(BTC)2 MOF was synthesized through electrochemical path and successfully employed for CO2 and CH4 adsorption. Characterization and structural investigation of the MOF was carried out by XRD, FE-SEM, TGA, FTIR and BET analyses. The highest amount of carbon dioxide and methane sorption was 26.89 and 6.63 wt%, respectively, at 298 K. The heat of adsorption for CO2 decreased monotonically, while an opposite trend was observed for CH4. The results also revealed that the selectivity of the developed MOF towards CO2 over CH4 enhanced with increase of pressure and composition of carbon dioxide component as predicted by the ideal adsorption solution theory (IAST). The regeneration of as-synthesized MOF was also studied in six consecutive cycles and no considerable reduction in CO2 adsorption capacity was observed.  相似文献   

5.
A K-promoted 10Ni-(x)K/MgAl2O4 catalyst was investigated for the combined H2O and CO2 reforming (CSCR) of coke oven gas (COG) for syngas production. The 10Ni-(x)K/MgAl2O4 catalyst was prepared by co-impregnation, and the K content was varied from 0 to 5 wt%. The BET, XRD, H2-chemisorption, H2-TPR, and CO2-TPD were performed for determining the physicochemical properties of prepared catalysts. Except under the condition of a K/Ni=0.1 (wt%/wt%), the Ni crystal size and dispersion decreased with increasing K/Ni. The coke resistance of the catalyst was investigated under conditions of CH4: CO2: H2: CO:N2=1 : 1 : 2 : 0.3 : 0.3, 800 °C, 5 atm. The coke formation on the used catalyst was examined by SEM and TG analysis. As compared to the 10Ni/MgAl2O4 catalyst, the Kpromoted catalyst exhibited superior activity and coke resistance, attributed to its strong interaction with Ni and support, and the improved CO2 adsorption characteristic. The 10Ni-1K/MgAl2O4 catalyst exhibited optimum activity and coke resistance with only 1wt% of K.  相似文献   

6.
Nano-sized bismuth sulfide (Bi2S3) and titanium dioxide (TiO2) with the orthorhombic and anatase tetragonal structures, respectively, were synthesized for application as catalysts for the reduction of carbon dioxide (CO2) to methane (CH4). Four double-layered dense films were fabricated with different coating sequences—TiO2 (bottom layer)/Bi2S3 (top layer), Bi2S3/TiO2, TiO2/Bi2S3: TiO2 (1 : 1) mix, and Bi2S3: TiO2 (1 : 1) mix/Bi2S3: TiO2 (1 : 1) mix—and applied to the photoreduction of CO2 to CH4; the catalytic activity of the fabricated films was compared to that of the pure TiO2/TiO2 and Bi2S3/Bi2S3 doubled-layered films. The TiO2/Bi2S3 double-layered film exhibited superior photocatalytic behavior, and higher CH4 production was obtained with the TiO2/Bi2S3 double-layered film than with the other films. A model of the mechanism underlying the enhanced photoactivity of the TiO2/Bi2S3 double-layered film was proposed, and it was attributed in effective charge separation.  相似文献   

7.
A co-precipitation method was employed to prepare Ni/Al2O3-ZrO2, Co/Al2 O3-ZrO2 and Ni-Co/Al2O3-ZrO2 catalysts. Their properties were characterized by N2 adsorption (BET), thermogravimetric analysis (TGA), temperature-programmed reduction (TPR), temperature-programmed desorption (CO2-TPD), and temperature-programmed surface reaction (CH4-TPSR and CO2-TPSR). Ni-Co/Al2O3-ZrO2 bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO2 adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO2 adsorption sites (C + CO2 = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH4-CO2-TPSR, there were 80.9% and 81.5% higher CH4 and CO2 conversion over Ni-Co/Al2O3-ZrO2 catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al2O3-ZrO2 catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.  相似文献   

8.
Ni/SiC and Ni/SiO2 catalysts prepared by both wet impregnation (WI) and deposition–precipitation (DP) methods were compared for CO and CO2 methanation. The prepared catalysts were characterized using N2 physisorption, temperature-programmed reduction with H2 (H2-TPR), H2 chemisorption, pulsed CO2 chemisorption, temperature-programmed desorption of CO2 (CO2-TPD), transmission electron microscopy, and X-ray diffraction. H2-TPR analysis revealed that the catalysts prepared by DP exhibit stronger interaction between the nickel oxides and support than those prepared by WI. The former catalysts exhibit higher Ni dispersions than the latter. The catalytic activities for both reactions over Ni/SiC and Ni/SiO2 catalysts prepared by WI increase on increasing the Ni content from 10 to 20 wt%. The Ni/SiC catalyst prepared by DP shows higher catalytic activity for CO and CO2 methanation than that of the Ni/SiC catalyst prepared by WI. Furthermore, it exhibits the highest catalytic activity for CO methanation among the tested catalysts. The high Ni dispersion achieved by the DP method and the high thermal conductivity enabled by SiC are beneficial for both CO and CO2 methanation.  相似文献   

9.
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   

10.
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   

11.
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   

12.
The concept of “waste-to-wealth” is spreading awareness to prevent global warming and recycle the restrictive resources. To contribute towards sustainable development, hydrogen energy is obtained from syngas (CO and H2) generated from waste gasification, followed by CO oxidation and CO2 removal. In H2 generation, it is key to produce more purified H2 from syngas using heterogeneous catalysts. In this respect, we prepared Pt/Al2O3 catalyst with nanoporous structure using precipitation method, and compared its catalytic activity with commercial alumina (Degussa). Based on the results of XRD and TEM, it was found that metal particles did not aggregate on the alumina surface and showed high dispersion. Optimum condition for CO conversion was 1.5 wt% Pt loaded on Al2O3 support, and pure hydrogen was obtained after removal of CO2 gas.  相似文献   

13.
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   

14.
This paper describes the adsorption of lead and cadmium ions from an aqueous solution using a composite of titanium dioxide (TiO2)-incorporated polyacrylonitrile (PAN) electrospun nanofibers. Adsorption capacities and the mechanical response of the PAN/TiO2 composite electrospun nanofibers are investigated at different weight percentages of TiO2 (0.5, 1.0, 2.0, and 5.0 wt.%). The adsorption capacities of the composite PAN/TiO2 (2.0 and 5.0 wt.%) for Pb(II) and Cd(II) are remarkably increased by approximately 114 and 47%, respectively, compared to those of pure PAN electrospun nanofibers. Moreover, the adsorption of Pb(II) and Cd(II) by PAN/TiO2 nanofibers reaches an equilibrium within 60 min, and the process can be described using the nonlinear pseudo-second-order kinetic model. The adsorption isotherm study can be represented by the Langmuir model, which suggests the homogeneous distribution of monolayer adsorptive sites on the composite nanofiber surface. Furthermore, the ultimate tensile strength and ductility of all nanofiber membranes are measured through a uniaxial tension test. Mechanical tests reveal a reduction in the tensile strength of the PAN/TiO2 composite nanofibers with increase in TiO2 amount due to the possible formation of agglomerates and voids in the nanofiber structure.  相似文献   

15.
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   

16.
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   

17.
Recent improvements in the performance of photocatalysts made it possible to tackle pollution through environment friendly methods. This study investigates the modification of the photocatalytic activity of TiO2 by employing WO3 and conductive polymers, namely, polyaniline (Pani) and polypyrrole (Ppy). Basing on our previous improvement of TiO2 using a conductive polymer and activated carbon (AC), this study determines the activated carbon forms of TiO2. The prepared composites are characterized using X-ray powder diffraction, transmission electron microscopy, Fourier transform infrared, thermogravimetric analysis, Brunauer–Emmet–Teller, and UV–Vis spectroscopy. The specific surface area of the mesoporous composites is as follows: WO3/TiO2·AC (Pani) > WO3/TiO2·AC (Ppy) > WO3/TiO2·Pani > WO3/TiO2·Ppy (127 > 98 > 68 > 44 m2 g?1), which exhibited a similar trend to the photocatalytic performances (100 > 95 > 91 > 72 % conversion rate). This result could be attributed to higher porosity, surge of charge separation, and photo-responding range extension induced by the synergistic effect of WO3, conducting polymers, and TiO2 in the samples.  相似文献   

18.
Methane activation through oxychlorination is in the spotlight due to the relatively mild reaction conditions at atmospheric pressure and in the temperature range of 450–550 °C. Although CO2 is known to exhibit good activity for methane oxychlorination, significant amounts of by-products such as CO2, CO and carbon deposits are produced during the reaction over CO2. We investigated the effect of iron in FeOx/CO2 catalysts on methane oxychlorination. FeOx/CO2 with 3 wt% iron shows the maximum yield at 510 °C with 23% conversion of methane and 65% selectivity of chloromethane. XRD and H2 TPR results indicate that iron-cerium solid solution was formed, resulting in the production of more easily reduced cerium oxide and the suppression of catalysts sintering during the reaction. Furthermore, the selectivity of by-products decreased more significantly over FeOx/CO2 than cerium oxide, which can be attributed to the facilitation of HCl oxidation arising from the enhanced reducibility of the former sample.  相似文献   

19.
Activated carbon (AC) electrodes were loaded with TiO2 by using sol–gel method after a pretreatment process, the effect of the acidic pretreatment of the TiO2 loaded electrode on its deionization efficiency of the wastewater containing NaCl solutions was studied; the physical, chemical and electrochemical properties of the electrode were characterized. The physical and chemical properties of the activated carbon before and after loaded with TiO2 nanoparticles are characterized by using scanning electron microscopy, energy dispersion spectrum analyzer, Brunauer–Emmett–Teller gas adsorption method, thermal gravimetric analysis, Fourier transform infrared spectroscopy respectively. Electrochemical properties were characterized by employing electrochemical workstation and electrical adsorption deionization test. It was found that both the specific capacitance and the ions removal efficiency of the activated carbon loaded with TiO2 had an increase of 16.4 and 49.8 % respectively in comparison with original activated carbon electrode. It was believed that this is due to the presence of crystal anatase TiO2 nanoparticles (the mass content of titanium element in the TiO2/AC complex is about 24.91 %) on the surface and pores in the activated carbon; while Ti–O–C bonds was found on the surface of the activated carbon, its surface wetting properties was significantly improved. However, it was also noticed that and the specific surface area of the activated carbon was decreased from 680.5 to 523.35 m2 g?1. This might lead to the decrease of the physical adsorption properties of the activated carbon electrodes, but its Electrical double-layer capacitance increases, electrical adsorption efficiency was improved.  相似文献   

20.
Adsorption of pure carbon dioxide and methane was examined on activated carbon prepared from pine cone by chemical activation with H3PO4 to determine the potential for the separation of CO2 from CH4. The prepared adsorbent was characterized by N2 adsorption-desorption, elemental analysis, FTIR, SEM and TEM. The equilibrium adsorption of CO2 and CH4 on AC was determined at 298, 308 and 318 K and pressure range of 1–16 bar. The experimental data of both gases were analyzed using Langmuir and Freundlich models. For CO2, the Langmuir isotherm presented a perfect fit, whereas the isotherm of CH4 was well described by Freundlich model. The selectivity of CO2 over CH4 by AC (CO2: CH4=50: 50, 298K, 5 bar), predicted by ideal adsorbed solution theory (IAST) model, was achieved at 1.68. These data demonstrated that pine cone-based AC prepared in this study can be successfully used in separation of CO2 from CH4.  相似文献   

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