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991.
Fan Xiao Lin Lin Zhicong Chao Chen Shao Zhe Chen Zixiang Wei Jingxiong Lu Yishun Huang Lanqing Li Quan Liu Yongye Liang Leilei Tian 《Angewandte Chemie (International ed. in English)》2020,59(24):9702-9710
DNA nanotechnology plays an increasingly important role in the biomedical field; however, its application in the design of organic nanomaterials is underexplored. Herein, we report the use of DNA nanotechnology to transport a NIR‐II‐emitting nanofluorophore across the blood–brain barrier (BBB), facilitating non‐invasive imaging of brain tumors. Specifically, the DNA block copolymer, PS‐b‐DNA, is synthesized through a solid‐phase click reaction. We demonstrate that its self‐assembled structure shows exceptional cluster effects, among which BBB‐crossing is the most notable. Therefore, PS‐b‐DNA is utilized as an amphiphilic matrix to fabricate a NIR‐II nanofluorephore, which is applied in in vivo bioimaging. Accordingly, the NIR‐II fluorescence signal of the DNA‐based nanofluorophore localized at a glioblastoma is 3.8‐fold higher than the NIR‐II fluorescence signal of the PEG‐based counterpart. The notably increased imaging resolution will significantly benefit the further diagnosis and therapy of brain tumors. 相似文献
992.
993.
Wen‐Jun Yue Jun‐Zhao Xiao Shuai Zhang Liang Yin 《Angewandte Chemie (International ed. in English)》2020,59(18):7057-7062
1,2‐Bisphosphines have been identified as one class of important and powerful chiral ligands in asymmetric catalysis with transition metals. Herein, a copper(I)‐catalyzed asymmetric hydrophosphination of α,β‐unsaturated phosphine sulfides was developed with the assistance of “soft–soft” interaction between copper(I)‐catalyst and the phosphine sulfide moiety, which afforded 1,2‐bisphosphine derivatives with diversified electronic nature and steric hindrance in high to excellent yields with high to excellent enantioselectivity. Moreover, the challenging catalytic asymmetric hydrophosphination/protonation reaction was achieved with excellent enantioselectivity. Strikingly, the dynamic kinetic resolution of racemic diarylphosphines was also successfully carried out with high to excellent diastereo‐ and enantioselectivities. Interestingly, the nucleophilic copper(I)‐diphenylphosphide species was characterized by 31P NMR spectrum and mass spectrum. At last, three products were transformed to chiral 1,2‐bisphosphines, which were employed as ligands in Rh‐catalyzed asymmetric hydrogenation of α‐amino‐α,β‐unsaturated ester. The α‐amino acid derivative was produced in high enantioselectivity, which demonstrated the utility of the present methodology. 相似文献
994.
995.
AbstractIn continuation of the search for new compounds from the terrestrial fungus Aspergillus sp., one new butyrolactone, 3″-hydroxymethyl-butyrolactone II (1) was isolated. The chemical structure of 1 was confirmed by extensive 1D and 2D NMR and HR-ESI mass data analysis, and by comparison with literature data. The absolute configuration was also determined by ECD calculations. 相似文献
996.
Xiao Sun Dong Pei Wen‐Da Duan Jian‐Fei Liu Duo‐Long Di Xin‐Yi Huang 《Journal of separation science》2020,43(17):3573-3584
Elution‐extrusion counter current chromatography extrudes the most solute retained in the column with the highest possible peak resolution. It can greatly improve the hydrophobic window. In recent years, elution‐extrusion counter current chromatography has received extensive attention in the separation of complex samples. This article first reviews the development and application of elution‐extrusion counter current chromatography, including its origin, mechanism, advantages and disadvantages, and some representative applications. At the same time, this review also shared our visions and ideas on how to improve the elution‐extrusion mode. This article aims to provide certain reference for the research of this technology. 相似文献
997.
Siyuan Li Weidong Zhang Qiang Wu Lei Fan Xinyang Wang Xiao Wang Zeyu Shen Yi He Yingying Lu 《Angewandte Chemie (International ed. in English)》2020,59(35):14935-14941
A rechargeable Li metal anode coupled with a high‐voltage cathode is a promising approach to high‐energy‐density batteries exceeding 300 Wh kg?1. Reported here is an advanced dual‐additive electrolyte containing a unique solvation structure and it comprises a tris(pentafluorophenyl)borane additive and LiNO3 in a carbonate‐based electrolyte. This system generates a robust outer Li2O solid electrolyte interface and F‐ and B‐containing conformal cathode electrolyte interphase. The resulting stable ion transport kinetics enables excellent cycling of Li/LiNi0.8Mn0.1Co0.1O2 for 140 cycles with 80 % capacity retention under highly challenging conditions (≈295.1 Wh kg?1 at cell‐level). The electrolyte also exhibits high cycling stability for a 4.6 V LiCoO2 (160 cycles with 89.8 % capacity retention) cathode and 4.95 V LiNi0.5Mn1.5O4 cathode. 相似文献
998.
Biwei Xiao Hanshuo Liu Ning Chen Mohammad Norouzi Banis Haijun Yu Jianwen Liang Qian Sun Tsun‐Kong Sham Ruying Li Mei Cai Gianluigi A. Botton Xueliang Sun 《Angewandte Chemie (International ed. in English)》2020,59(34):14313-14320
Li‐ and Mn‐rich layered oxides are among the most promising cathode materials for Li‐ion batteries with high theoretical energy density. Its practical application is, however, hampered by the capacity and voltage fade after long cycling. Herein, a finite difference method for near‐edge structure (FDMNES) code was combined with in situ X‐ray absorption spectroscopy (XAS) and transmission electron microscopy/electron energy loss spectroscopy (TEM/EELS) to investigate the evolution of transition metals (TMs) in fresh and heavily cycled electrodes. Theoretical modeling reveals a recurring partially reversible LiMn2O4‐like sub‐nanodomain formation/dissolution process during each charge/discharge, which accumulates gradually and accounts for the Mn phase transition. From the modeling of spectra and maps of the valence state over large regions of the cathodes, it was found that the phase change is size‐dependent. After prolonged cycling, the TMs displayed different levels of inactivity. 相似文献
999.
Qun‐Liang Zhang Qin Xiong Miao‐Miao Li Wei Xiong Bin Shi Yu Lan Liang‐Qiu Lu Wen‐Jing Xiao 《Angewandte Chemie (International ed. in English)》2020,59(33):14096-14100
Higher‐order cycloadditions, particularly [8+2] cycloadditions, are a straightforward and efficient strategy for constructing significant medium‐sized architectures. Typically, configuration‐restrained conjugated systems are utilized as 8π‐components for higher‐order concerted cycloadditions. However, for this reason, 10‐membered monocyclic skeletons have never been constructed via catalytic asymmetric [8+2] cycloaddition with high peri‐ and stereoselectivity. Here, we accomplished an enantioselective [8+2] dipolar cycloaddition via the merger of visible‐light activation and asymmetric palladium catalysis. This protocol provides a new route to 10‐membered monocyclic architectures bearing chiral quaternary stereocenters with high chemo‐, peri‐, and enantioselectivity. The success of this strategy relied on the facile in situ generation of Pd‐containing 1,8‐dipoles and their enantioselective trapping by ketene dipolarophiles, which were formed in situ via a photo‐Wolff rearrangement. 相似文献
1000.
Kai Chen Gang Huang Jin‐Ling Ma Jin Wang Dong‐Yue Yang Xiao‐Yang Yang Yue Yu Xin‐Bo Zhang 《Angewandte Chemie (International ed. in English)》2020,59(38):16661-16667
The lithium (Li)–air battery has an ultrahigh theoretical specific energy, however, even in pure oxygen (O2), the vulnerability of conventional organic electrolytes and carbon cathodes towards reaction intermediates, especially O2?, and corrosive oxidation and crack/pulverization of Li metal anode lead to poor cycling stability of the Li‐air battery. Even worse, the water and/or CO2 in air bring parasitic reactions and safety issues. Therefore, applying such systems in open‐air environment is challenging. Herein, contrary to previous assertions, we have found that CO2 can improve the stability of both anode and electrolyte, and a high‐performance rechargeable Li–O2/CO2 battery is developed. The CO2 not only facilitates the in situ formation of a passivated protective Li2CO3 film on the Li anode, but also restrains side reactions involving electrolyte and cathode by capturing O2?. Moreover, the Pd/CNT catalyst in the cathode can extend the battery lifespan by effectively tuning the product morphology and catalyzing the decomposition of Li2CO3. The Li–O2/CO2 battery achieves a full discharge capacity of 6628 mAh g?1 and a long life of 715 cycles, which is even better than those of pure Li–O2 batteries. 相似文献