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ABSTRACT: Developing a synthetic methodology for the fabrication of hierarchically porous metal-organic monoliths that feature high surface area, low density and tunable porosity is imperative for mass transfer applications, including bulky molecule capture, heterogeneous catalysis and drug delivery. Here we report a versatile and facile synthetic route towards ultralight micro/mesoporous metal-organic aerogels based on the two-step gelation of metal-organic framework nanoparticles. Heating represents a key factor in the control of gelation versus crystallization of Al(III)-multicarboxylate systems. The porosity of the resulting metal-organic aerogels can be readily tuned, leading to the formation of well-ordered intraparticle micropores and aerogel-specific interparticle mesopores, thereby integrating the merits of both crystalline metal-organic frameworks and light aerogels. The hierarchical micro/mesoporosity of the Al-metal-organic aerogels is thoroughly evaluated by N2 sorption. The good accessibility of the micro/mesopores is verified by vapour/dye uptake, and their potential for utilization as effective fibre-coating absorbents is tested in solid-phase microextraction analyses.
Nature Communications 01/2013; 4:1774. · 7.40 Impact Factor
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ABSTRACT: A combined and sequential use of quantum mechanical (QM) calculations and classical molecular dynamics (MD) simulations was made to investigate the σ and π types of hydrogen bond (HB) in benzene-water and pyrrole-water as clusters and as their liquid mixture, respectively. This paper aims at analyzing similarities and differences of these HBs resulted from QM and MD on an equal footing. Based on the optimized geometry at ωb97xD/aug-cc-pVTZ level of theory, the nature and property of σ and π types of HBs are unveiled by means of atoms in molecules (AIM), natural bond orbital (NBO) and energy decomposition analysis (EDA). In light of the above findings, MD simulation with OPLS-AA and SPC model was applied to study the liquid mixture at different temperatures. The MD results further characterize the behavior and structural properties of σ and π types HBs, which are somewhat different but reasonable for the clusters by QM. Finally, we provide a reasonable explanation for the different solubility between benzene/water and pyrrole/water.
Journal of Molecular Modeling 11/2012; · 1.80 Impact Factor
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ABSTRACT: Self-diffusion and structural properties of n-alkanes have been studied by molecular dynamics simulation in the temperature range between the melting pressure curve and 600 K at pressures up to 300 MPa. The simulated results of lower n-alkanes are in good agreement with the existing experimental data, and support the reliability of results of the simulations of self-diffusion coefficients obtained at the extreme conditions. We predict the self-diffusion coefficients for methane, ethane, propane and n-butane at the similar reduced temperatures and pressures to draw a comparison between them. Then the correlation between self-diffusion and structural properties are further investigated by calculating the coordination numbers. Moreover, we define four distances and their corresponding relative deviations to characterize the flexibility of long-chain n-alkanes. The simulated results show that the self-diffusion of n-alkane molecules is mainly affected by the close packing, and the flexibility has a strong impact on the self-diffusion of longer n-alkane molecules.
Journal of Molecular Modeling 07/2012; · 1.80 Impact Factor
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ABSTRACT: An assessment study is presented about energy decomposition analysis (EDA) in combination with DFT including revised dispersion correction (DFT-D3) with Slater-type orbital (STO) basis set. There has been little knowledge about the performance of the EDA + DFT-D3 concerning STOs. In this assessment such an approach was applied to calculate noncovalent interaction energies and their corresponding components. Complexes in S22 set were used to evaluate the performance of EDA in conjunction with four representative types of GGA-functionals of DFT-D3 (BP86-D3, BLYP-D3, PBE-D3 and SSB-D3) with three STO basis sets ranging in complexity from DZP, TZ2P to QZ4P. The results showed that the approach of EDA + BLYP-D3/TZ2P has a better performance not only in terms of calculating noncovalent interaction energy quantitatively but also in analyzing corresponding energy components qualitatively. This approach (EDA + BLYP-D3/TZ2P) was thus applied further to two representative large-system complexes including porphine dimers and fullerene aggregates to gain a better insight into binding characteristics.
Journal of Molecular Modeling 05/2012; 18(10):4577-89. · 1.80 Impact Factor
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Chemistry 02/2011; 17(8):2369-72. · 5.93 Impact Factor
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ABSTRACT: Self-diffusion and structural properties of ammonia, methylamine and trimethylamine have been studied by molecular dynamics simulation in the temperature range between the melting pressure curve and 700 K at pressures up to 400 MPa. The calculation results agree well with the experiment, which suggests that one can use the simulation method as a powerful tool to obtain self-diffusion coefficients over wide range of temperatures and pressures, under which it is rather difficult for experiments. The local structures of such fluids are investigated by calculating radial distribution functions (RDFs), the numbers of hydrogen bonds and coordination numbers. The correlation between self-diffusion and structural properties, and the influence of temperature and pressure on them are discussed. The simulation results demonstrate that the temperature effects are more pronounced than the pressure effects on self-diffusion and structural properties, and the effect of hydrogen bonding on the translational dynamics in any of these systems is a minor factor, while it is mainly affected by the close packing of amine molecules.
Physical Chemistry Chemical Physics 12/2010; 12(45):15007-17. · 3.57 Impact Factor
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ABSTRACT: Inorganic/polymer nanocomposite silica-poly(N-isopropylacrylamide) (SiO(2)-PNIPA) was successfully synthesized through a one-pot approach in supercritical carbon dioxide (scCO(2)). All raw materials, N-isopropylacrylamide (NIPA), vinyltriethoxysilane (VTEO), tetraethoxysilane (TEOS), initiator 2,2'-azobisisobutyronitrile (AIBN), crosslinker N,N'-methylenebisacrylamide (MBAM) and hydrolysis agent acetic acid (AA) were introduced into one autoclave and the parallel reactions of free radical polymerization and hydrolysis/condensation occurred simultaneously in the reaction mixture with scCO(2) as solvent. The obtained novel composite particles were characterized by Fourier transform infrared spectroscopy (FTIR), scanning electronic microscopy (SEM), transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS). The swelling ratios (SR) and lower critical solution temperatures (LCSTs) of the prepared thermoresponsive microspheres were investigated by swelling tests and ultraviolet-visible (UV) spectrophotometry, respectively. TEM images demonstrated that well-dispersed particles with diameter less than 100 nm were formed. The composite microgels exhibited higher LCSTs than poly(N-isopropylacrylamide) (PNIPA) microgels did. The in vitro release simulation of the particles in situ impregnated with ibuprofen indicated that SiO(2)-PNIPA composites could improve the drug releasing effect of the microgels as controlled drug delivery systems.
Journal of Colloid and Interface Science 11/2009; 343(1):141-8. · 3.07 Impact Factor
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ABSTRACT: The clinically applied value of myocardial perfusion and systolic function in patients with coronary artery disease after coronary artery bypass surgery using real-time myocardial contrast echocardiography (RT-MCE) combined with two-dimensional strain echocardiography was assessed. Twenty patients underwent intravenous RT-MCE by intravenous injections of SonoVue before and after coronary artery bypass surgery. Two-dimensional images were recorded from the left ventricular four-chamber view, two-chamber view and the apical view before, and two weeks and three months after coronary artery bypass surgery, and the peak systolic longitudinal strain was measured. The results showed that myocardial perfusion was significantly increased after coronary artery bypass surgery in about 71.6% segments. In the group that myocardial perfusion was improved, the peak systolic longitudinal strain three months after bypass surgery was significantly higher than that before operation [(-15.78+/-5.91)% vs (-10.45+/-8.31)%, P<0.05]. However, the parameters did not change in the group without myocardial perfusion improvement [(-10.33+/-6.53)% vs (-9.41+/-6.09)%, P>0.05]. It was concluded that whether or not the improvement of myocardial perfusion can mirror the recovery trend of regional systolic function, two-dimensional strain echocardiography can observe dynamic change of regional systolic function. The combination of myocardial perfusion with two-dimensional strain echocardiography can more accurately assess the curative effectiveness of coronary artery bypass surgery.
Journal of Huazhong University of Science and Technology 10/2009; 29(5):664-8. · 0.38 Impact Factor
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ABSTRACT: A simple hydrothermal method has been developed for the one-step synthesis of copper-core/carbon-sheath nanocables in solution. The obtained nanostructures were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and high-resolution TEM (HRTEM), Raman, and UV-vis spectrum analysis. These copper@carbon nanocables formed through the hydrothermal reduction/carbonization in the presence of surfactant cetyltrimethylammonium bromide (CTAB) acting as the structure-directing agent by hydrothermal treatment. HRTEM and selected-area electron diffraction (SAED) indicate that the resulted Cu nanowires had the preferred [110] growth direction. The influence of the reaction temperature, reaction time, and pH on the final products was investigated in detail. The possible formation mechanism for copper-core/carbon-sheath nanocables was also proposed. Amorphous carbon nanotubes can be obtained by etching the copper core in the nanocables.
The Journal of Physical Chemistry B 07/2006; 110(24):11711-6. · 3.70 Impact Factor
