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1.
Photocatalytic degradation of the reactive triazine dyes Reactive Yellow 84 (RY 84), Reactive Red 120 (RR 120), and Reactive Blue 160 (RB 160) on anatase phase N-doped TiO2 in the presence of natural sunlight has been carried out in this work. The effect of experimental parameters like initial pH and concentration of dye solution and dosage of the catalyst on photocatalytic degradation have also been investigated. Adsorption of dyes on N-doped TiO2 was studied prior to photocatalytic studies. The studies show that the adsorption of dyes on N-doped TiO2 was high at pH 3 and follows the Langmuir adsorption isotherm. The Langmuir monolayer adsorption capacity of dyes on N-doped TiO2 was 39.5, 86.0, and 96.3 mg g?1 for RY 84, RR 120, and RB 160, respectively. The photocatalytic degradation of the dyes follows pseudo first-order kinetics and the rate constant values are higher for N-doped TiO2 when compared with that of undoped TiO2. Moreover, the degradation of RY 84 on N-doped TiO2 in sunlight was faster than the commercial Aeroxide® P25. However, the P25 has shown higher photocatalytic activity for the other two dyes, RR 120 and RB 160. The COD of 50 mg l?1 Reactive Yellow-84, RR 120 and RB 160 was reduced by 65.1, 73.1, and 69.6 %, respectively, upon irradiation of sunlight for 3 h in the presence of N-doped TiO2. The photocatalyst shows low activity for the degradation of RY 84 dye, when its concentration was above 50 mg l?1, due to the strong absorption of photons in the wavelength range 200–400 nm by the dye solution. LC–MS analysis shows the presence of some triazine compounds and formimidamide derivatives in the dye solutions after 3 h solar light irradiation in the presence of N-doped TiO2.  相似文献   

2.
To understand the separation behavior of Zr(IV) in the partitioning process for high level liquid waste, a silica-based macroporous adsorbent (TODGA/SiO2-P) was prepared by impregnating N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide (TODGA) into a macroporous silica/polymer composite particles support (SiO2-P). Adsorption and desorption behavior of Zr(IV) from nitric acid solution onto silica-based TODGA/SiO2-P adsorbent were investigated by batch experiment. It was found that TODGA/SiO2-P showed strong adsorption affinity to Zr(IV) and this adsorption process reached equilibrium state around 6 h at 298 K. Meanwhile, HNO3 concentration had no significant effect on the adsorption of Zr(IV) above 1 M. From calculated thermodynamic parameters, this adsorption process could occur spontaneously at the given temperature and was confirmed to be an exothermic reaction. This adsorption process could be expressed by Langmuir monomolecular layer adsorption mode and the maximum adsorption capacity were determined to be 0.283 and 0.512 mmol/g for Zr(IV) at 298 and 323 K, respectively. In addition, more than 90 % of Zr(IV) adsorbed onto adsorbent could be desorbed with 0.01 M diethylenetriamine pentaacetic acid solution within 24 h at 298 K.  相似文献   

3.
Pristine multiwalled carbon nanotubes (MWCNTs) were impregnated in acrylonitrile butadiene rubber (NBR) using internal dispersion kneader and two roller mixing mill to investigate the effects of various nanotubes concentrations on the thermal transport/stability of rubber nanocomposites. Thermal conductivity (λ N) and thermal impedance (R) measurement experimental setups were established according to ASTM E1225-99 and D5470-03. The 1 mass % addition of MWCNTs in the polymer matrix has enhanced R up to 44 % and reduced λ N of the rubber nanocomposite up to 40 % compare to the base composite formulation. Thermal decomposition and differential thermal analyses of the fabricated composite specimens simulate that the thermal stability and endothermic capability are augmented with increasing the nanotubes contents in the host matrix. The progressive incorporations of carbon nanotubes into the rubber matrix have efficiently influenced the composite specimens regarding glass transition, crystallization, and melting temperatures including their specific enthalpies. Scanning electron microscopy along with the energy dispersive spectroscopy was used to analyze MWCNTs dispersion in NBR matrix, compositional analysis of the nanocomposite, and impregnated nanotubes.  相似文献   

4.
Applying activated carbons for SO2 adsorption and conversion to H2SO4, as a dry process, has been considered the development direction of desulfurization technology. Coal-based activated carbon, coconut shell activated carbon, single wall carbon nanotube and multi-wall carbon nanotubes were used as typical carbonaceous materials to study the SO2 adsorption mechanism. SEM, N2 adsorption, XPS and fixed-bed reaction system were employed to study the morphology, pore structure, surface functional groups and SO2 adsorption behaviors of the four adsorbents. The fixed-bed experiment was carried out at normal pressure and SO2 concentration was set 1,000 ppm. According to SEM and N2 adsorption results, hierarchical pore structure was an important characteristic of activated carbon. Aggregation was an important characteristic of CNTs. Mesopores and macropores took the dominance of pore structure in CNTs. According the SO2 adsorption data and correlation analysis, it can be concluded that the dominant adsorption type on activated carbons does not alter with adsorption temperature changing. However, the adsorption type of SO2 adsorption on CNTs changes with adsorption temperature varying. With adsorption temperature increasing, the dominant adsorption type transforms to chemisorption by physisorption. Higher-density π–π* in carbon nanotubes may be the active sites for the SO2 chemical adsorption. Micropores with the diameter smaller than 0.7 nm were the best SO2 adsorption place for both activated carbons and carbon nanotubes. The results provided a profound insight into the microstructure and SO2 adsorption mechanism of the two kinds of carbonaceous materials.  相似文献   

5.
Titanate nanotubes (TNTs) have been synthesized by a hydrothermal method using rutile TiO2 powder as titanium source. The determination of the structure and morphology was characterized by XRD, FTIR, SEM and TEM. The results indicate that the TNTs successfully synthesized under hydrothermal conditions of 150 °C. The adsorption of Th(IV) on TNTs was studied as a function of contact time, pH values, ionic strength, initial Th(IV) concentration and temperature under ambient conditions by using batch technique. The results indicate that adsorption of Th(IV) on TNTs is strongly dependent on pH values, but weakly dependent on ionic strength; Adsorption kinetics was better described by the pseudo-second-order model. The adsorption isotherms are simulated by Langmuir and Freundlich models well. ΔG°, ΔH° and ΔS° free energy were calculated from experimental data, The results indicate that the adsorption of Th(IV) on TNTs is an endothermic and a spontaneous process, and increases with increasing temperature. The adsorption of Th(IV) on TNTs is mainly dominated by chemical sorption or surface complexation.  相似文献   

6.
Nitrous oxide (N2O) adsorption on the pristine and Stone–Wales (SW)-defected hexagonal BN nanosheets were investigated using density functional calculations including dispersion correction. It was found that N2O is weakly adsorbed on the pristine sheet (h-BN) through van der Waals interaction with adsorption energy of ?1.2 kcal/mol. SW-defected sheet was found to be more reactive toward N2O molecule having no significant change in electronic properties. However, the formation of B–B and N–N bond pairs in SW-defected sheet can be avoided, if there is a C–C pair doped in sheet (C2-SW-h-BN). In this case, a strong adsorption is found due to large adsorption energy (?23.7 kcal/mol) and short bond length compared to the SW-h-BN complex. Interestingly, it was indicated that the N2O molecule could be reduced into the N2 on the C2-SW-h-BN.  相似文献   

7.
Porous copolymers of divinylbenzene (DVB) and acrylic acid (AA) having DVB:AA ratios of 6:4, 8:2 and 9:1 were prepared following a distillation-precipitation method, using toluene as the porogenic agent. The materials thus obtained, which showed specific surface area in the range of 380–600 m2 g?1 and pore volume in the range of 0.14–0.18 cm3 g?1, were investigated as possible adsorbents for CO2 capture from the flue gas of coal-fired power stations. For that purpose, the isosteric heat of adsorption (and CO2 adsorption capacity) was analysed from N2 and CO2 adsorption equilibrium isotherms obtained over a temperature range. For CO2, q st resulted to be in the range of 27–31 kJ mol?1 (the highest value corresponding to the 6:4 sample), while for N2 a value of q st ≈ 12 kJ mol?1 was obtained. Equilibrium adsorption capacity for CO2 (at ambient temperature and pressure) showed the value of about 1.35 mmol g?1. These results are discussed in the broader context of corresponding literature data for CO2 capture using protonic zeolites.  相似文献   

8.
Industrial grade multi-walled carbon nanotubes (IG-MWCNTs) are a low-cost substitute for commercially purified multi-walled carbon nanotubes (P-MWCNTs). In this work, IG-MWCNTs were functionalized with tetraethylenepentamine (TEPA) for CO2 capture. The TEPA impregnated IG-MWCNTs were characterized with various experimental methods including N2 adsorption/desorption isotherms, elemental analysis, X-ray diffraction, Fourier transform infrared spectroscopy and thermogravimetric analysis. Both the adsorption isotherms of IG-MWCNTs-n and the isosteric heats of different adsorption capacities were obtained from experiments. TEPA impregnated IG-MWCNTs were also shown to have high CO2 adsorption capacity comparable to that of TEPA impregnated P-MWCNTs. The adsorption capacity of IG-MWCNTs based adsorbents was in the range of 2.145 to 3.088 mmol/g, depending on adsorption temperatures. Having the advantages of low-cost and high adsorption capacity, TEPA impregnated IG-MWCNTs seem to be a promising adsorbent for CO2 capture from flue gas.  相似文献   

9.
Density functionla theory (DFT) calculations are performed to characterize geometric and electronic features of the octahedral Al n N n and Al n P n cages (n = 12, 16, 28, 32, and 48). Toward this aim, 15N, 27Al, and 31P chemical shielding (CS) tensors as well as natural charge analyses are calculated for the optimized structures. CS parameters detect three distinct electronic environments for atoms within the Al n N n and Al n P n cages. The chemical shifts of N2 sites belonging to a hexagon and surrounded by three hexagons and a square obtained are different from those of N3 sites belonging to a hexagon that is surrounded only by hexagons—due to different curvatures exerted at the sites with different local structures. In addition, there is an increasing tendency in the Δσ values of the three local structures, Δσ (N1) > Δσ (N2) > Δσ (N3), N1 sites belonging to four-membered rings. The chemical shieldings of those Al and P sites belonging to a hexagon that is surrounded only by hexagons in the cages (360.7–366.7 and 496.5–514.7 ppm) are close to those previously reported for AlP nanotubes. Three distinct electrostatic environments around the N, Al, and P nuclei are also confirmed by the calculated natural charges. It should be noted that the positively charged Al atoms on the cages turn out to be the available sites for adsorption of H2 molecules.  相似文献   

10.
The electronic excitation transitions of carbazole-based oligomers, (Cz-co-Cz) N , (Cz-co-Fl) N and (Cz-co-Th) N (N = 2–4) were investigated using density functional theory (DFT) and time-dependent (TD) DFT methods. Our results show that the calculated ground state geometries favor a more aromatic, planer structure, while the electronically excited geometries favor a quinoidic type structure. Absorption and fluorescence energies have been obtained from TD-B3LYP/SVP calculations performed on the S1 optimized geometries and are in excellent agreement with experimental data. The experimental fluorescence excitation energies for (Cz-co-Cz)4, (Cz-co-Fl)4 and (Cz-co-Th)4 (2.76, 2.63, and 2.25 eV, respectively) correspond closely with the predicted S1 transitions (2.84, 3.91 and 2.43 eV, respectively). We also report the predicted radiative lifetimes 0.52, 0.47, and 0.99 ns for (Cz-co-Cz) N , (Cz-co-Fl) N and (Cz-co-Th) N , discuss the origin of the small stoke shift of the carbazole based oligomers and the magnitude of bathochromic shifts. We conclude by discussing the benefits of theoretical calculations, which can provide critical structural and electronic understanding of excitation–relaxation phenomena that can be exploited in design of novel optical materials.  相似文献   

11.
The adsorption of the potassium atom onto the surface of (n,0) zigzag nanotube (n = 5–10) and (n,n) armchair nanotubes (n = 3, 5) has been studied by density functional theory. The local density approximation calculation of adsorption energy (E ads) emphasized on the dependency of E ads to the diameter and chirality of the nanotube. E ads decreases when the diameter increases. So the (5,0)-K system has the highest adsorption energy among all structures. Furthermore, a significant change was observed in the electronic properties of potassium-adsorbed single-walled carbon nanotube (SWCNT) and the metallic behavior of the nanotube improved. Therefore, our results showed that such modified SWCNTs can be applied in nanodevices such as transistors.  相似文献   

12.
To separate platinum group metals (PGMs) from high level liquid waste (HLLW), a novel silica-based (Crea + TOA)/SiO2–P adsorbent was synthesized by impregnating Crea (N′,N′-di-n-hexyl-thiodiglycolamide) and TOA (trioctylamine) two extractants into the macroporous SiO2–P support with a mean diameter of 60 μm. Adsorption properties and behavior of PGMs from simulated HLLW onto the novel silica-based (Crea + TOA)/SiO2–P adsorbent were investigated by batch method. It was found that (Crea + TOA)/SiO2–P adsorbent exhibited good adsorption selectivity for PGMs over the other tested fission product element in a wide HNO3 concentration. This adsorbent showed strong affinity to Pd(II) but almost no adsorption for rare earth elements. Adsorption process of PGMs could be expressed by Langmuir monomolecular layer adsorption mode and be governed by the chemisorption process. In addition, the adsorption isotherms and thermodynamic parameters of tested elements were calculated by Langmuir equation, Freundlich equation and van’t Hoff equation, respectively.  相似文献   

13.
Poly(cyclotriphosphazene-co-4,4′-sulfonyldiphenol) (PZS) nanotubes were evaluated as an efficient adsorbent for the removal of Rhodamine B (RhB), a cationic dye from aqueous solution. The as-synthesized adsorbent (PZS nanotubes) were characterized by scanning electron microscopy (SEM), transmission electron microscope (TEM), Fourier transform infrared spectroscopy (FTIR) and N2 adsorption/desorption isotherms. The factors influencing the adsorption efficiency and capacity had been systematically studied. Results showed that the adsorption was highly dependent on temperature, initial RhB concentration and adsorbent dose. Effects of initial solution pH indicate that the adsorption can proceed in both basic and acidic environment. The equilibrium absorption capacity at 25°C can reach up to 35.58 mg/g within 60 min implying the adsorption procedure was highly rapid. The kinetic data was better described by the pseudo-second-order model with the correlation coefficient (R2 = 0.9981), and the adsorption process followed Weber's intraparticle model, indicating the adsorption process could be divided into two stages. Results also showed that the adsorption equilibrium obeyed the Langmuir isotherm, and the value of equilibrium parameter RL suggested that the PZS nanotubes were an efficient adsorbent for the removal of RhB from aqueous solution.  相似文献   

14.
Commercial lipase from Burkholderia cepacia is immobilized on functionalized multi-walled carbon nanotubes (MWNT-COOH and MWNT-OH) provided by a physical adsorption. The immobilization processes for the carbon nanotubes are defined using immobilization time (0–30 min) and distinct adsorbent:adsorbate ratios (1:4, 1:7, and 1:10) with lipase loading of 100, 175, and 250 mg, respectively. The characterization of the immobilized preparations, the free lipase, and the pure nanotubes (MWNT-COOH and MWNT-OH) indicate that the lipase adsorption is increased. Thermogravimetric analysis, differential scanning calorimetry, and scanning electron microscopy are used. The specific surface area, pore volumes, and average pore diameters are determined by nitrogen adsorption–desorption isotherms. For the pure lipase, in the range between 40 and 300 °C, the micrograph is acquired. Experimental results clearly show an effective lipase adsorption in a lower period of time (5 min) in MWNT-COOH and MWNT-OH as well as a decrease in the surface area (98.30–45.9(86)?±?2.5 and 97.61–37.71?±?3.3(7) m2 g?1) and the pore volume (0.48–0.25?±?0.01 and 0.39–0.24?±?0.05 cm3 g?1), indicating that functionalized multi-walled carbon nanotubes can be successfully used as enzyme support.  相似文献   

15.
In this work, the interaction of an aspirin (AS) molecule with the external surface of a boron nitride fullerene-like nanocage (B12N12) is studied by means of density functional theory (DFT) calculations. Equilibrium geometry, electronic properties, adsorption energy and thermodynamic stability are identified for all of the adsorbed configurations. Four stable configurations are obtained for the interaction of AS molecule with the B12N12 nanocage, with adsorption energies in the range of ?10.1 to ?37.7 kcal/mol (at the M06-2X/6-31 + G** level). Our results clearly indicate that Al-doping of the B12N12 tends to increase the adsorption energy and thermodynamic stability of AS molecule over this nanocage. We further study the adsorption of AS over the B12N12 and B11N12Al in the presence of a protic (water) or aprotic (benzene) solvent. It is found that the calculated binding distances and adsorption energies by the PCM and CPCM solvent models are very similar, especially for the B12N12 complexes. According to time-dependent DFT calculations, the Al-doping can shift estimated λ max values toward longer wavelengths (redshift). Solvent effects also have an important influence on the calculated electronic absorption spectra of AS-B12N12 complexes.  相似文献   

16.
In this study, the use of the organic fraction of municipal solid waste as an abundant and low-cost raw material for producing activated carbon was investigated. For this purpose, ZnCl2 was used as a chemical activation agent and the carbonization process took place at 800 °C in N2 atmosphere. Seven sorbents were prepared by chemical activation (pyrolysis under N2 atmosphere at temperature of 800 °C after impregnation with ZnCl2) with different ratios of ZnCl2. The optimum ratio of organic fraction of municipal solid waste to ZnCl2 was inspected via methylene blue number and iodine number (ASTM Designation: D4607–94). The results showed that the adsorbent with 60 % ZnCl2/raw material was the most appropriate one with a satisfactory adsorption capacity, 112.4 mg g?1 for methylene blue and 134.0 mg g?1 for iodine. In addition, the structural analysis of this sorbent was performed using FT-IR, BET surface area, SEM–EDX and thermal analysis. Application of this sorbent to remove Cr(VI) from wastewater was studied to find an adsorption capacity of 66.7 mg g?1. The experimental adsorption equilibrium data were fitted to Langmuir adsorption model with an acceptable adsorption capacity of 66.7 mg g?1.  相似文献   

17.
To accomplish an effective analysis of adsorption, the strong acid dye from aqueous solution of sodium alginate (SA) and multi-walled carbon nanotubes (MWCNTs) composite gel beads were used as important parameters. Differential scanning calorimetry (DSC) was used to measure the heat of breakdown reaction. The experimental conditions were set at 0.5, 1, 2, 4, and 8 °C min?1, and the temperature range was 30–300 °C. The heating rates and the temperature range were set as follows: Four kinds of proportion in this experiment contained 2 SA % w/v (SA), 0.03, 0.09, 0.18, 0.36 % w/v (MWCNTs), and 10 % w/v calcium chloride, respectively. Four samples, 5, 6, 7, 8, and 9 mg, were used to detect the experimental data. It contributed to understanding the reaction for the distinctive MWCNTs. With the thermokinetic data by isoconversional approach obtained from advanced kinetics and technology solutions (AKTS), the related thermal safety information can be obtained from the thermal reaction of MWCNTs. Valuable parameters, such as activation energy (E a) and heat of decomposition, can be applied in operation, including adsorption and desorption processes. After DSC tests, and under the four compositions of SA/MWCNTs, at different heating rates of 0.5, 1, 2, 4, and 8 °C min?1, primarily we found that when the heating rate was increased, exothermic onset temperature would increase gradually. After analyzing E a value by isoconversional kinetics, we learned that in four different adsorption compositions, SA/MWCNTs0.03 (161.20 kJ mol?1) was the minimum. Among them, the highest value was SA/MWCNTs0.18 (220.48 kJ mol?1). However, in this study, for SA/MWCNTs compositions we found that E a value will drop in the final material SA/MWCNTs0.36. Accordingly, if the ratio of SA and calcium chloride was fixed, then different compositions of the MWCNTs would affect adsorption efficiency of SA/MWCNTs and E a variation.  相似文献   

18.
The feasibility of C3F8 abatement via combining nonthermal plasma with adsorption and/or catalysis is investigated in this study. In terms of the simultaneous combination of plasma, adsorption and catalysis (CPAC), three different configurations including A/C layer (adsorbent layer prior to catalyst layer), C/A layer (catalyst layer prior to adsorbent layer) and A/C mixture (adsorbent and catalyst are mechanically mixed) are adopted. For all the experimental tests conducted in this study, the gas stream consists of 500 ppm C3F8, 2% O2, and balanced N2. The experimental results indicate that C3F8 removal efficiencies depend on what kind of packing material is adopted (adsorbent, catalyst or both) and how the material is packed within the plasma reactor. The removal efficiencies obtained with different reactors are in the order as: CPAC (A/C layer; AC mixture) > CPA (plasma with adsorbent alone) > CPC (plasma with catalyst alone) > CPAC (C/A layer). The indentified products after treatment include CO2, CO, N2O and CF4. The formation of C2F6 is not observed in this study, which is encouraging since the global warming potential of C2F6 is actually higher than that of C3F8.  相似文献   

19.
We prepared poly(N,N-diethylacrylamide-co-acrylic acid) (P(DEA-co-AA)) microgels which could efficiently remove UO2 2+ from aqueous solutions. In this study, the effect of adsorption parameters such as pH value, adsorbent dose, shaking time, and temperature has investigated. It is found that the pseudo-second-order model is more suitable for our experiment. The adsorption kinetic data indicated that the chemical adsorption was the swiftness processes, the adsorption equilibrium could be achieved within 30 min. And there are very good correlation coefficients of linearized equations for Langmuir isotherm model, which indicated that the sorption isotherm of the hydrogel for UO2 2+ can be fitted to the Langmuir isotherm model. The adsorption process was spontaneous (?G 0 < 0) and exothermic (?H 0 < 0). The adsorbed UO2 2+ can be desorbed effectively by 0.1 M HNO3 and the adsorption capacity is not significantly reduced after five cycles. Present study suggests that this P(DEA-co-AA) can be used as a potential adsorbent for sorption UO2 2+ and also provide a simple, fast separation method for removal of UO2 2+ ions from aqueous solution.  相似文献   

20.
The properties of trioctylmethyl ammonium dodecanedioate (TAD) as a corrosion inhibitor (CI) of API 5L X52 steel in production water (PW) were evaluated in steady state using weight loss and polarization techniques within a Reynolds number (N Re ) interval ranging from 500 to 40,000. The highest obtained IE was 87 % at 100 ppm with N Re  = 2500, whereas the lowest IE was 15 % at 10 ppm with N Re  = 4000. TAD was classified as a mixed-type CI of API 5L X52 steel in PW. The \(\Delta G_{\text{ads}}^{^\circ }\) data established a relationship between the N Re and the adsorption process, confirming the occurrence of physical adsorption phenomena.  相似文献   

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