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341.
Swanson JM Maupin CM Chen H Petersen MK Xu J Wu Y Voth GA 《The journal of physical chemistry. B》2007,111(17):4300-4314
The excess proton in aqueous media plays a pivotal role in many fundamental chemical (e.g., acid-base chemistry) and biological (e.g., bioenergetics and enzyme catalysis) processes. Understanding the hydrated proton is, therefore, crucial for chemistry, biology, and materials sciences. Although well studied for over 200 years, excess proton solvation and transport remains to this day mysterious, surprising, and perhaps even misunderstood. In this feature article, various efforts to address this problem through computer modeling and simulation will be described. Applications of computer simulations to a number of important and interesting systems will be presented, highlighting the roles of charge delocalization and Grotthuss shuttling, a phenomenon unique in many ways to the excess proton in water. 相似文献
342.
Anderson AS Dattelbaum AM Montaño GA Price DN Schmidt JG Martinez JS Grace WK Grace KM Swanson BI 《Langmuir : the ACS journal of surfaces and colloids》2008,24(5):2240-2247
We report a general procedure to prepare functional organic thin films for biological assays on oxide surfaces. Silica surfaces were functionalized by self-assembly of an amine-terminated silane film using both vapor- and solution-phase deposition of 3'-aminopropylmethyldiethoxysilane (APMDES). We found that vapor-phase deposition of APMDES under reduced pressure produced the highest quality monolayer films with uniform surface coverage, as determined by atomic force microscopy (AFM), ellipsometry, and contact angle measurements. The amine-terminated films were chemically modified with a mixture of carboxylic acid-terminated poly(ethylene glycol) (PEG) chains of varying functionality. A fraction of the PEG chains (0.1-10 mol %) terminated in biotin, which produced a surface with an affinity toward streptavidin. When used in pseudo-sandwich assays on waveguide platforms for the detection of Bacillus anthracis protective antigen (PA), these functional PEG surfaces significantly reduced nonspecific binding to the waveguide surface while allowing for highly specific binding. Detection of PA was used to validate these films for sensing applications in both buffer and complex media. Ultimately, these results represent a step toward the realization of a robust, reusable, and autonomous biosensor. 相似文献
343.
We have measured the light scattering intensity and homogeneous ice nucleation temperatures from water droplets containing 0-33 wt % ammonium sulfate. In these laboratory experiments, we used a free-fall freezing tube technique to determine the fraction of frozen droplets at a particular droplet temperature by measuring the depolarized light scattering intensity from the droplets in free-fall. Previously reported freezing temperatures for solution concentrations greater than 5 wt % display a larger spread than can be accounted for by the reported experimental errors. We find freezing temperatures in good agreement with the lowest temperature freezing results reported by previous experiments. Our ammonium sulfate freezing temperature data set with water activity less than 0.98 is consistent with a curve that deviates in activity shift by about 5% from the best-fit ice nucleation temperature versus water activity curve found by Koop et al. in 2000, but the significance of this deviation will only be known with further high-precision ice nucleation temperature measurements for other aqueous solutions. 相似文献
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A range of hydrophobically-modified water-soluble polymers, based upon acrylic acid and methacrylic acid as hydrophilic components, has been studied using various luminescence techniques. Time-resolved anisotropy measurements, on fluorescently labelled macromolecules, have been used to quantify the extent to which the conformational behaviour of a given polyelectrolyte affects its segmental mobility, and to gauge how such behaviour can be controlled by hydrophobic modification. Room-temperature stabilized phosphorescence from the labels and/or occluded guests and energy transfer experiments have been used to investigate the nature of the hydrophobic domains formed in these polymers. Hydrophobic modification of polyelectrolytes can be used to enhance the scope of water-soluble macromolecules as solubilizing media for photochemical and spectroscopic applications. 相似文献