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1.
《分离科学与技术》2012,47(10):1448-1455
The article describes transport of Pb(II) through bulk liquid membrane (BLM) containing calix[6]arene hexaester derivative (1) as a carrier. The effect of various parameters such as temperature, carrier concentration, stirring speed and type of solvent on the Pb(II) transport efficiency of the carrier through BLM was evaluated. The activation energy values for the extraction and re-extraction were found as 56.33 kJ mol?1 and 14.79 kJ mol?1, respectively. These values demonstrate that the process is diffusionally controlled by Pb(II). Observations indicate that the membrane entrance and exit rate constants (k1, k2) increase with increasing stirring speed as well as carrier concentration and decrease with increasing temperature. The effect of solvent on k1 and k2 was found to be in the order of CH2Cl2 > CHCl3 > CCl4.  相似文献   

2.
Mixed matrix membranes (MMMs) are gaining increasing interest in academic and industrial research due to their combined, desirable properties of both polymers and organic/inorganic filler as important materials. In this work, synthesized zeolitic imidazolate framework (ZIF-8) suspension (10–50 wt%) was directly incorporated into a [poly (amide-b-ethylene oxide) Pebax® 1657] matrix in order to improve the gas separation performance of the membrane. Dynamic light scattering (DLS) analysis showed an average diameter of 77.4 nm for the prepared nanoparticles. The transparent membranes were characterized by scanning electron microscopy (SEM), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), Fourier transform infrared (FTIR) spectroscopy, and X-ray diffractometry (XRD). These indicated excellent dispersion of nanoparticles, which was achieved by ultrasonication before casting the solution. Incorporation of ZIF-8 as filler in the polymer matrix led to improved thermal and mechanical stability of the membranes. This was confirmed by TGA and tensile analyses, indicating good contacts provided at the polymer/filler interfaces. The effect of ZIF-8 loading (up to 50 wt%) on membrane performance was investigated and it showed an optimum loading of 30 %. Single gas (CO2, N2 and CH4) permeation tests revealed rapid, enhanced permeability of the nanocomposite membranes without significant changes in selectivity (compared to those of the pristine polymeric membrane). The permeability increases for CO2, CH4 and N2 in the optimum Pebax® 1657/ZIF-8 (30 wt%) membrane were found in the stated order as 111, 88 and 99 %. The study revealed that Pebax® 1657/ZIF-8 membranes displayed better gas permeation properties compared to those of Pebax® 1657.  相似文献   

3.
《分离科学与技术》2012,47(16):2320-2330
In this research, continuous SAPO-34 membranes were synthesized via secondary growth method onto both α-Al2O3 and mullite supports at three levels of synthesis temperature: 185, 195, and 220°C for 24 h. The synthesized membranes were characterized using XRD and SEM analysis and single gas permeation experiments. It was found out that support material and synthesis temperature both have significant effects on the membrane performance. At higher synthesis temperature, SAPO-34 crystals grown over the mullite support become more uniform and smaller in size but those grown on the α-Al2O3 support become larger. Effect of synthesis temperature on single gas permeation properties of the synthesized SAPO-34 membranes was also studied. For the mullite supported membranes, the CH4 and CO2 permeances decrease as synthesis temperature increases; but in the case of the alumina supported membranes, by increasing synthesis temperature, CH4 and CO2 permeances first decrease up to 195°C and then increase up to 220°C. Even in equal membrane thicknesses, the mullite supported membrane shows lower gas permenaces. Increasing synthesis temperature decreases CO2/CH4 ideal selectivity for the α-Al2O3 supported membranes, while increases for the mullite supported membranes. Under optimum synthesis conditions, at room temperature and 2 bar feed pressure, the CO2 permeance through the α-Al2O3 and the mullite supported SAPO-34 membranes are 8.2 × 10?7 and 8.5 × 10?8 (mol/m2 · s · Pa), respectively, and CO2/CH4 ideal selectivities are 51 and 61, respectively.  相似文献   

4.
The present field study investigated the effects of the system of rice intensification (SRI) on greenhouse gas emissions and rice yield, in the first field trial of its kind in Cambodia. The study was a 2 × 4 factorial design, including SRI and conventional management practices (CMP) with the following treatments: control, composted farmyard manure (FYM), mineral fertiliser (MF) and FYM + MF. The results indicated large seasonal variations of CH4 patterns during the growing season with a peak emission of about 1,300 mg CH4 m?2 day?1 under both production systems 2 weeks after rice transplanting. There was large temporal variability of CH4 fluxes from morning to midday. Emission of N2O was below the detection limit in both systems. Under each production system, the highest seasonal emission of CH4 was under the FYM + MF treatment, namely 282 kg ha?1 under CMP and 213 kg ha?1 under SRI. Total CH4 emission under SRI practices was reduced by 22 % in the FYM treatment, 17 % in the MF treatment and 24 % in the FYM + MF treatment compared to CMP. There was no effect of water management on CH4 emission in the non-fertilized treatment. Grain yields were not significantly affected by the production system. Thus the yield-scaled global warming potential (GWP) was lower under SRI than CMP, namely 21 % in FYM and FYM + MF treatments, and 8 % in MF treatment. The application of mineral fertilisers moderately increased CH4 emission but significantly increased rice yields, resulting in a significantly lower yield-scaled-GWP compared to farmyard manure.  相似文献   

5.
The present paper renders a modeling and a 2D numerical simulation for the removal of CO2 from CO2/CH4 gaseous stream utilizing sodium hydroxide (NaOH), monoethanolamine (MEA) and triethanolamine (TEA) liquid absorbents inside the hollow fiber membrane contactor. Counter-current arrangement of absorbing agents and CO2/CH4 gaseous mixture flows are implemented in the modeling and numerical simulation. Non-wetting and partial wetting modes of operation are considered where in the partial wetting mode, CO2/CH4 gaseous mixture and liquid absorbents fill the membrane pores. The deteriorated removal of CO2 in the partial wetting mode of operation is mainly due to the mass transfer resistance imposed by the liquid in the pores of membrane. The validation of numerical simulation is done based on the comparison of simulation results of CO2 removal using NaOH and experimental data under non-wetting mode of operation. The comparison illustrates a desirable agreement with an average deviation of less than 5%. According to the results, MEA provides higher efficiency for CO2 removal in comparison with the other liquid absorbents. The order for CO2 removal performance is MEA > NaOH > TEA. The influence of non-wetting and partial wetting modes of operation on CO2 removal are evaluated in this article as one of the novelties. Besides, the percentage of CO2 sequestration as a function of gas velocity for various percentages of membrane pores wetting ranging from 0 (non-wetting mode of operation) to 100% (complete wetting mode of operation) is studied in this research paper, which can be proposed as the other novelty. The results indicate that increase in some operational parameters such as module length, membrane porosity and absorbents concentration encourage the removal percentage of CO2 from CO2/CH4 gaseous mixture while increasing in membrane tortuosity, gas velocity and initial CO2 concentration has unfavorable influence on the separation efficiency of CO2.  相似文献   

6.
《分离科学与技术》2012,47(1):58-65
Tetraaza-14-crown-4 and oleic acid was successfully applied for transport of Cu(II) in chloroform bulk liquid membrane. The uphill moving of Cu(II) during the liquid membrane transport process has occurred. The main effective variable such as the type of the metal ion acceptor in the receiving phase and its concentration, tetraaza-14-crown-4 and oleic acid concentration in the organic phase on the efficiency of the ion-transport system were examined. By using L-cysteine as a metal ion acceptor in the receiving phase, the maximum amount of copper (II) transported across the liquid membrane was achieved to 96 ± 1.5% after 140 minutes. The selectivity of copper ion transport from the aqueous solutions containing Pb2+, Tl+, Ag+, Co2+, Ni2+, Mg2+, Zn2+, Hg2+, Cd2+ and Ca2+ ions were investigated. In the presence of CH3COONH4 and Na4P2O7 as suitable masking agents in the source phase, the interfering effects of Pb+2 and Cd2+ were diminished drastically.  相似文献   

7.
In this work, the response surface methodology (RSM) based on the central composite design (CCD) was used to examine effects of different gamma alumina (γ-Al2O3) loadings (0 to 8 wt.%) and various polyethylene glycol 1000 (PEG1000) contents (0 to 40 wt.%) as parameters on membrane preparation. Accordingly, pure carbon dioxide (CO2) and methane (CH4) gasses permeability and ideal CO2/CH4 selectivity values were considered as responses. Poly (ether block amide) 1657 (Pebax1657) was used as the base polymer matrix for the membranes fabrication. The neat Pebax1657 membrane was prepared via solution casting-solvent evaporation method and the other membranes were prepared via solution blending technique. Analysis of variance (ANOVA) was used to analyze the experiments statistically and the results indicated that the optimized amounts of γ-Al2O3 nanoparticles and PEG1000 in order to enhance both CO2 permeability and ideal CO2/CH4 selectivity were 8 wt.% and 10 wt.%, respectively. Additionally, a comparison between the separation performance of the neat membrane, the nanocomposite membrane with the optimum amount of γ-Al2O3 nanoparticles, the blended membrane with optimum amounts of PEG1000, and the blended nanocomposite membrane with optimum amounts of γ-Al2O3 nanoparticles and PEG1000 was presented. The obtained gas permeation results showed that the blended nanocomposite membrane exhibits the highest CO2/CH4 separation performance compared to the neat Pebax membrane.  相似文献   

8.
Soil salinization adversely affects sustainable land use and limitation of greenhouse gas emission. Methane (CH4) uptake and the specific activity of methanotrophs in three saline–alkaline soils—S1, electrical conductivity (EC) 4.80?dS?m?1; S2, EC 2.60?dS?m?1; and S3, EC 0.74?dS?m?1—were observed and measured across crop phenological development in the Hetao Irrigation District of Inner Mongolia, China. There were significant differences in CH4 uptake between the three soil types. The cumulative uptake of CH4 was 97.97 mg m?2, 109.49 mg m?2, and 150.0 mg m?2 in S1, S2, and S3, respectively. Cumulative CH4 uptake was 35%, 35%, and 53% lower in S1 than in S3, and was 27%, 28%, and 19% lower in S2 than in S3 in 2014, 2015, and 2016, respectively. Differences in CH4 uptake were driven by the different specific activities of the methanotrophs in the three soils, of which the key controlling factor was soil EC. The findings demonstrate that saline–alkaline soils with high EC led to low CH4 uptake and thereby significantly increased the total greenhouse effect of CH4.  相似文献   

9.
A new family of lauryl trimethyl ammonium surfactants of the general formula CH3(CH2)11 N+(CH3)3X? (X = CH3OCOO, HCOO, CH3COO, CH3CHOHCOO) were prepared and characterized both structurally and as aqueous surfactants. Lauryl trimethyl ammonium mono-methyl carbonate was synthesized by using dimethyl carbonate (DMC) as the alkylating agent and lauryl dimethyl amine as the starting material. The latter compound was reacted with formic acid, acetic acid, and lactic acid, respectively, to give the corresponding quaternary ammonium salts with other counteranions. They were structurally characterized by IR, 1H NMR, MS. Members of this family reduced the surface tension of water to 32–38 mN/m at concentration levels of 10?2 mol/L.  相似文献   

10.
Samarium-doped ceria (SDC) is coated onto a Ni/yttria-stabilized zirconia (Ni/YSZ) anode for the direct use of methane in solid-oxide fuel cells. Porous SDC thin layer is applied to the anode using the sol–gel coating method. The experiment was performed in H2 and CH4 conditions at 800 °C. The cell performance was improved by approximately 20 % in H2 conditions by the SDC coating, due to the high ionic conductivity, the mixed ionic and electronic conductive property of the SDC, and the increased triple phase boundary area by the SDC coating in the anode. Carbon was hardly deposited in the SDC-coated Ni/YSZ anode. The cell performance of the SDC-coated Ni/YSZ anode did not show any significant degradation for up to 90 h under 0.1 A cm?2 at 800 °C. The porous thin SDC coating on the Ni/YSZ anode provided the electrochemical oxidation of CH4 over the whole anode, and minimized the carbon deposition by electrochemical carbon oxidation.  相似文献   

11.
We report on the gas storage behaviour and electrochemical charge storage properties of high surface area activated nanoporous carbon obtained from rice husk through low temperature chemical activation approach. Rice husk derived porous carbon (RHDPC) exhibits varying porous characteristics upon activation at different temperatures and we observed high gas uptake and efficient energy storage properties for nanoporous carbon materials activated even at a moderate activation temperature of 500 °C. Various experimental techniques including Fourier transform-infrared spectroscopy, Raman spectroscopy, scanning electron microscopy, high resolution transmission electron microscopy and pore size analyser are employed to characterise the samples. Detailed studies on gas adsorption behaviour of CO2, H2 and CH4 on RHDPCs have been performed at different temperatures using a volumetric gas analyser. High adsorption capacities of ~9.4 mmol g?1 (298 K, 20 bar), 1.8 wt% (77 K, 10 bar) and ~5 mmol g?1 (298 K, 40 bar) were obtained respectively for CO2, H2 and CH4, superior to many other carbon based physical adsorbents reported so far. In addition, these nanoporous carbon materials exhibit good electrochemical performance as supercapacitor electrodes and a maximum specific capacitance of 112 F g?1 has been obtained using aqueous 1 M Na2SO4 as electrolyte. Our studies thus demonstrate that nanoporous carbon with high porosity and surface area, obtained through an efficient approach, can act as effective materials for gas storage and electrochemical energy storage applications.  相似文献   

12.
Carbon molecular sieve membranes (CMSM) were prepared from the pyrolysis of polyimide films within a temperature range of 600°C-800°C under nitrogen stream. The membrane samples were characterized and tested for the permeation of He, CH4, CO2, and N2 at different pressures and temperatures, respectively. The CMSM700 membrane (pyrolyzed at 700°C) showed an ideal selectivity of ~ 11 for N2/CH4 with a permeability of 2.18 × 10−15 mol · m/m2 · s · Pa for N2. The separation mechanism for the N2/CH4 pair was shown to be largely molecular sieving rather than surface flow. The membrane showed an ideal selectivity of ~ 500 for the CO2/CH4 pair with a CO2 permeability of 9.72 × 10−14 mol · m/m2 · s · Pa. The permeability of He was lower than that of CO2, suggesting that the surface flow played a significant role in the CO2 permeation. The updated permeability-selectivity tradeoff curves show that this CMSM membrane compared favourably with other membrane materials reported in the literature for the removal of N2 and CO2 from CH4 for natural gas upgrading.  相似文献   

13.
In membrane technology, wettability is one of the most crucial points for successful industrial application of membrane contactors. To solve this issue, a non-wetting polypropylene (PP) hollow fiber membrane was prepared by the incorporation of modified silica nanoparticles (CH3SiO2) synthesized through sol–gel process on the surface and the cross-section of the membrane. Tetraethylorthosilicate (TEOS) and methyltriethoxysilane (MTES) were used as precursor and hydrophobic agent, respectively, to synthesize CH3SiO2 nanoparticles (NPs). In preparation procedure of NPs, the influential parameters including MTES/TEOS and H2O/TEOS molar ratios and NH4OH concentration were optimized using central composite design of response surface method (RSM) by considering contact angle (CA) as response variable. The CA of 168° was obtained using analysis of variance (ANOVA) when the MTES/TEOS molar ratio, H2O/TEOS molar ratio and NH4OH concentration were, respectively, 3.774, 8.000 and 0.511 M. ATR-FTIR, FE-SEM, mechanical strength and porosity measurements were used to characterize the optimum membrane. The neat and modified membranes were also tested for the CO2 absorption process in a gas–liquid membrane contactor system. The CO2 absorption flux of modified membrane almost remained constant within 30 days, while the neat membrane slightly suffered from wetting problem, resulted in a continuous decline in the CO2 flux.  相似文献   

14.
Manure storage contributes significantly to greenhouse gas (GHG), NH3 and odour emissions from intensive livestock production. A pilot-scale facility with eight 6.5-m3 slurry storage units was used to quantify emissions of CH4, N2O, NH3, and odorants from pig slurry during winter and summer storage. Pig slurry was stored with or without a straw crust, and with or without interception of precipitation, i.e., four treatments, in two randomized blocks. Emissions of total reduced S (mainly H2S) and p-cresol, but not skatole, were reduced by the straw crust. Total GHG emissions were 0.01–0.02 kg CO2 eq m?3 day?1 during a 45-day winter storage, and 1.1–1.3 kg CO2 eq m?3 day?1 during a 58-day summer storage period independent of storage conditions; the GHG balance was dominated by CH4 emissions. Nitrous oxide emissions occurred only during summer storage where, apparently, emissions were related to the water balance of the surface crust. An N2O emission factor for slurry storage with a straw crust was estimated at 0.002–0.004. There was no evidence for a reduction of CH4 emissions with a crust. Current Intergovernmental Panel on Climate Change recommendations for N2O and CH4 emission factors are discussed.  相似文献   

15.
In this study, 3-(2-Aminoethyl thiophene) (2AET) monomer was electropolymerized on glassy carbon electrode (GCE) using various electrolytes (lithium perchlorate (LiClO4), sodium perchlorate (NaClO4), tetrabutyl ammonium tetra fluoroborate (TBABF4) and tetraethyl ammonium tetra fluoroborate (TEABF4) in acetonitrile (CH3CN) as solvent. Poly(3-(2-aminoethyl thiophene) (P(2AET))/GCE was characterized by cyclic voltammetry (CV), Fourier transform infrared reflectance spectrophotometry (FTIR-ATR), scanning electron microscopy, energy dispersive X-ray analysis (EDX), and electrochemical impedance spectroscopy (EIS) techniques. The electrochemical impedance spectroscopic results were given by Nyquist, Bode-magnitude, Bode-phase, capacitance and admittance plots. The highest low frequency capacitance (C LF) value obtained was 0.65 mF cm?2 in 0.1 M LiClO4/CH3CN for the initial monomer concentration of 1.5 mM. The highest double layer capacitance (C dl = ~0.63 mF cm?2) was obtained in 0.1 M LiClO4/ACN for [2AET]0 = 0.5, 1.0 and 1.5 mM. The maximum phase angles (θ = 76.1o at 26.57 Hz) and conductivity (Y″ = 3.5 mS) were obtained in TEABF4/ACN for [2AET]0 = 0.5 and 1.0 mM, respectively. An equivalent circuit model of R(Q(R(Q(R(CR))))) was simulated for different electrolytes (LiClO4, NaClO4, TBABF4 and TEABF4)/P(2AET)/GCE system. A good fitting was obtained for the calculated experimental and theoretical EIS measurement results. The electroactivity of P(2AET)/GCE opens the possibility of using modified coated electrodes for electrochemical micro-capacitor electrodes and biosensor applications.  相似文献   

16.
A novel organic molecule of 9H-carbazole-9-carbothioic methacrylic thioanhydride (CzCS2metac) was synthesized by incorporating CS2 and methacrylate groups into the carbazole monomer structure. CzCS2metac was characterized by FTIR, 1H-NMR and 13C-NMR spectroscopy. CzCS2metac was electropolymerized in 0.1 M tetraethylammonium tetrafluoroborate (TEABF4)/acetonitrile (CH3CN) on glassy carbon electrode (GCE). The characterization of the electrocoated P(CzCS2metac)/CFME thin film was studied by various techniques, such as cyclic voltammetry, scanning electron microscopy–energy-dispersive X-ray analysis and electrochemical impedance spectroscopy. The specific capacitance (C sp) of P(CzCS2metac)/MWCNT/GCE in the scan rate of 20 mV s?1 (C sp = 38.48 F g?1 from area formula, C sp = 38.52 F g?1 from charge formula) was increased ~15.66 and ~15.64 times in area and charge formulas compared to P(CzCS2metac)/GCE (C sp = 2.46 F g?1 from area and charge formulas). The same results were also obtained from Nyquist graphs. The specific capacitance value of composite film (C sp = 1.09 × 10?3 F) is ~15.66 times higher than the polymer film (C sp = 6.92 × 10?5 F). The composite film may be used as supercapacitor electrode material in energy storage devices.  相似文献   

17.
Simultaneous production of hydrogen as an energy carrier and chlorine as a valuable chemical from recycled hydrogen chloride was investigated employing a lab-scale membrane electrolysis setup. The effects of various process parameters including current density (1–4 kA m?2), cell temperature (45°–75°C), flow rate of hydrochloric acid feed (200–500 mL min?1), and concentration of acid (18–21 wt.%) on the cell voltage and chlorine current efficiency (ChCE) were studied. The Taguchi design of experiments (L16 array) was employed to design the minimum number of experiments necessary to fully study the process. A filter press type cell of 10 cm2 surface area comprising a DSA anode, an alloy of predominantly nickel cathode and Nafion 115 membrane, was used. It was observed that increasing anolyte flow rate, anolyte concentration, or cell temperature caused a decrease in cell voltage and an increase in ChCE, while increasing current density linearly increased cell voltage and decreased ChCE.  相似文献   

18.
19.
The novel fixed‐site‐carrier (FSC) membranes were prepared by coating carbon nanotubes reinforced polyvinylamine/polyvinyl alcohol selective layer on top of ultrafiltration polysulfone support. Small pilot‐scale modules with membrane area of 110–330 cm2 were tested with high pressure permeation rig. The prepared hybrid FSC membranes show high CO2 permeance of 0.084–0.218 m3 (STP)/(m2 h bar) with CO2/CH4 selectivity of 17.9–34.7 at different feed pressures up to 40 bar for a 10% CO2 feed gas. Operating parameters of feed pressure, flow rate, and CO2 concentration were found to significantly influence membrane performance. HYSYS simulation integrated with ChemBrane and cost estimation was conducted to evaluate techno‐economic feasibility of a membrane process for natural gas (NG) sweetening. Simulation results indicated that the developed FSC membranes could be a promising candidate for CO2 removal from low CO2 concentration (10%) NGs with a low NG sweetening cost of 5.73E?3 $/Nm3 sweet NG produced. © 2014 American Institute of Chemical Engineers AIChE J 60: 4174–4184, 2014  相似文献   

20.
《分离科学与技术》2012,47(12):1698-1708
Hybrid organic-inorganic H2-selective membranes consisting of single-layer or dual-layers of silica incorporating aromatic groups are deposited on a porous alumina support by chemical vapor deposition (CVD) in an inert atmosphere at high temperature. The single-layer silica membranes, which are made by the simultaneous decomposition of phenyltriethoxysilane (PTES) and tetraethylorthosilicate (TEOS), have good hydrothermal stability at high temperature and a high permeance for hydrogen in the order of 10?7 mol m?2 s?1 Pa?1 at 873 K, while preventing the passage of other larger molecular gases such as CH4 and CO2. The dual-layer silica membranes, which are obtained from the sequential decomposition of PTES and TEOS, exhibit an extremely high permeance for hydrogen of 3.6 × 10?6 mol m?2 s?1 Pa?1 at 873 K with a permselectivity of hydrogen over methane of 30. A normalized Knudsen based permeance method is applied to measure the pore size of PTES-derived silica membrane on the dual-layer silica membrane before treatment with TEOS. The method indicates that the pore size of the silica network is approximately in the range of 0.50–0.85 nm, which is higher than the characteristic length of pure silica membranes of 0.3 nm, accounting for the high permeance of the hybrid membranes.  相似文献   

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