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How Does Solvation Affect the Binding of Hydrophilic Amino Saccharides to Cucurbit[7]uril with Exceptional Anomeric Selectivity? 下载免费PDF全文
Jianping Wang Yoonjung Jang Jayshree K. Khedkar Jin Young Koo Yonghwi Kim Chang Jun Lee Young Min Rhee Kimoon Kim 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(44):15791-15799
Cucurbit[7]uril (CB[7]) is known to bind strongly to hydrophilic amino saccharide guests with exceptional α‐anomer selectivities under aqueous conditions. Single‐crystal X‐ray crystallography and computational methods were used to elucidate the reason behind this interesting phenomenon. The crystal structures of protonated galactosamine (GalN) and glucosamine (GluN) complexes confirm the inclusion of α anomers inside CB[7] and disclose the details of the host–guest binding. Whereas computed gas‐phase structures agree with these crystal structures, gas‐phase binding free energies show preferences for the β‐anomer complexes over their α counterparts, in striking contrast to the experimental results under aqueous conditions. However, when the solvation effect is considered, the binding structures drastically change and the preference for the α anomers is recovered. The α anomers also tend to bind more tightly and leave less space in the CB[7] cavity toward inclusion of only one water molecule, whereas loosely bound β anomers leave more space toward accommodating two water molecules, with markedly different hydrogen‐bonding natures. Surprisingly, entropy seems to contribute significantly to both anomeric discrimination and binding. This suggests that of all the driving factors for the strong complexation of the hydrophilic amino saccharide guests, water mediation plays a crucial role in the anomer discrimination. 相似文献
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Nonlinear Dynamics - In this paper, the Riemann–Hilbert approach is systematically established for the Newell-type long-wave–short-wave equation. Firstly, we start spectral analysis... 相似文献
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Spectrum reservation strategy is an effective technology for conserving communication resources in Cognitive Radio Networks. In order to better adapt to changes of the system load, we present an adaptive control approach to determine the reservation ratio of the licensed spectrum for secondary users and propose a novel adaptive spectrum reservation strategy. We then establish a three-dimensional discrete time Markov Chain model to capture the stochastic behavior of users. By using a method similar to that of the matrix geometric solution, we obtain the steady-state probability distribution for the system model, and derive the formulas for some required performance measures of two types of users. Numerical experiments and simulation experiments indicate that the system performance is sensitive to system parameters like the adaptive control factor and the admission threshold. Finally, we construct a system cost function to balance different performance measures, and present an intelligent searching algorithm to optimize the system parameters with the global minimum system cost. 相似文献
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Jian-Ming Zhang Shang-Ru Zhai Bin Zhai Qing-Da An Ge Tian 《Journal of Sol-Gel Science and Technology》2012,64(2):347-357
Multifunctional nanomaterials with task-specific physicochemical properties, especially core?Cshell nanostructures with Fe3O4 core and NH2-functional shells (Fe3O4@SiO2?CNH2), have been extensively investigated as high-performance adsorbents, catalysts and catalyst supports; and in most cases the controllable sol?Cgel technique is the choice for fabrication of this kind of widely applied materials. Herein, we demonstrated that mono-dispersed and spherical Fe3O4@SiO2?CNH2 nanomaterials with magnetic response core, NH2-functional shell structure can be facilely prepared by co-condensation of TEOS with APTMS using a versatile sol?Cgel process. It was shown that the proper usage of APTMS and appropriate pre-hydrolysis time of TEOS were crucial and key steps for formation of highly uniform and desirable amino loading Fe3O4@SiO2?CNH2 materials. The TEOS pre-hydrolysis and the critical time (around 90?min) before the addition of APTMS prove to be vital for uniform structure evolution, while the appropriate concentration of APTMS (~2.28?mmol?L?1 in our system) leads to well-dispersed materials with relatively high loading of amino functionality. The as-prepared Fe3O4@SiO2?CNH2 magnetic nanoparticles prepared under optimum conditions possessing superparamagnetic behavior, uniform core?Cshell structure (~200?nm in diameter), relatively large BET surface area (~138?m2/g) and high incorporation of amino-functionality (~2.90?wt?%). 相似文献
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An optical multicarrier generator based on the improved re-circulating frequency shifter (RFS) to generate a larger number of frequency-locked carriers with high-quality has been studied. By eliminating the third-order crosstalk components, the output carrier's number and optical signal-to-noise-ratio (OSNR) of the generator have been improved significantly. In addition, the maximum output OSNR and optimal radio-frequency drive voltages in the cases of different desired carrier numbers have been obtained. Using the improved configuration, 130-tone with high-quality (tone-to-noise ratio ~20 dB and superior flatness <3 dB) where the drive voltage is only around 0.5Vπ can be achieved. The simulation results show a good agreement with the theoretical analysis. The multicarrier generator based on the improved RFS has the potential application in the terabit superchannel optical transmission. 相似文献
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