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71.
A Novel Bismuth‐Based Metal–Organic Framework for High Volumetric Methane and Carbon Dioxide Adsorption 下载免费PDF全文
Mathew Savage Dr. Sihai Yang Dr. Mikhail Suyetin Prof. Dr. Elena Bichoutskaia Dr. William Lewis Prof. Dr. Alexander J. Blake Sarah A. Barnett Prof. Dr. Martin Schröder 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(26):8024-8029
Solvothermal reaction of H4L (L=biphenyl‐3,3′,5,5′‐tetracarboxylate) and Bi(NO3)3 ? (H2O)5 in a mixture of DMF/MeCN/H2O in the presence of piperazine and nitric acid at 100 °C for 10 h affords the solvated metal–organic polymer [Bi2(L)1.5(H2O)2] ? (DMF)3.5 ? (H2O)3 (NOTT‐220‐solv). A single crystal X‐ray structure determination confirms that it crystallises in space group P2/c and has a neutral and non‐interpenetrated structure comprising binuclear {Bi2} centres bridged by tetracarboxylate ligands. NOTT‐220‐solv shows a 3,6‐connected network having a framework topology with a {4 ? 62}2{42 ? 65 ? 88}{62 ? 8} point symbol. The desolvated material NOTT‐220a shows exceptionally high adsorption uptakes for CH4 and CO2 on a volumetric basis at moderate pressures and temperatures with a CO2 uptake of 553 g L?1 (20 bar, 293 K) with a saturation uptake of 688 g L?1 (1 bar, 195 K). The corresponding CH4 uptake was measured as 165 V(STP)/V (20 bar, 293 K) and 189 V(STP/V) (35 bar, 293 K) with a maximum CH4 uptake for NOTT‐220a recorded at 20 bar and 195 K to be 287 V(STP)/V, while H2 uptake of NOTT‐220a at 20 bar, 77 K is 42 g L?1. These gas uptakes have been modelled by grand canonical Monte Carlo (GCMC) and density functional theory (DFT) calculations, which confirm the experimental data and give insights into the nature of the binding sites of CH4 and CO2 in this porous hybrid material. 相似文献
72.
This study confirms the enzyme-mediated phosphorylation of cellulose nanofibers (CNF) by using hexokinase and adenosine-5′-triphosphate in the presence of Mg-ions, resulting in a phosphate group’s creation predominantly at C-6-O positioned hydroxyl groups of cellulose monomer rings. A proof-of-concept is provided using 12C CPMAS, 31P MAS nuclear magnetic resonance, attenuated total reflectance-Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy (XPS) analyzing methods. The degree of substitution (DS) is determined by elemental analysis and compared to DS estimated by XPS analysis. From the thermal degradation measurements using thermo-gravimetric analysis, the C-6-O phosphorylation was found to noticeably prevent the CNF derivatives from weight loss in the pyrolysis process, thus, providing them flame-resistance functionality. Furthermore, phosphorylation significantly enhanced adsorption capacity of Fe3+ ions making them interesting for fabrication of biobased filters and membranes. Finally, the biomimetic growth of Ca–P crystals (hydroxyapatite) in simulated body fluid was characterized by scanning electron microscopy and energy dispersive X-ray, showing potential application as biomedical materials. 相似文献
73.
Houssine Sehaqui Uxua Perez de Larraya Peng Liu Numa Pfenninger Aji P. Mathew Tanja Zimmermann Philippe Tingaut 《Cellulose (London, England)》2014,21(4):2831-2844
Biobased nanofibers are increasingly considered in purification technologies due to their high mechanical properties, high specific surface area, versatile surface chemistry and natural abundance. In this work, cellulose and chitin nanofibers functionalized with carboxylate entities have been prepared from pulp residue (i.e., a waste product from the pulp and paper production) and crab shells, respectively, by chemically modifying the initial raw materials with the 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) mediated oxidation reaction followed by mechanical disintegration. A thorough investigation has first been carried out in order to evaluate the copper(II) adsorption capacity of the oxidized nanofibers. UV spectrophotometry, X-ray photoelectron spectroscopy and wavelength dispersive X-rays analysis have been employed as characterization tools for this purpose. Pristine nanofibers presented a relatively low content of negative charges on their surface thus adsorbing a low amount of copper(II). The copper adsorption capacity of the nanofibers was enhanced due to the oxidation treatment since the carboxylate groups introduced on the nanofibers surface constituted negative sites for electrostatic attraction of copper ions (Cu2+). The increase in copper adsorption on the nanofibers correlated both with the pH and carboxylate content and reached maximum values of 135 and 55 mg g?1 for highly oxidized cellulose and chitin nanofibers, respectively. Furthermore, the metal ions could be easily removed from the contaminated nanofibers through a washing procedure in acidic water. Finally, the adsorption capacity of oxidized cellulose nanofibers for other metal ions, such as nickel(II), chromium(III) and zinc(II), was also demonstrated. We conclude that TEMPO oxidized biobased nanofibers from waste resources represent an inexpensive and efficient alternative to classical sorbents for heavy metal ions removal from contaminated water. 相似文献
74.
Solid polymer electrolytes (SPEs) with high ionic conductivity and acceptable mechanical properties are of particular interest for increasing the performance of batteries. In the present work, SPEs based on poly(ethylene oxide)/poly (vinyl pyrrolidone) (PEO/PVP) with various lithium salts were prepared by solvent casting technique. The amorphous nature of the polymer-salt complex was studied by X-ray diffraction analysis. The complexation of the prepared electrolytes was confirmed by Fourier transform infrared analysis. Ionic conductivity as a function of frequency was studied at various temperatures in the range of 303–353 K. The maximum ionic conductivity value was found to be 1.08 × 10?5 S/cm for the film containing lithium bis trifluoromethane sulfonoimide (LiN[CF3SO2]2) at room temperature and the temperature dependent ionic conductivity values seem to obey Vogel-Tamman-Fulcher relation. Thermogravimetry was used to ascertain the thermal stability of the electrolytes. Photoluminescence measurements demonstrated that the sample having maximum ionic conductivity shows the minimum luminescence intensity. Ultra violet-visible analysis reveals that the values of the band gap energies were changed with the addition of various lithium salts. Porosity of the sample containing lithium bis trifluoromethane sulfonoimide (LiN[CF3SO2]2) was studied by Atomic force microscope. 相似文献
75.
K.Kesavan Chithra M.Mathew S.Rajendran 《中国化学快报》2014,25(11):1428-1434
Poly(ethylene oxide), poly(vinyl pyrrolidone)(PEO/PVP), lithium perchlorate salt(Li Cl O4) and different plasticizer based, gel polymer electrolytes were prepared by the solvent casting technique. XRD results show that the crystallinity decreases with the addition of different plasticizers. Consequently, there is an enhancement in the amorphousity of the samples responsible for the process of ion transport. FTIR spectroscopy is used to characterize the structure of the polymer and confirms the complexation of plasticizer with host polymer matrix. The ionic conductivity has been calculated using the bulk impedance obtained through impedance spectroscopy. Among the various plasticizers, the ethylene carbonate(EC) based complex exhibits a maximum ionic conductivity value of the order of2.7279 10 4S cm 1. Thermal stability of the prepared electrolyte films shows that they can be used in batteries at elevated temperatures. PEO(72%)/PVP(8%)/Li Cl O4(8%)/EC(12%) has the maximum ionic conductivity value which is supported by the lowest optical band gap and lowest intensity in photoluminescence spectroscopy near 400–450 nm. Two and three dimensional topographic images of the sample having a maximum ionic conductivity show the presence of micropores. 相似文献
76.
Nair Supriya Aswathy UV Mathew Ann Raghavan Rajeev 《Journal of Thermal Analysis and Calorimetry》2017,128(3):1731-1741
Journal of Thermal Analysis and Calorimetry - Thermal decomposition, thermal conductivity, specific heat and flammability of polydimethyl siloxane (PDMS) resin and three PDMS-based systems with... 相似文献
77.
78.
Mathew A. Cleveland Nick A. Gentile Todd S. Palmer 《Journal of computational physics》2010,229(16):5707-5723
Implicit Monte Carlo (IMC) and Implicit Monte Carlo Diffusion (IMD) are approaches to the numerical solution of the equations of radiative transfer. IMD was previously derived and numerically tested on grey, or frequency-integrated problems [1]. In this research, we extend Implicit Monte Carlo Diffusion (IMD) to account for frequency dependence, and we implement the difference formulation [2] as a source manipulation variance reduction technique. We derive the relevant probability distributions and present the frequency dependent IMD algorithm, with and without the difference formulation. The IMD code with and without the difference formulation was tested using both grey and frequency dependent benchmark problems. The Su and Olson semi-analytic Marshak wave benchmark was used to demonstrate the validity of the code for grey problems [3]. The Su and Olson semi-analytic picket fence benchmark was used for the frequency dependent problems [4]. The frequency dependent IMD algorithm reproduces the results of both Su and Olson benchmark problems. Frequency group refinement studies indicate that the computational cost of refining the group structure is likely less than that of group refinement in deterministic solutions of the radiation diffusion methods. Our results show that applying the difference formulation to the IMD algorithm can result in an overall increase in the figure of merit for frequency dependent problems. However, the creation of negatively weighted particles from the difference formulation can cause significant numerical instabilities in regions of the problem with sharp spatial gradients in the solution. An adaptive implementation of the difference formulation may be necessary to focus its use in regions that are at or near thermal equilibrium. 相似文献
79.
Noncovalent engineering of carbon nanotube surfaces by rigid,functional conjugated polymers 总被引:8,自引:0,他引:8
Chen J Liu H Weimer WA Halls MD Waldeck DH Walker GC 《Journal of the American Chemical Society》2002,124(31):9034-9035
We report a new nonwrapping approach to noncovalent engineering of carbon nanotube surfaces by short, rigid functional conjugated polymers, poly(aryleneethynylene)s. Our technique not only enables the dissolution of various types of carbon nanotubes in organic solvents, which represents the first example of solubilization of carbon nanotubes via pi-stacking without polymer wrapping, but could also introduce numerous neutral and ionic functional groups onto the carbon nanotube surfaces. 相似文献
80.
Craig F Ferris Tara Stolberg Praveen Kulkarni Murali Murugavel Robert Blanchard D Caroline Blanchard Marcelo Febo Mathew Brevard Neal G Simon 《BMC neuroscience》2008,9(1):111