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991.
Meng Zhao Dr. Hong-Jie Peng Bo-Quan Li Dr. Xiao Chen Jin Xie Dr. Xinyan Liu Prof. Qiang Zhang Prof. Jia-Qi Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):9096-9102
In situ evolution of electrocatalysts is of paramount importance in defining catalytic reactions. Catalysts for aprotic electrochemistry such as lithium–sulfur (Li-S) batteries are the cornerstone to enhance intrinsically sluggish reaction kinetics but the true active phases are often controversial. Herein, we reveal the electrochemical phase evolution of metal-based pre-catalysts (Co4N) in working Li-S batteries that renders highly active electrocatalysts (CoSx). Electrochemical cycling induces the transformation from single-crystalline Co4N to polycrystalline CoSx that are rich in active sites. This transformation propels all-phase polysulfide-involving reactions. Consequently, Co4N enables stable operation of high-rate (10 C, 16.7 mA cm−2) and electrolyte-starved (4.7 μL mgS−1) Li-S batteries. The general concept of electrochemically induced sulfurization is verified by thermodynamic energetics for most of low-valence metal compounds. 相似文献
992.
Yuchao Zhu Ziyao Zhang Rui Jin Jianzhong Liu Guoquan Liu Prof. Bing Han Prof. Ning Jiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20023-20028
Control of selectivity is one of the central topics in organic chemistry. Although unprecedented alkoxyl-radical-induced transformations have drawn a lot of attention, compared to selective C−H activation, selective radical O−H activation remains less explored. Herein, we report a novel selective radical O−H activation strategy of diols by combining spatial effects with proton-coupled electron transfer (PCET). It was found that DMSO is an essential reagent that enables the regioselective transformation of diols. Mechanistic studies indicated the existence of the alkoxyl radical and the selective interaction between DMSO and hydroxyl groups. Moreover, the distal C−C cleavage was realized by this selective alkoxyl-radical-initiation protocol. 相似文献
993.
Rational Design of Cyclometalated Iridium(III) Complexes for Three-Photon Phosphorescence Bioimaging
Dr. Chengzhi Jin Fengyin Liang Dr. Jinquan Wang Dr. Lili Wang Dr. Jiangping Liu Xinxing Liao Dr. Thomas W. Rees Bo Yuan Prof. Dr. Hui Wang Prof. Dr. Yong Shen Prof. Dr. Zhong Pei Prof. Dr. Liangnian Ji Prof. Dr. Hui Chao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16121-16125
Compared to 2PE (two-photon excitation) microscopy, 3PE microscopy has superior spatial resolution, deeper tissue penetration, and less defocused interference. The design of suitable agents with a large Stokes shift, good three-photon absorption (3PA), subcellular targeting, and fluorescence lifetime imaging (FLIM) properties, is challenging. Now, two IrIII complexes (3PAIr1 and 3PAIr2) were developed as efficient three-photon phosphorescence (3PP) agents. Calculations reveal that the introduction of a new group to the molecular scaffold confers a quadruple promotion in three-photon transition probability. Confocal and lifetime imaging of mitochondria using IrIII complexes as 3PP agents is shown. The complexes exhibit low working concentration (50 nm ), fast uptake (5 min), and low threshold for three-photon excitation power (0.5 mW at 980 nm). The impressive tissue penetration depth (ca. 450 μm) allowed the 3D imaging and reconstruction of brain vasculature from a living specimen. 相似文献
994.
Feng-Xing Li Shu-Jian Ren Pei-Fang Li Peng Yang Prof. Jin Qu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18631-18636
The rapid synthesis of marine ladder polyethers from polyepoxide precursors (in analogy with the biosynthetic pathway hypothesized by Nakanishi) is hampered by the fact that the exo-selective epoxide-opening cyclization cascade that gives THF-type polyethers is preferred over the endo-selective cascade that gives the desired products. We found that perfluoro-tert-butanol (PFTB) cooperating with 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM]BF4) can promote endo-selective epoxide-opening cyclization reactions of trisubstituted epoxy alcohols. Starting from readily accessible homochiral polyepoxy alcohols with a methyl group at all the endo-cyclization sites, we were able to construct polyethers up to five consecutive fused 6-, 7-, and/or 8-membered rings in one step. Notably, molecules with the 7/7/6/6 and 7/7/6/7/6 polyether frameworks of hemibrevetoxin B and brevenal, respectively, could be synthesized in 40 % and 17 % chemical yields. 相似文献
995.
Yun Liu Guangze Yang Song Jin Run Zhang Peng Chen Tengjisi Lianzhou Wang Dong Chen David A. Weitz Chun-Xia Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20240-20249
Understanding drug-release kinetics is critical for the development of drug-loaded nanoparticles. We developed a J-aggregate-based Förster-resonance energy-transfer (FRET) method to investigate the release of novel high-drug-loading (50 wt %) nanoparticles in comparison with low-drug-loading (0.5 wt %) nanoparticles. Single-dye-loaded nanoparticles form J-aggregates because of the high dye-loading (50 wt %), resulting in a large red-shift (≈110 nm) in the fluorescence spectrum. Dual-dye-loaded nanoparticles with high dye-loading using FRET pairs exhibited not only FRET but also a J-aggregate red-shift (116 nm). Using this J-aggregate-based FRET method, dye-core–polymer-shell nanoparticles showed two release processes intracellularly: the dissolution of the dye aggregates into dye molecules and the release of the dye molecules from the polymer shell. Also, the high-dye-loading nanoparticles (50 wt %) exhibited a slow release kinetics in serum and relatively quick release in cells, demonstrating their great potential in drug delivery. 相似文献
996.
Yufei Shu Dr. Xing Lin Dr. Haiyan Qin Zhuang Hu Prof. Yizheng Jin Prof. Xiaogang Peng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22496-22507
This article offers a materials-chemistry perspective for colloidal quantum dots (QDs) in the field of display, including QD-enhanced liquid-crystal-display (QD-LCD) and QD-based light-emitting-diodes (QLEDs) display. The rapid successes of QDs for display in the past five years are not accidental but have a deep root in both maturity of their synthetic chemistry and their unique chemical, optical, and optoelectronic properties. This article intends to discuss the natural match of QD emitters for display and chemical means to eventually bring about their full potential. 相似文献
997.
Kai Chen Gang Huang Jin-Ling Ma Jin Wang Dong-Yue Yang Xiao-Yang Yang Yue Yu Prof. Xin-Bo Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(38):16804-16810
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
998.
Dr. Song Jin Youxuan Ni Zhimeng Hao Prof. Kai Zhang Dr. Yong Lu Dr. Zhenhua Yan Dr. Yajuan Wei Dr. Ying-Rui Lu Dr. Ting-Shan Chan Prof. Jun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22069-22073
A general graphene quantum dot-tethering design strategy to synthesize single-atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0–4.5 wt %. The direct transmission electron microscopy imaging and X-ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications. 相似文献
999.
Shaojun Yang Qiao Tang Long Chen Jin Chang Tian Jiang Jingyi Zhao Prof. Ming Wang Prof. Peng R. Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18243-18250
The abundance of bacterial effectors have inspired us to explore their potential in rewiring malignant cell signaling. Their incapability for entering cells, however, hinders such application. Herein we developed a cationic lipid-based high throughput library screening platform for effective intracellular delivery of bacterial effectors. As the misregulated MAPK signaling is a hallmark of many types of cancer, we turned to the Shigella effector OspF which irreversibly inactivates ERK, the terminal component of MAPK cascade. We created a function-based screening assay to obtain AMPA-O16B lipid nanoparticles for effective OspF intracellular delivery, which inhibited the malignant MAPK signaling and tumor growth in vitro and in vivo. Furthermore, the optimized lipid nanoparticle formulation can deliver OspF to modulate the immunosuppressive responses in macrophages. Our work is a general strategy to explore the therapeutic potentials of naturally evolved bacterial effectors. 相似文献
1000.
Yu-Xin Guo Xiao-Ye Jin Zhi-Yu Xia Chong Chen Wei Cui Bo-Feng Zhu 《Electrophoresis》2020,41(9):649-656
In this study, a small set of ancestry informative SNPs was selected to differentiate African, European, East and South Asian samples, which was detected by the next-generation sequencing technology. A total of 127 Chinese Shaanxi Han individuals were collected as test samples. No statistically significant linkage disequilibrium of any pair of loci or departure from Hardy–Weinberg equilibrium of each locus was observed in the test population. To evaluate the performance of ancestry assignment using this panel, admixture analysis, principal component analysis, and likelihood ratio calculations were conducted based on the 1000 genome data and test samples. All populations were clustered into four groups, African, European, South and East Asian populations, which were consistent with their geographical origins. The pairwise fixation index (FST) between populations from different continental groups ranged from 0.140 to 0.621 with average 0.415, and the pairwise FST between populations from the same continent ranged from 0.000 to 0.056 with average 0.012. The likelihood ratio results of 125 test individuals indicated that their ancestry components were highly possible from East Asia. In conclusion, this small set of ancestry informative SNPs can be used as a reliable tool to identify and quantify ancestry components of unknown samples. 相似文献