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11.
An Investigation of Photo‐ and Pressure‐Induced Effects in a Pair of Isostructural Two‐Dimensional Spin‐Crossover Framework Materials 下载免费PDF全文
Dr. Natasha F. Sciortino Dr. Suzanne M. Neville Dr. Cédric Desplanches Dr. Jean‐François Létard Dr. Victor Martinez Prof. José Antonio Real Dr. Boujemaa Moubaraki Prof. Keith S. Murray Prof. Cameron J. Kepert 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(24):7448-7457
Two new isostructural iron(II) spin‐crossover (SCO) framework (SCOF) materials of the type [Fe(dpms)2(NCX)2] (dpms=4,4′‐dipyridylmethyl sulfide; X=S ( SCOF‐6(S) ), X=Se ( SCOF‐6(Se) )) have been synthesized. The 2D framework materials consist of undulating and interpenetrated rhomboid (4,4) nets. SCOF‐6(S) displays an incomplete SCO transition with only approximately 30 % conversion of high‐spin (HS) to low‐spin iron(II) sites over the temperature range 300–4 K (T1/2=75 K). In contrast, the NCSe? analogue, SCOF‐6(Se) , displays a complete SCO transition (T1/2=135 K). Photomagnetic characterizations reveal quantitative light‐ induced excited spin‐state trapping (LIESST) of metastable HS iron(II) sites at 10 K. The temperature at which the photoinduced stored information is erased is 58 and 50 K for SCOF‐6(S) and SCOF‐6(Se) , respectively. Variable‐pressure magnetic measurements were performed on SCOF‐6(S) , revealing that with increasing pressure both the T1/2 value and the extent of spin conversion are increased; with pressures exceeding 5.2 kbar a complete thermal transition is achieved. This study confirms that kinetic trapping effects are responsible for hindering a complete thermally induced spin transition in SCOF‐6(S) at ambient pressure due to an interplay between close T1/2 and T(LIESST) values. 相似文献
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Hoo Christopher M. Starostin Natasha West Paul Mecartney Martha L. 《Journal of nanoparticle research》2008,10(1):89-96
This paper compares the accuracy of conventional dynamic light scattering (DLS) and atomic force microscopy (AFM) for characterizing size distributions of polystyrene nanoparticles in the size range of 20–100 nm. Average DLS values for monosize dispersed particles are slightly higher than the nominal values whereas AFM values were slightly lower than nominal values. Bimodal distributions were easily identified with AFM, but DLS results were skewed toward larger particles. AFM characterization of nanoparticles using automated analysis software provides an accurate and rapid analysis for nanoparticle characterization and has advantages over DLS for non-monodispersed solutions. 相似文献
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Pajewski R Ferdani R Pajewska J Djedovic N Schlesinger PH Gokel GW 《Organic & biomolecular chemistry》2005,3(4):619-625
Heptapeptides having dioctadecyl, N-terminal hydrocarbon chains insert in phospholipid bilayer membranes and form pores through which at least chloride ions pass. Although amphiphilic, these compounds do not typically form vesicles themselves. They insert in the bilayers of phospholipid vesicles and mediate the release of carboxyfluorescein. Hill analysis indicates that at least two molecules of the amphiphile are involved in pore formation. In CD2Cl2, dimer formation is detected by NMR chemical shift changes. The anion release activity of individual anion transporters is increased by linking them covalently at the C-terminus or, even more, by linking them at the N-terminus. Evidence is presented that either linked molecule releases chloride from liposomes more effectively and rapidly than the individual transporter molecule at a comparable concentration. 相似文献
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Smits R Warner N McQueen JM Cutler A 《The Journal of the Acoustical Society of America》2003,113(1):563-574
We present the results of a large-scale study on speech perception, assessing the number and type of perceptual hypotheses which listeners entertain about possible phoneme sequences in their language. Dutch listeners were asked to identify gated fragments of all 1179 diphones of Dutch, providing a total of 488,520 phoneme categorizations. The results manifest orderly uptake of acoustic information in the signal. Differences across phonemes in the rate at which fully correct recognition was achieved arose as a result of whether or not potential confusions could occur with other phonemes of the language (long with short vowels, affricates with their initial components, etc.). These data can be used to improve models of how acoustic-phonetic information is mapped onto the mental lexicon during speech comprehension. 相似文献
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Schlesinger PH Djedovic NK Ferdani R Pajewska J Pajewski R Gokel GW 《Chemical communications (Cambridge, England)》2003,(3):308-309
Two membrane-anchored heptapeptides have been prepared and their pore-formation behavior in phospholipid bilayer membranes has been found to differ profoundly as a result only of alkyl chain length. 相似文献
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Fornberg Bengt; Flyer Natasha; Hovde Susan; Piret Cecile 《IMA Journal of Numerical Analysis》2008,28(1):121-142
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Ghizlane Choukrani Jimena Álvarez Freile Natasha Ustyanovska Avtenyuk Wei Wan Kerstin Zimmermann Edwin Bremer Lars Dähne 《Particle & Particle Systems Characterization》2021,38(7):2100012
Nanoparticles may limit off-tumor/on-target ubiquitous activation of signaling by protein-based drugs. However, many challenges still exist in the design of a nanoparticle for protein delivery. In this study, conditions to establish vaterite nanoparticles as a pH-sensitive drug delivery system (DDS) for encapsulated protein drugs are comprehensively evaluated. Low coprecipitation pH of vaterite and protein prevents protein denaturation and yields high loading efficiency. Unprotected vaterite recrystallizes in aqueous solutions within 3 h to calcite and releases the loaded protein completely, but surface-modified particles with carboxyl groups containing polymers prove stable for more than 5 months. Notably, modification of vaterite with sulfonated polymers increases the loading of cationic proteins by a multiple. A system is developed for vaterite exposure to (pH) conditions under body-like-flow rates, with the dissolution of vaterite and simultaneous release of active proteins at tumor microenvironmental pH reaching up to 80% and only 20% at physiological pH within 2 h. Importantly, the immunomodulatory protein tumor necrosis factor preserves its native structure and fully retains functional activity in vitro after release from the particles. In conclusion, the studies described here provide a framework for the development of vaterite-based DDS as a carrier for bioactive protein-based therapeutics. 相似文献
20.
Kim J Middlemiss DS Chernova NA Zhu BY Masquelier C Grey CP 《Journal of the American Chemical Society》2010,132(47):16825-16840
Iron phosphates (FePO(4)) are among the most promising candidate materials for advanced Li-ion battery cathodes. This work reports upon a combined nuclear magnetic resonance (NMR) experimental and periodic density functional theory (DFT) computational study of the environments and electronic structures occurring in a range of paramagnetic Fe(III) phosphates comprising FePO(4) (heterosite), monoclinic Li(3)Fe(2)(PO(4))(3) (anti-NASICON A type), rhombohedral Li(3)Fe(2)(PO(4))(3) (NASICON B type), LiFeP(2)O(7), orthorhombic FePO(4)·2H(2)O (strengite), monoclinic FePO(4)·2H(2)O (phosphosiderite), and the dehydrated forms of the latter two phases. Many of these materials serve as model compounds relevant to battery chemistry. The (31)P spin-echo mapping and (7)Li magic angle spinning NMR techniques yield the hyperfine shifts of the species of interest, complemented by periodic hybrid functional DFT calculations of the respective hyperfine and quadrupolar tensors. A Curie-Weiss-based magnetic model scaling the DFT-calculated hyperfine parameters from the ferromagnetic into the experimentally relevant paramagnetic state is derived and applied, providing quantitative finite temperature values for each phase. The sensitivity of the hyperfine parameters to the composition of the DFT exchange functional is characterized by the application of hybrid Hamiltonians containing admixtures 0%, 20%, and 35% of Fock exchange. Good agreement between experimental and calculated values is obtained, provided that the residual magnetic couplings persisting in the paramagnetic state are included. The potential applications of a similar combined experimental and theoretical NMR approach to a wider range of cathode materials are discussed. 相似文献