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91.
92.
Emmanuel Urandu Mapesa Ludwig Popp Wycliffe Kiprop Kipnusu Martin Tress Friedrich Kremer 《Soft Materials》2014,12(4):S22-S30
Broadband Dielectric Spectroscopy (BDS) is used to probe the molecular dynamics of Type A polymer, poly(cis-1,4-isoprene), when confined in the 1-dimensional (1D) exploring space of thin layers and the 2-dimensional (2D) constraining geometry of unidirectional anodic aluminum oxide (AAO) nanopores. For both cases, it was observed that the structural relaxation remains bulk-like in its mean relaxation rate, although the distribution of its relaxation times is broadened in 2D confinement. Furthermore, the fluctuation of the end-to-end vector is interrupted, with the 1D case being relatively less pronounced. By this clear-cut comparison, it is demonstrated that the effects of confinement on molecular dynamics depend, inter alia, on the dimensionality of the restricting space. 相似文献
93.
94.
Jinxiong Lin Dr. Friedrich Wossidlo. Dr. Nathan T. Coles Manuela Weber Dr. Simon Steinhauer Priv.-Doz. Dr. Tobias Böttcher Prof. Dr. Christian Müller 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(7):e202104135
A phosphinine-borane adduct of a Me3Si-functionalized phosphinine and the Lewis acid B(C6F5)3 has been synthesized and characterized crystallographically for the first time. The reaction strongly depends on the nature of the substituents in the α-position of the phosphorus heterocycle. In contrast, the reaction of B2H6 with various substituted phosphinines leads to an equilibrium between the starting materials and the phosphinine–borane adducts that is determined by the Lewis basicity of the phosphinine. The novel phosphinine borane adduct ( 6 -B(C6F5)3) shows rapid and facile insertion and [4+2] cycloaddition reactivity towards phenylacetylene. A hitherto unknown dihydro-1-phosphabarrelene is formed with styrene. The reaction with an ester provides a new, facile and selective route to 1-R-phosphininium salts. These salts then undergo a [4+2] cycloaddition in the presence of Me3Si−C≡CH and styrene to cleanly form unprecedented derivatives of 1-R-phosphabarrelenium salts. 相似文献
95.
Mingming Huang Dr. Jiefeng Hu Shasha Shi Dr. Alexandra Friedrich Johannes Krebs Prof. Dr. Stephen A. Westcott Prof. Dr. Udo Radius Prof. Dr. Todd B. Marder 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(24):e202200480
Defunctionalization of readily available feedstocks to provide alkenes for the synthesis of multifunctional molecules represents an extremely useful process in organic synthesis. Herein, we describe a transition metal-free, simple and efficient strategy to access alkyl 1,2-bis(boronate esters) via regio- and diastereoselective diboration of secondary and tertiary alkyl halides (Br, Cl, I), tosylates, and alcohols. Control experiments demonstrated that the key to this high reactivity and selectivity is the addition of a combination of potassium iodide and N,N-dimethylacetamide (DMA). The practicality and industrial potential of this transformation are demonstrated by its operational simplicity, wide functional group tolerance, and the late-stage modification of complex molecules. From a drug discovery perspective, this synthetic method offers control of the position of diversification and diastereoselectivity in complex ring scaffolds, which would be especially useful in a lead optimization program. 相似文献
96.
Thomas Wiesner Dr. Zhu Wu Dr. Jie Han Prof. Dr. Lei Ji Dr. Alexandra Friedrich Dr. Ivo Krummenacher Michael Moos Prof. Dr. Christoph Lambert Prof. Dr. Holger Braunschweig Benjamin Rudin Dr. Hilmar Reiss Olena Tverskoy Dr. Frank Rominger Prof. Dr. Andreas Dreuw Prof. Dr. Todd B. Marder Dr. Jan Freudenberg Prof. Dr. Uwe H. F. Bunz 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(69):e202201919
Tetraiodotetraazapentacene I4TAP , the last missing derivative in the series of halogenated silylated tetraazapentacenes, was synthesized via condensation chemistry from a TIPS-ethynylated diaminobenzothiadiazol in three steps. Single and double reduction furnished its air-stable monoanion and relatively air-stable dianion, both of which were characterized by crystallography. All three species are structurally and spectroscopically compared to non-halogenated TAP and Br4TAP . I4TAP is an n-channel material in thin-film transistors with average electron mobilities exceeding 1 cm2 (Vs)−1. 相似文献
97.
Kirill Arapov Kaarle Jaakkola Vladimir Ermolov Guy Bex Eric Rubingh Samiul Haque Henrik Sandberg Robert Abbel Gijsbertus de With Heiner Friedrich 《固体物理学:研究快报》2016,10(11):812-818
Despite the great promise of printed flexible electronics from 2D crystals, and especially graphene, few scalable applications have been reported so far that can be termed roll‐to‐roll compatible. Here we combine screen printed graphene with photonic annealing to realize radio‐frequency identification devices with a reading range of up to 4 meters. Most notably our approach leads to fatigue resistant devices showing less than 1% deterioration of electrical properties after 1000 bending cycles. The bending fatigue resistance demonstrated on a variety of technologically relevant plastic and paper substrates renders the material highly suitable for various printable wearable devices, where repeatable dynamic bending stress is expected during usage. All applied printing and post‐processing methods are compatible with roll‐to‐roll manufacturing and temperature sensitive flexible substrates providing a platform for the scalable manufacturing of mechanically stable and environmentally friendly graphene printed electronics.
98.
We determine the probability distribution of the first passage time for a class of non-Markovian processes. This class contains, amongst others, the well-known continuous time random walk (CTRW), which is able to account for many properties of anomalous diffusion processes. In particular, we obtain the mean first passage time for CTRW processes with truncated power-law transition time distribution. Our treatment is based on the fact that the solutions of the non-Markovian master equation can be obtained via an integral transform from a Markovian Langevin process. 相似文献
99.
Xing Chen Dr. Guoyun Meng Guanming Liao Dr. Florian Rauch Dr. Jiang He Dr. Alexandra Friedrich Prof. Dr. Todd B. Marder Dr. Nan Wang Dr. Pangkuan Chen Prof. Dr. Suning Wang Dr. Xiaodong Yin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(20):6274-6282
A series of 9-borafluorene derivatives, functionalised with electron-donating groups, have been prepared. Some of these 9-borafluorene compounds exhibit strong yellowish emission in solution and in the solid state with relatively high quantum yields (up to 73.6 % for FMesB-Cz as a neat film). The results suggest that the highly twisted donor groups suppress charge transfer, but the intrinsic photophysical properties of the 9-borafluorene systems remain. The new compounds showed enhanced stability towards the atmosphere, and exhibited excellent thermal stability, revealing their potential for application in materials science. Organic light-emitting diode (OLED) devices were fabricated with two of the highly emissive compounds, and they exhibited strong yellow-greenish electroluminescence, with a maximum luminance intensity of >22 000 cd m−2. These are the first two examples of 9-borafluorene derivatives being used as light-emitting materials in OLED devices, and they have enabled us to achieve a balance between maintaining their intrinsic properties while improving their stability. 相似文献
100.
Dr. Goutam Kumar Kole Dr. Julia Merz Dr. Anissa Amar Dr. Bruno Fontaine Dr. Abdou Boucekkine Dr. Jörn Nitsch Sabine Lorenzen Dr. Alexandra Friedrich Dr. Ivo Krummenacher Marta Košćak Prof. Dr. Holger Braunschweig Prof. Dr. Ivo Piantanida Prof. Dr. Jean-François Halet Prof. Dr. Klaus Müller-Buschbaum Prof. Dr. Todd B. Marder 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(8):2837-2853
Two N-methylpyridinium compounds and analogous N-protonated salts of 2- and 2,7-substituted 4-pyridyl-pyrene compounds were synthesised and their crystal structures, photophysical properties both in solution and in the solid state, electrochemical and spectroelectrochemical properties were studied. Upon methylation or protonation, the emission maxima are significantly bathochromically shifted compared to the neutral compounds, although the absorption maxima remain almost unchanged. As a result, the cationic compounds show very large apparent Stokes shifts of up to 7200 cm−1. The N-methylpyridinium compounds have a single reduction at ca. −1.5 V vs. Fc/Fc+ in MeCN. While the reduction process was reversible for the 2,7-disubstituted compound, it was irreversible for the mono-substituted one. Experimental findings are complemented by DFT and TD-DFT calculations. Furthermore, the N-methylpyridinium compounds show strong interactions with calf thymus (ct)-DNA, presumably by intercalation, which paves the way for further applications of these multi-functional compounds as potential DNA-bioactive agents. 相似文献