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941.
942.
943.
944.
945.
Pas SJ Dargusch MS MacFarlane DR 《Physical chemistry chemical physics : PCCP》2011,13(25):12033-12040
The properties of ionic liquids give rise to applications in diverse technology areas including mechanical engineering, mining, aerospace and defence. The arbitrary physical property that defines an ionic liquid is a melting point below 100 °C, and as such, an understanding of crystallisation phenomena is extremely important. This is the first report dealing with the mechanism of crystallisation in ionic liquids. Assuming crystallisation of the ionic liquids is a thermal or mass diffusion-controlled process, the values of the isothermal Avrami exponent obtained from three different ionic liquids with three different anions and cations all indicate that growth occurs with a decreasing nucleation rate (n=1.8-2.2). For one of the ionic liquids it was possible to avoid crystallisation by fast cooling and then observe a devitrification upon heating through the glass transition. The isothermal Avrami exponent of devitrification suggested growth with an increasing nucleating rate (n=4.1), compared to a decreasing nucleation rate when crystallisation occurs on cooling from the melt (n=2.0). Two non-isothermal methods were employed to determine the Avrami exponent of devitrification. Both non-isothermal Avrami exponents were in agreement with the isothermal case (n=4.0-4.15). The applicability of JMAK theory suggests that the nucleation event in the ionic liquids selected is a random stochastic process in the volume of the material. Agreement between the isothermal and non-isothermal techniques for determining the Avrami exponent of devitrification suggests that the pre-exponential factor and the activation energy are independent of thermal history. The heating rate dependence of the glass transition enabled the calculation of the fragility index, which suggests that the ionic liquid is a "strong" glass former. This suggests that the temperature dependence of the rate constant could be close to Arrhenius, as assumed by JMAK theory. More generally, therefore, it can be concluded that there is nothing unusual about the crystallisation mechanism of the ionic liquids studied here. 相似文献
946.
Using results from the dielectric theory of polar solids and liquids, we calculate the mesoscopic, spatially-varying dielectric constant at points in and around a protein by combining a generalization Kirkwood-Fr?hlich theory along with short all-atom molecular dynamics simulations of equilibrium protein fluctuations. The resulting dielectric permittivity tensor is found to exhibit significant heterogeneity and anisotropy in the protein interior. Around the surface of the protein it may exceed the dielectric constant of bulk water, especially near the mobile side chains of polar residues, such as K, N, Q, and E. The anisotropic character of the protein dielectric selectively modulates the attractions and repulsions between charged groups in close proximity. 相似文献
947.
Zhong Q Bhattacharya S Kotsopoulos S Olson J Taly V Griffiths AD Link DR Larson JW 《Lab on a chip》2011,11(13):2167-2174
Quantitative polymerase chain reactions (qPCR) based on real-time PCR constitute a powerful and sensitive method for the analysis of nucleic acids. However, in qPCR, the ability to multiplex targets using differently colored fluorescent probes is typically limited to 4-fold by the spectral overlap of the fluorophores. Furthermore, multiplexing qPCR assays requires expensive instrumentation and most often lengthy assay development cycles. Digital PCR (dPCR), which is based on the amplification of single target DNA molecules in many separate reactions, is an attractive alternative to qPCR. Here we report a novel and easy method for multiplexing dPCR in picolitre droplets within emulsions-generated and read out in microfluidic devices-that takes advantage of both the very high numbers of reactions possible within emulsions (>10(6)) as well as the high likelihood that the amplification of only a single target DNA molecule will initiate within each droplet. By varying the concentration of different fluorogenic probes of the same color, it is possible to identify the different probes on the basis of fluorescence intensity. Adding multiple colors increases the number of possible reactions geometrically, rather than linearly as with qPCR. Accurate and precise copy numbers of up to sixteen per cell were measured using a model system. A 5-plex assay for spinal muscular atrophy was demonstrated with just two fluorophores to simultaneously measure the copy number of two genes (SMN1 and SMN2) and to genotype a single nucleotide polymorphism (c.815A>G, SMN1). Results of a pilot study with SMA patients are presented. 相似文献
948.
Characterization of heterogeneous solids via wave methods in computational microelasticity 总被引:1,自引:0,他引:1
Real solids are inherently heterogeneous bodies. While the resolution at which they are observed may be disparate from one material to the next, heterogeneities heavily affect the dynamic behavior of all microstructured solids. This work introduces a wave propagation simulation methodology, based on Mindlin's microelastic continuum theory, as a tool to dynamically characterize microstructured solids in a way that naturally accounts for their inherent heterogeneities. Wave motion represents a natural benchmark problem to appreciate the full benefits of the microelastic theory, as in high-frequency dynamic regimes do microstructural effects unequivocally elucidate themselves. Through a finite-element implementation of the microelastic continuum and the interpretation of the resulting computational multiscale wavefields, one can estimate the effect of microstructures upon the wave propagation modes, phase and group velocities. By accounting for microstructures without explicitly modeling them, the method allows reducing the computational time with respect to classical methods based on a direct numerical simulation of the heterogeneities. The numerical method put forth in this research implements the microelastic theory through a finite-element scheme with enriched super-elements featuring microstructural degrees of freedom, and implementing constitutive laws obtained by homogenizing the microstructure characteristics over material meso-domains. It is possible to envision the use of this modeling methodology in support of diverse applications, ranging from structural health monitoring in composite materials to the simulation of biological and geomaterials. From an intellectual point of view, this work offers a mathematical explanation of some of the discrepancies often observed between one-scale models and physical experiments by targeting the area of wave propagation, one area where these discrepancies are most pronounced. 相似文献
949.
Stacey E. Rudd Jessica K. Van Zuylekom Anna Raicevic Lesley A. Pearce Carleen Cullinane Charlotte C. Williams Timothy E. Adams Rodney J. Hicks Paul S. Donnelly 《Chemical science》2021,12(26):9004
Identification of tumors which over-express Epidermal Growth Factor Receptor (EGFR) is important in selecting patients for anti-EGFR therapies. Enzymatic bioconjugation was used to introduce positron-emitting radionuclides (89Zr, 64Cu) into an anti-EGFR antibody fragment for Positron Emission Tomography (PET) imaging the same day as injection. A monovalent antibody fragment with high affinity for EGFR was engineered to include a sequence that is recognized by the transpeptidase sortase A. Two different metal chelators, one for 89ZrIV and one for 64CuII, were modified with a N-terminal glycine to enable them to act as substrates in sortase A mediated bioconjugation to the antibody fragment. Both fragments provided high-quality PET images of EGFR positive tumors in a mouse model at 3 hours post-injection, a significant advantage when compared to radiolabeled full antibodies that require several days between injection of the tracer and imaging. The use of enzymatic bioconjugation gives reproducible homogeneous products with the metal complexes selectively installed on the C-terminus of the antibody potentially simplifying regulatory approval.Enzymatic bioconjugation to introduce positron-emitting radionuclides (89Zr, 64Cu) into an anti-EGFR antibody fragment allows same day imaging with positron emission tomography. 相似文献
950.
Steven van Terwingen Daniel Brüx Ruimin Wang Ulli Englert 《Molecules (Basel, Switzerland)》2021,26(13)
In the hydrochloride of a pyrazolyl-substituted acetylacetone, the chloride anion is hydrogen-bonded to the protonated pyrazolyl moiety. Equimolar co-crystallization with tetrafluorodiiodobenzene (TFDIB) leads to a supramolecular aggregate in which TFDIB is situated on a crystallographic center of inversion. The iodine atom in the asymmetric unit acts as halogen bond donor, and the chloride acceptor approaches the -hole of this TFDIB iodine subtending an almost linear halogen bond, with Cl···I = Å and Cl···I–C = 179.32(6)°. This contact is roughly orthogonal to the N–H···Cl hydrogen bond. An analysis of the electron density according to Bader’s Quantum Theory of Atoms in Molecules confirms bond critical points (bcps) for both short contacts, with = 0.129 for the halogen and e for the hydrogen bond. Our halogen-bonded adduct represents the prototype for a future class of co-crystals with tunable electron density distribution about the -hole contact. 相似文献