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991.
Gabriela R. Stadler Dr. Takuya F. Segawa Matthias Bütikofer Dr. Venita Decker Dr. Sandra Loss Dr. Barbara Czarniecki Dr. Felix Torres Prof. Roland Riek 《Angewandte Chemie (International ed. in English)》2023,62(40):e202308692
Fragment-based drug design is a well-established strategy for rational drug design, with nuclear magnetic resonance (NMR) on high-field spectrometers as the method of reference for screening and hit validation. However, high-field NMR spectrometers are not only expensive, but require specialized maintenance, dedicated space, and depend on liquid helium cooling which became critical over the recurring global helium shortages. We propose an alternative to high-field NMR screening by applying the recently developed approach of fragment screening by photoinduced hyperpolarized NMR on a cryogen-free 80 MHz benchtop NMR spectrometer yielding signal enhancements of up to three orders in magnitude. It is demonstrated that it is possible to discover new hits and kick-off drug design using a benchtop NMR spectrometer at low micromolar concentrations of both protein and ligand. The approach presented performs at higher speed than state-of-the-art high-field NMR approaches while exhibiting a limit of detection in the nanomolar range. Photoinduced hyperpolarization is known to be inexpensive and simple to be implemented, which aligns greatly with the philosophy of benchtop NMR spectrometers. These findings open the way for the use of benchtop NMR in near-physiological conditions for drug design and further life science applications. 相似文献
992.
Feng Huang Dr. Xiao-Chun Fan Ying-Chun Cheng Hao Wu Xin Xiong Jia Yu Prof. Kai Wang Prof. Xiao-Hong Zhang 《Angewandte Chemie (International ed. in English)》2023,62(32):e202306413
Building blocks and heteroatom alignments are two determining factors in designing multiple resonance (MR)-type thermally activated delayed fluorescence (TADF) emitters. Carbazole-fused MR emitters, represented by CzBN derivatives, and the heteroatom alignments of ν-DABNA are two star series of MR-TADF emitters that show impressive performances from the aspects of building blocks and heteroatom alignments, respectively. Herein, a novel CzBN analog, Π-CzBN, featuring ν-DABNA heteroatom alignment is developed via facile one-shot lithium-free borylation. Π-CzBN exhibits superior photophysical properties with a photoluminescence quantum yield close to 100 % and narrowband sky blue emission with a full width at half maximum (FWHM) of 16 nm/85 meV. It also gives efficient TADF properties with a small singlet-triplet energy offset of 40 meV and a fast reverse intersystem crossing rate of 2.9×105 s−1. The optimized OLED using Π-CzBN as the emitter achieves an exceptional external quantum efficiency of 39.3 % with a low efficiency roll-off of 20 % at 1000 cd m−2 and a narrowband emission at 495 nm with FWHM of 21 nm/106 meV, making it one of the best reported devices based on MR emitters with comprehensive performance. 相似文献
993.
Erandi Peiris Sébastien Hanauer Tien Le Jiale Wang Taha Salavati-fard Paul Brasseur Eric V. Formo Bin Wang Pedro H. C. Camargo 《Angewandte Chemie (International ed. in English)》2023,62(4):e202216398
Plasmonic catalysis enables the use of light to accelerate molecular transformations. Its application to the control reaction selectivity is highly attractive but remains challenging. Here, we have found that the plasmonic properties in AgPd nanoparticles allowed different reaction pathways for tunable product formation under visible-light irradiation. By employing the hydrogenation of phenylacetylene as a model transformation, we demonstrate that visible-light irradiation can be employed to steer the reaction pathway from hydrogenation to homocoupling. Our data showed that the decrease in the concentration of H species at the surface due to plasmon-enhanced H2 desorption led to the control in selectivity. These results provide important insights into the understanding of reaction selectivity with light, paving the way for the application of plasmonic catalysis to the synthesis of 1,3-diynes, and bringing the vision of light-driven transformations with target selectivity one step closer to reality. 相似文献
994.
Dr. Ribal Jabbour Dr. Christopher W. Ashling Thomas C. Robinson Dr. Arafat Hossain Khan Dr. Dorothea Wisser Dr. Pierrick Berruyer Dr. Ashta C. Ghosh Alisa Ranscht Dr. David A. Keen Prof. Dr. Eike Brunner Dr. Jérôme Canivet Prof. Dr. Thomas D. Bennett Dr. Caroline Mellot-Draznieks Dr. Anne Lesage Dr. Florian M. Wisser 《Angewandte Chemie (International ed. in English)》2023,62(44):e202310878
995.
Kaiyuan Zhang Dr. Xingdong Wang Yufei Chang Yuliang Wu Dr. Shumeng Wang Prof. Lixiang Wang 《Angewandte Chemie (International ed. in English)》2023,62(47):e202313084
The hyperfluorescence has drawn great attention in achieving efficient narrowband emitting devices based on multiple resonance thermally activated delayed fluorescence (MR-TADF) emitters. However, achieving efficient solution-processed pure blue hyperfluorescence devices is still a challenge, due to the unbalanced charge transport and serious exciton quenching caused by that the holes are easily trapped on the high-lying HOMO (the highest occupied molecular orbital) level of traditional diphenylamine-decorated emitters. Here, we developed two narrowband blue organoboron emitters with low-lying HOMO levels by decorating the MR-TADF core with weakly electron-donating carbazoles, which could suppress the hole trapping effect by reducing the hole traps between host and MR-TADF emitter from deep (0.40 eV) to shallow (0.14/0.20 eV) ones for facilitating hole transport and exciton formation, as well as avoiding exciton quenching. And the large dihedral angle between the carbazole and MR-TADF core makes the carbazole act as a steric hindrance to inhibit molecular aggregation. Accordingly, the optimized solution-processed pure blue hyperfluorescence devices simultaneously realize record external quantum efficiency of 29.2 %, narrowband emission with a full-width at half-maximum of 16.6 nm, and pure blue color with CIE coordinates of (0.139, 0.189), which is the best result for the solution-processed organic light-emitting diodes based on MR-TADF emitters. 相似文献
996.
Dr. Lingling Zhang Yilin Chen Dr. Jiapeng Zheng Dr. George R. Lewis Xinyue Xia Prof. Emilie Ringe Prof. Wei Zhang Prof. Jianfang Wang 《Angewandte Chemie (International ed. in English)》2023,62(52):e202312615
Chiral plasmonic nanoparticles have attracted much attention because of their strong chiroptical responses and broad scientific applications. However, the types of chiral plasmonic nanoparticles have remained limited. Herein we report on a new type of chiral nanoparticle, chiral Au nanorod (NR) with five-fold rotational symmetry, which is synthesized using chiral molecules. Three different types of Au seeds (Au elongated nanodecahedrons, nanodecahedrons, and nanobipyramids) are used to study the growth behaviors. Different synthesis parameters, including the chiral molecules, surfactant, reductant, seeds, and Au precursor, are systematically varied to optimize the chiroptical responses of the chiral Au NRs. The chiral scattering measurements on the individual chiral Au NRs and their dimers are performed. Intriguingly, the chiroptical signals of the individual chiral Au NRs and their end-to-end dimers are similar, while those of the side-by-side dimers are largely reduced. Theoretical calculations and numerical simulations reveal that the different chiroptical responses of the chiral NR dimers are originated from the coupling effect between the plasmon resonance modes. Our study enriches chiral plasmonic nanoparticles and provides valuable insight for the design of plasmonic nanostructures with desired chiroptical properties. 相似文献
997.
Resonant capture describes the behavior of a weakly coupled multi-degree-of-freedom system when two or more of its uncoupled frequencies become locked in resonance. Flow on the region of phase space near the resonance (the resonance manifold) involves a region bounded by a separatrix in the uncoupled (=0) system. Capture corresponds to motions which appear to cross into the interior of the separated region for >0. We offer two approximate methods for estimating which initial conditions lead to capture: an energy method and a perturbation method based on invariant manifold theory. These methods are applied to a model problem involving the spinup of an unbalanced rotor attached to an elastic support. 相似文献
998.
中性红共振光散射法测定脱氧核糖核酸 总被引:10,自引:0,他引:10
本文基于脱氧核糖核酸 (DNA)对有机染料中性红的共振光散射的增强效应 ,拟订了一种测定DNA的共振光散射法。在pH 5 0~ 7 0范围内 ,有机染料中性红在DNA分子表面进行长距组装导致共振光散射增强。在 335 0nm处的共振光谱散射增强程度与DNA浓度呈线性关系 ,其线性范围为 0~ 6 0 0ng·mL-1,检出限可达 12 8ng·mL-1。该方法简便、快速 ,具有较高的灵敏度和准确度。将该方法用于混合样品中DNA的测定 ,结果令人满意。 相似文献
999.
超临界流体分离与NMR联用技术及其应用 总被引:10,自引:0,他引:10
本文重点描述了SFC-NMR和SFE-NMR联用装置的特点及其探头设计,举例说明了它们的几种典型应用,分析比较了超临界流体分离和NMR联用系统与HPLC-NMR联用系统的特性,并讨论了超临界流体分离与NMR联用技术的发展前景。 相似文献
1000.
波谱分析技术在宝石鉴定中的应用评述 总被引:2,自引:0,他引:2
波谱分析技术已被成功地应用于宝石学研究和宝石鉴定领域,如红外光谱技术,拉曼光谱技术和顺磁共振技术均可以有效,快速,无损和准确地鉴定宝石的类别,如天然宝石,人工合成宝石和优化处理宝石。 相似文献