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1.
A new fluorescent hybrid porous polymer (HPP) is synthesized by an anhydrous FeCl3‐mediated oxidative coupling reaction of octa[4‐(9‐carbazolyl)phenyl]silsesquioxane (OCPS). The polymer possesses a surface area of 1741 m2 g?1 and hierarchical bimodal micropores (1.41 and 1.69 nm) and mesopores (2.65 nm). The material serves as an excellent adsorbent for CO2 and dyes with high adsorption capacity for CO2 (8.53 wt %,1.94 mmol g?1), congo red (1715 mg g?1) and rhodamine B (1501 mg g?1). In addition, the presence of peripheral cabozolyl groups with extended π‐conjugation in the crosslinked framework imparts luminescent character to the polymer and offers the detection of nitroaromatic compounds.  相似文献   

2.
Highly ordered amino‐functionalized hexagonal mesoporous silica (HMS‐NH2) had been synthesized successfully by co‐condensation. The resultant materials were characterized by means of XRD, TEM, FT‐IR, N2 ad‐desorption and 29Si NMR to confirm the ordered mesoporous structure and the functionalization of the amino groups. The sample was employed as a Pb2+ adsorbent in aqueous solutions at room temperature. Both Lagergren's first order kinetic model and Lagergren's second order kinetic model were used to describe the adsorption data. It was found that the pseudo second order model fitted the sorption kinetic data better than the pseudo first order model. According to the information analyzed from AAS, HMS‐NH2 had a Pb2+ adsorption amount of over 90.7 mg·g?1, showing a promising application for the treatment of wastewater containing Pb2+ ions.  相似文献   

3.
A microporous La–metal‐organic framework (MOF) has been synthesized by the reaction of La(NO3)3 ? 6 H2O with a ligand 4,4′,4′′‐s‐triazine‐1,3,5‐triyltri‐p‐aminobenzoate (TATAB) featuring three carboxylate groups. Crystal structure analysis confirms the formation of 3D MOF with hexagonal micropores, a Brunauer–Emmett—Teller (BET) surface area of 1074 m2 g?1 and high thermal and chemical stability. The CO2 adsorption capacities are 76.8 cm3 g?1 at 273 K and 34.6 cm3 g?1 at 293 K, a highest measured CO2 uptake for a Ln–MOFs.  相似文献   

4.
A new bi-functionalized xerogel is fabricated and then was identified by 29Si CP MAS NMR, SEM, FTIR, and nitrogen adsorption–desorption approaches. As-prepared xerogel efficiency for simultaneous uptake of methylene blue (MB) and Pb2+ ions from aqueous solution is investigated. Individual and combination effects of operating variables (xerogel mass, contact time and initial MB and Pb2+ ion concentration) on the retention performance is achieved with central composite design (CCD) and upgraded through response surface method (RSM). Batch equilibrium outcomes uncovered that MB and Pb2+ ions adsorption onto hybrid composite could be all around depicted by Langmuir isotherm model contrasted with Freundlich equation. Howbeit, the column trials reported that the breakthrough capacities of MB and Pb(II) are observed to be 512 mg.g−1 and 400 mg.g−1 respectively. XPS and FTIR investigations uncovered that the main mechanism of lead uptake ought to be credited to the chelation with –NH2 and ion exchange with –SH groups in the xerogel frameworks. While the MB adsorption system is proposed to be electrostatic attractions, π-π stacking interactions and hydrogen bonds. The work undertaken in this research highlights the major role of the as-synthesized xerogel for treatment of industrial wastewater.  相似文献   

5.
Heck coupling reactions are introduced as an efficient method to prepare porous polymers. Novel inorganic‐organic hybrid porous polymers (HPPs) were constructed via Heck coupling reactions from cubic functional polyhedral oligomeric silsesquioxanes (POSS), iodinated octaphenylsilsesquioxanes (OPS) and octavinylsilsesquioxanes (OVS) using Pd(OAc)2/PPh3 as the catalyst. Here, two iodinated OPS were used, IOPS and p‐I8OPS. IOPS was a mixture with 90% octasubstituted OPS (I8) and some nonasubstituted OPS (I9), while p‐I8OPS was a nearly pure compound with ≥99% I8 and ≥93% para‐substitution. IOPS and p‐I8OPS reacted with OVS to produce the porous materials HPP‐1 and HPP‐2, which exhibited comparable specific surface areas with SBET of 418 ± 20 m2 g−1 and 382 ± 20 m2 g−1, respectively, with total pore volumes of 0.28 ± 0.01 cm3 g−1 and 0.23 ± 0.01 cm3 g−1, respectively. HPP‐1 showed a broader pore size distribution and possessed a more significant contribution from the mesopores, when compared with HPP‐2, thereby indicating that IOPS may induce more disorder because of the geometrical asymmetry. HPP‐1 and HPP‐2 possessed moderate carbon dioxide uptakes of 134 and 124 cm3 g−1 at 1 bar at 195 K, making them promising candidates for CO2 capture and storage. The synthesized porous polymers may be easily post‐functionalized using the retained ethenylene groups.

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6.
A nanostructured organic–inorganic framework, hexagonal NH2‐MIL‐88B, has been prepared through a facile one‐pot reflux reaction and then it was characterized using various techniques. The as‐prepared sample with high specific surface area (414 m2 g?1) showed excellent adsorption for 2,4,6‐trinitrophenol (TNP) in the liquid phase. Detailed studies of the adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were conducted. The adsorption mechanism of NH2‐MIL‐88B for TNP may be ascribed to hydrogen bond interaction, and the complexation between ─OH in TNP and unsaturated Fe(III) on the surface of NH2‐MIL‐88B. The maximum adsorption capacity of NH2‐MIL‐88B for TNP based on the Langmuir isotherm was 163.66 mg g?1. The as‐prepared NH2‐MIL‐88B adsorbent seems to be a promising material in practice for TNP removal from aqueous solution.  相似文献   

7.
It is of vital importance to capture lanthanides (nuclear fission products) from waste solutions for radionuclide remediation owing to their hazards. The effective separation of lanthanides are achieved by an acid/base‐stable and radiation‐resistant vanadate, namely, [Me2NH2]V3O7 ( 1 ). It exhibits high adsorption capacities for lanthanides (qmEu=161.4 mg g?1; qmSm=139.2 mg g?1). And high adsorption capacities are maintained over a pH range of 2.0–6.9 (qmEu=75.1 mg g?1 at low pH of 2.5). It displays high selectivity for Eu3+ (simulant of An3+) against a large excess of interfering ions. It can efficiently separate Eu3+ and Cs+ (or Sr2+) with the highest separation factor SFEu/Cs of 156 (SFEu/Sr of 134) to date. The adsorption mechanism is revealed by calculations and XPS, EXAFS, Raman, and elemental analyses. These merits combined with facile synthesis and convenient elution makes the title vanadate a promising lanthanide scavenger for environmental remediation.  相似文献   

8.
Various polyoxometalates (POMs) were successfully immobilized to the mesoporous coordination polymer MIL‐101 resulting in a series of POM–MOF composite materials POM@MIL‐101 (POM=K4PW11VO40, H3PW12O40, K4SiW12O40). These materials were synthesized by a simple one‐pot reaction of Keggin POMs, tetramethylammonium hydroxide (TMAH), terephthalic acid (H2bdc), and Cr3+ ions. XRD, FTIR, thermogravimetric analyses (TG), inductively coupled plasma (ICP) spectrometry, and energy‐dispersive X‐ray spectroscopy (EDX) collectively confirmed the successful combination of POMs and the porous framework. Further, these composites POM@MIL‐101 with different loading of POMs were achieved by variation of the POM dosage. Notably, the uptake capacity of MIL‐101 towards organic pollutants in aqueous solution was significantly improved by immobilization of hydrophilic POMs into cages of MIL‐101. An uptake capacity of 371 mg g?1, comparable to that of the graphene oxide sponges, and much higher than that of the commercial activated carbon, was achieved at room temperature in 5 min when dipping 20 mg PW11V@MIL‐101 in the methylene blue (MB) solution (100 mL of 100 mg L?1 MB solution). Further study revealed that the POM@MIL‐101 composite materials not only exhibited a fast adsorption rate towards dye molecules, but also possessed of selective adsorption ability of the cationic dyes in wastewater. For example, the adsorption efficiency of PW11V@MIL‐101 (10 mg) towards MB (100 mL of 10 mg L?1) could reach 98 % in the initial 5 min, and it could capture MB dye molecules from the binary mixture of the MB and MO with similar size. Also, the POM@MIL‐101 materials could be readily recycled and reused, and no POM leached in the dye adsorption process.  相似文献   

9.
We evaluated the ability of CO2 adsorption in functionalized activated carbons granular and monolithic type, obtained by chemical activation of African palm stone with H3PO4 and CaCl2. We made a comparison between two methods of incorporation of nitrogen groups: the impregnation method with NH4OH solution and NH3 gasification. The materials were texturally characterized by N2 adsorption at 77 K, the isotherms shows obtaining microporous materials with surface areas between 545–1425 m2?g?1 and pore volumes between 0.22 to 0.53 cm3?g?1. It was established that with the methodologies used for functionalization is increased content of nitrogen groups, was achieved a higher proportion of such groups when carrying out the process in liquid phase with NH4OH. The incorporation of nitrogen groups in the material generates an increase of up to 65 % in the CO2 adsorption capacity of the MCa2 (Monolith prepared with CaCl2 solution at 2 %) sample. Was reached a maximum adsorption capacity of 344 mgCO2?g?1 in the MCa2FAL (sample MCa2 functionalized with NH4OH solution) sample.  相似文献   

10.
A new amino‐functionalized strontium–carboxylate‐based metal–organic framework (MOF) has been synthesized that undergoes single crystal to single crystal (SC‐to‐SC) transformation upon desolvation. Both structures have been characterized by single‐crystal X‐ray analysis. The desolvated structure shows an interesting 3D porous structure with pendent ?NH2 groups inside the pore wall, whereas the solvated compound possesses a nonporous structure with DMF molecules on the metal centers. The amino group was postmodified through Schiff base condensation by pyridine‐2‐carboxaldehyde and palladium was anchored on that site. The modified framework has been utilized for the Suzuki cross‐coupling reaction. The compound shows high activity towards the C?C cross‐coupling reaction with good yields and turnover frequencies. Gas adsorption studies showed that the desolvated compound had permanent porosity and was microporous in nature with a BET surface area of 2052 m2 g?1. The material also possesses good CO2 (8 wt %) and H2 (1.87 wt %) adsorption capabilities.  相似文献   

11.
Maleic anhydride–styrene–methyl methacrylate (MA–S–MM) terpolymer was prepared. It was modified by ethylenediamine (EDA) and diethylenetriamine (DETA) in order to get cross-linked polymers bearing carboxyl and amine groups. Modified polymers used as an adsorbent for the removal of UO2 2+ from water. The characterizations of structures of all the polymers were performed by Fourier transform infrared. The adsorptive features of adsorbents were then investigated for UO2 2+ in view of dependency on ion concentration, pH, temperature and kinetics. Experimentally obtained isotherms were evaluated with reference to Langmuir, Freundlich and Dubinin–Radushkevich models. The maximum monolayer adsorption capacity for UO2 2+ was found to be 1.59 and 2.43 mol kg?1 for EDA–MA–S–MM and DETA–MA–S–MM, respectively. It can be said that the new modified polymers prepared in our laboratory have been suggested as new adsorbents for uranyl ions.  相似文献   

12.
In the present work, high quality γ‐Mo2N catalysts for ammonia decomposition were successfully synthesized via temperature programmed nitridation of α‐MoO3 nanobelts. The optimal conditions for the synthesis of MoO3 precursors were obtained by using the orthogonal experimental method. The MoO3 precursors and the corresponding fresh and used Mo2N catalysts were characterized by various characterization techniques, including transmission electron microscopy, X‐ray diffraction and N2 adsorption‐desorption. Furthermore, temperature‐ programmed desorption by N2 or NH3 and X‐ray photoelectron spectroscopy analysis were performed to better understand the chemical properties of Mo2N catalysts. The results revealed that Mo2N catalyst has good NH3 adsorption ability and facilitates the dissociation adsorption of N2. Moreover, the morphology and structure of Mo2N catalysts well maintained after the reaction. Therefore, among the three transition metal nitrides (Mo2N, W2N and VN) and some Mo‐based catalysts previously reported, Mo2N catalysts showed very high activity and stability. Nearly 94% conversion of NH3 could be reached at 550°C with the gas hourly space velocity of 22000 cm3?gcat–1?h–1 and no obvious deactivation was observed during a 72 h test.  相似文献   

13.
A series of amphiphilic silica/fluoropolymer nanoparticles of SiO2g‐P(PEGMA)‐b‐P(12FMA) were prepared by silica surface‐initiating atom transfer radical polymerization (SI‐ATRP) of poly(ethylene glycol) methyl ether methacrylate (PEGMA) and poly dodecafluoroheptyl methacrylate (P12FMA). Their amphiphilic behavior, lower critical solution temperature (LCST), and surface properties as protein‐resistance coatings were characterized. The introduction of hydrophobic P(12FMA) block leads SiO2‐g‐P(PEGMA)‐b‐P(12FMA) to form individual spherical nanoparticles (~150 nm in water and ~170 nm in THF solution) as P(PEGMA)‐b‐P(12FMA) shell grafted on SiO2 core (~130 nm), to gain obvious lower LCST at 36–52 °C and higher thermostability at 290–320 °C than SiO2‐g‐P(PEGMA) (LCST = 78–90 °C, Td = 220 °C). The water‐casted SiO2‐g‐P(PEGMA)‐b‐P(12FMA) films obtain much rougher surface (125.3–178.4 nm) than THF‐casted films (11.5–16.9 nm) and all SiO2‐g‐P(PEGMA) films (26.8–31.3 nm). Therefore, the water‐casted surfaces exhibit obvious higher water adsorption amount (Δf = ?494 ~ ?426 Hz) and harder adsorbed layer (viscoelasticity of ΔDf = ?0.28 ~ ?0.36 × 10?6/Hz) than SiO2‐g‐P(PEGMA) films, but present loser adsorbed layer than THF‐casted films (ΔDf = ?0.29 ~ ?0.63 × 10?6/Hz). While, the introduction of P(12FMA) segments does not show obviously reduce in the protein‐repelling adsorption of SiO2‐g‐P(PEGMA)‐b‐P(12FMA) films (△f = ?15.7 ~ ?22.3 Hz) compared with SiO2‐g‐P(PEGMA) films (△f = ?8.3 ~ ?11.3 Hz) and no obvious influence on water adsorption of ancient stone. Therefore, SiO2‐g‐P(PEGMA)‐b‐P(12FMA) is suggested to be used as protein‐resistance coatings. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016 , 54, 381–393  相似文献   

14.
Ion diffusion efficiency at the solid–liquid interface is an important factor for energy storage and adsorption from aqueous solution. Although K2Mn4O8 (KMO) exhibits efficient ion diffusion and ion‐exchange capacities, due to its high interlayer space of 0.70 nm, how to enhance its mass transfer performance is still an issue. Herein, novel layered KMO/reduced graphene oxide (RGO) nanocomposites are fabricated through the anchoring of KMO nanoplates on RGO with a mild solution process. The face‐to‐face structure facilitates fast transfer of lithium and lead ions; thus leading to excellent lithium storage and lead ion adsorption. The anchoring of KMO on RGO not only increases electrical conductivity of the layered nanocomposites, but also effectively prevents aggregation of KMO nanoplates. The KMO/RGO nanocomposite with an optimal RGO content exhibits a first cycle charge capacity of 739 mA h g?1, which is much higher than that of KMO (326 mA h g?1). After 100 charge–discharge cycles, it still retains a charge capacity of 664 mA h g?1. For the adsorption of lead ions, the KMO/RGO nanocomposite exhibits a capacity of 341 mg g?1, which is higher than those of KMO (305 mg g?1) and RGO (63 mg g?1) alone.  相似文献   

15.
The complex [Cu(phen)2(POAc)3]ClO·4H2O has been synthesized and investigated by elemental analysis, IR spec-troscopy and X-ray diffraction methods, where phen = 1,10-phenanthroline, POAc = phenylacetate group). The complex crystallizes in the triclinic space group PI with two molecules in a unit cell of dimensions a = 1.0579(2) nm, b = 1.2423(3) nm, c = 1.9190(4) nm, α = 71.84(1)°, β = 80.50(2)°, γ = 88.60(1)°, V = 2.3625(9) nm3, R = 0.0407 and Rw = 0.0656. The complex results from bridging of two Cu(phen)2 units by three carboxylate groups, and each Cu2 ion is in a distorted square pyramidal geometry with two nitrogen atoms of phen and three carboxylate oxygen atoms of POAc. It has been showed that intramolecular stacking interactions occur between the phenyl moieties of POAc and aromatic rings of phen, leading to a novel molecule structure with two coordinating modes of carboxylate ligands, of which two phenylacetates are μ2-carboxylate-O-bridging ligands, and the other is a μ2-carboxylate-  相似文献   

16.
Three isostructural lanthanide‐based two‐ dimensional coordination polymers (CPs) {[Ln2(L)3(H2O)2]n ? 2n CH3OH) ? 2n H2O} (Ln=Gd3+ ( 1 ), Tb3+ ( 2 ), Dy3+ ( 3 ); H2L=cyclobutane‐1,1‐dicarboxylic acid) were synthesized by using a low molecular weight dicarboxylate ligand and characterized. Single‐crystal structure analysis showed that in complexes 1 – 3 lanthanide centers are connected by μ3‐bridging cyclobutanedicarboxylate ligands along the c axis to form a rod‐shaped infinite 1D coordination chain, which is further linked with nearby chains by μ4‐connected cyclobutanedicarboxylate ligands to form 2D CPs in the bc plane. Viewing the packing of the complexes down the b axis reveals that the lattice methanol molecules are located in the interlayer space between the adjacent 2D layers and form H‐bonds with lattice and coordinated water molecules to form 1D chains. Magnetic properties of complexes 1 – 3 were thoroughly investigated. Complex 1 exhibits dominant ferromagnetic interaction between two nearby gadolinium centers and also acts as a cryogenic magnetic refrigerant having a significant magnetic entropy change of ?ΔSm=32.8 J kg?1 K?1 for ΔH=7 T at 4 K (calculated from isothermal magnetization data). Complex 3 shows slow relaxation of magnetization below 10 K. Impedance analysis revealed that the complexes show humidity‐dependent proton conductivity (σ=1.5×10?5 S cm?1 for 1 , σ=2.07×10?4 S cm?1 for 2 , and σ=1.1×10?3 S cm?1 for 3 ) at elevated temperature (>75 °C). They retain the conductivity for up to 10 h at high temperature and high humidity. Furthermore, the proton conductivity results were correlated with the number of water molecules from the water‐vapor adsorption measurements. Water‐vapor adsorption studies showed hysteretic and two‐step water vapor adsorption (182000 μL g?1 for 1 , 184000 μL g?1 for 2 , and 1874000 μL g?1 for 3 ) in the experimental pressure range. Simulation of water‐vapor adsorption by the Monte Carlo method (for 1 ) confirmed the high density of adsorbed water molecules, preferentially in the interlayer space between the 2D layers.  相似文献   

17.
The present study deals with the synthesis and characterization (FE‐SEM, particle size distribution, XRD and point of zero charge) SnO2/(NH4)2‐SnCl6 nanocomposites loaded on activated carbon (SnO2/(NH4)2‐SnCl6‐NCs‐AC) and its subsequent application for the simultaneous removal of Methylene Blue (MB) and Orange G (OG) from aqueous solution. Response surface methodology (RSM) based on central composite design (CCD) give trend of influencing responses with respect to five parameters such as contact time (X1), OG concentration (X2), MB concentration (X3), adsorbent mass (X4) and pH (X5). In later stage following recognition of significant variables and interaction, quadratic model generated which are able to predict the dyes removal in different conditions. Justification and selection of significant terms was conducted based on analysis of variance and Fisher's F‐test Optimal value of contact time, OG concentration, MB concentration, adsorbent mass and pH were set at 4.0 min, 10 mg l?1, 20 mg L?1, 0.015 g and 6.0, respectively, which lead to achievement of best experiment removal percentage of 97.0 and 99.5% OG and MB respectively, from their binary solutions. The whole experimental data follow pseudo‐first‐order and pseudo‐second‐order rate equations. The fitting experimental data to more available conventional model like Langmuir, Freundlich, Temkin and Dubinin‐Radushkevich isotherm models revel more ability of Langmuir model (with R2 > 0.997) for explanation of system in equilibrium. The adsorption efficiency remained high even after the five cycle of reuse (99.76% and 95.56% for MB and OG, respectively).  相似文献   

18.
The graft polymers [poly(isoprene)‐graft‐poly(styrene)] (PI‐g‐PS), [poly(isoprene)‐graft‐poly(isoprene)] (PI‐g‐PI), [poly(isoprene)‐graft‐(poly(isoprene)‐block‐poly(styrene))] PI‐g‐(PI‐b‐PS), and [poly(isoprene)‐graft‐(poly(styrene)‐block‐poly(isoprene))] PI‐g‐(PS‐b‐PI) with PI as main chain were synthesized through living anionic polymerization (LAP) mechanism and the efficient coupling reaction. First, the PI was synthesized by LAP mechanism and epoxidized in H2O2/HCOOH system for epoxidized PI (EPI). Then, the graft polymers with controlled molecular weight of main chain and side chains, and grafting ratios were obtained by coupling reaction between PI?Li+, PS?Li+, PS‐b‐PI?Li+, or PI‐b‐PS?Li+ macroanions and the epoxide on EPI. The target polymers and all intermediates were well characterized by SEC,1H NMR, as well as their thermal properties were also evaluated by DSC. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2012  相似文献   

19.
Amino group-functionalized Fe3O4 is loaded on a coordination complex-modified polyoxometalate nanoparticle. In this composite material, Fe3O4 and coordination complex-modified polyoxometalate are connected with intense hydrogen bonds as suggested by FTIR. This composite material exhibits excellent methylene blue (MB) adsorption, with adsorption capacity of 175.5 mg g?1. It also possesses selective separation ability between cationic and anionic dye molecules. In binary solution of MB and methyl orange (MO), MB adsorption efficiency reaches 75%, but it exhibits almost no effect on the adsorption of methyl orange. The saturation magnetization value of this composite material is 18.89 emu g?1, allowing magnetic separation, which facilitates the recycle and reuse of this composite adsorbent.  相似文献   

20.
n‐Dodecyltriethoxysilane (DTEOS) modified NaHSO4/MCM‐41 catalysts (silanized catalysts) were synthesized by different impregnation sequences and evaluated in the liquid‐phase dehydration of castor oil. The samples were evaluated by X‐ray diffraction, nitrogen adsorption‐desorption, SEM, TEM, FT‐IR spectroscopy, XPS, 29Si MAS NMR spectroscopy, contact angle measurements, NH3‐TPD, and pyridine‐FT‐IR spectroscopy. The analyses demonstrated that silanization enhanced the hydrophobicity of the catalysts, and the impregnation sequence of silanized catalysts had a significant effect on the NaHSO4 dispersion, surface area, acid distribution, and hydrophobicity of the silanized catalysts. The catalytic activity of the silanized catalysts was much higher than that of NaHSO4/MCM‐41. Among the silanized catalysts, the catalyst prepared by simultaneous impregnation with DTEOS and NaHSO4 showed the highest iodine value of 141.8 [g(I2) per 100 g] and lowest hydroxyl value of 11.3 [mg(KOH) · g–1].  相似文献   

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