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361.
362.
Sonia E. Létant David F. Plant Thomas S. Wilson Cynthia T. Alviso Mark S.D. Read Robert S. Maxwell 《Polymer Degradation and Stability》2011,96(11):2019-2028
We report on the application of Density Functional Theory (DFT) methodologies to investigate the degradation of polymer materials and provide new insights into the effects of degradation on molecular geometry. The temperature- and radiation-assisted degradation of a cross-linked ethylene–vinyl acetate–vinyl alcohol (EVA-OH) elastomer was studied both experimentally and theoretically, in order to correlate observable parameters with theoretically calculated electronic properties. Experiments showed ‘yellowing’ of the material, outgassing of acetic acid, and attenuated IR deformation modes upon exposure to increased levels of gamma radiation or increased temperatures, consistent with the de-acetylation model in which acetic acid is abstracted from the vinyl acetate group via a molecular rearrangement involving the displacement of a hydrogen atom from the ethylene backbone toward the acetyl group, and the propagation of the mechanism to adjacent vinyl acetate groups, forming polyenes in the polymer backbone. DFT modeling predicted the molecular structures of the cross-linked EVA-OH polymer for various degrees of de-acetylation, with corresponding IR and UV–visible absorption spectra. Theoretical attenuated IR deformation modes matched experimental observations, and the theoretical absorption spectrum of polyenes with 5 double bonds matched the optical absorption data, shedding light onto the final chemical structure of the polymer fragment. In addition, DFT unveiled precise and local effects of de-acetylation on the geometry of both the remaining polymer chain and cross-linker, which could only be detected as methylene deformation mode reflectance changes by IR spectroscopy. 相似文献
363.
The acoustical cues for sound location are generated by spatial- and frequency-dependent filtering of propagating sound waves by the head and external ears. Although rats have been a common model system for anatomy, physiology, and psychophysics of localization, there have been few studies of the acoustical cues available to rats. Here, directional transfer functions (DTFs), the directional components of the head-related transfer functions, were measured in six adult rats. The cues to location were computed from the DTFs. In the frontal hemisphere, spectral notches were present for frequencies from approximately 16 to 30 kHz; in general, the frequency corresponding to the notch increased with increases in source elevation and in azimuth toward the ipsilateral ear. The maximum high-frequency envelope-based interaural time differences (ITDs) were 130 mus, whereas low-frequency (<3.5 kHz) fine-structure ITDs were 160 mus; both types of ITDs were larger than predicted from spherical head models. Interaural level differences (ILDs) strongly depended on location and frequency. Maximum ILDs were <10 dB for frequencies <8 kHz and were as large as 20-40 dB for frequencies >20 kHz. Removal of the pinna eliminated the spectral notches, reduced the acoustic gain and ILDs, altered the acoustical axis, and reduced the ITDs. 相似文献
364.
R. S. Hughesdon G. J. Robertson J. Read G. Tammann K. L. Dreyer M. Bodenstein H. Mainz J. Corbière W. Krings und H. Salmang 《Fresenius' Journal of Analytical Chemistry》1931,84(6-7):248-253
Ohne Zusammenfassung 相似文献
365.
366.
Julian Kund Jan-Hendrik Kruse Andreas Gruber Dr. Ivan Trentin Marcel Langer Dr. Clarissa Read Dr. Gregor Neusser Dominik Blaimer Dr. Ulrich Rupp Prof. Dr. Carsten Streb Prof. Dr. Kerstin Leopold Prof. Dr. Felix H. Schacher Prof. Dr. Christine Kranz 《Angewandte Chemie (International ed. in English)》2023,62(22):e202217196
Heterogeneous light-driven catalysis is a cornerstone of sustainable energy conversion. Most catalytic studies focus on bulk analyses of the hydrogen and oxygen evolved, which impede the correlation of matrix heterogeneities, molecular features, and bulk reactivity. Here, we report studies of a heterogenized catalyst/photosensitizer system using a polyoxometalate water oxidation catalyst and a model, molecular photosensitizer that were co-immobilized within a nanoporous block copolymer membrane. Via operando scanning electrochemical microscopy (SECM), light-induced oxygen evolution was determined using sodium peroxodisulfate (Na2S2O8) as sacrificial electron acceptor. Ex situ element analyses provided spatially resolved information on the local concentration and distribution of the molecular components. Infrared attenuated total reflection (IR-ATR) studies of the modified membranes showed no degradation of the water oxidation catalyst under the reported light-driven conditions. 相似文献
367.
Jesus Guillen Campos Friedrich Stricker Kyle D. Clark Minwook Park Sophia J. Bailey Alexa S. Kuenstler Ryan C. Hayward Javier Read de Alaniz 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(1):e202214339
Aligned liquid crystal polymers are materials of interest for electronic, optic, biological and soft robotic applications. The manufacturing and processing of these materials have been widely explored with mechanical alignment establishing itself as a preferred method due to its ease of use and widespread applicability. However, the fundamental chemistry behind the required two-step polymerization for mechanical alignment has limitations in both fabrication and substrate compatibility. In this work we introduce a new protection-deprotection approach utilizing a two-stage Diels–Alder cyclopentadiene-maleimide step-growth polymerization to enable mild yet efficient, fast, controlled, reproducible and user-friendly polymerizations, broadening the scope of liquid crystal systems. Thorough characterization of the films by DSC, DMA, POM and WAXD show the successful synthesis of a uniaxially aligned liquid crystal network with thermomechanical actuation abilities. 相似文献