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991.
Dr. Wei Bai Jingyu Gao Dr. Kun Li Gongrui Wang Dr. Tengfei Zhou Pengju Li Prof. Shengyong Qin Prof. Genqiang Zhang Prof. Zaiping Guo Prof. Chong Xiao Prof. Yi Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(40):17647-17651
Volume expansion and poor conductivity are two major obstacles that hinder the pursuit of the lithium-ion batteries with long cycling life and high power density. Herein, we highlight a misfit compound PbNbS3 with a soft/rigid superlattice structure, confirmed by scanning tunneling microscopy and electrochemical characterization, as a promising anode material for high performance lithium-ion batteries with optimized capacity, stability, and conductivity. The soft PbS sublayers primarily react with lithium, endowing capacity and preventing decomposition of the superlattice structure, while the rigid NbS2 sublayers support the skeleton and enhance the migration of electrons and lithium ions, as a result leading to a specific capacity of 710 mAh g−1 at 100 mA g−1, which is 1.6 times of NbS2 and 3.9 times of PbS. Our finding reveals the competitive strategy of soft/rigid structure in lithium-ion batteries and broadens the horizons of single-phase anode material design. 相似文献
992.
Qun-Liang Zhang Qin Xiong Miao-Miao Li Wei Xiong Bin Shi Prof. Yu Lan Prof. Liang-Qiu Lu Prof. Wen-Jing Xiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):14200-14204
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
993.
Yajie Liu Zelin Duan Jing Fang Fan Zhang Prof. Junyu Xiao Prof. Wen-Bin Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16256-16261
Herein, we report the biosynthesis of protein heterocatenanes using a programmed sequence of multiple post-translational processing events including intramolecular chain entanglement, in situ backbone cleavage, and spontaneous cyclization. The approach is general, autonomous, and can obviate the need for any additional enzymes. The catenane topology was convincingly proven using a combination of SDS-PAGE, LC-MS, size exclusion chromatography, controlled proteolytic digestion, and protein crystallography. The X-ray crystal structure clearly shows two mechanically interlocked protein rings with intact folded domains. It opens new avenues in the nascent field of protein-topology engineering. 相似文献
994.
Guangjun Li Weigang Hu Yongnan Sun Jiayu Xu Xiao Cai Xinglian Cheng Yuying Zhang Ancheng Tang Xu Liu Prof. Mingyang Chen Prof. Weiping Ding Prof. Yan Zhu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21321-21328
The emergence of atomically precise metal nanoclusters with unique electronic structures provides access to currently inaccessible catalytic challenges at the single-electron level. We investigate the catalytic behavior of gold Au25(SR)18 nanoclusters by monitoring an incoming and outgoing free valence electron of Au 6s1. Distinct performances are revealed: Au25(SR)18− is generated upon donation of an electron to neutral Au25(SR)180 and this is associated with a loss in reactivity, whereas Au25(SR)18+ is generated from dislodgment of an electron from neutral Au25(SR)180 with a loss in stability. The reactivity diversity of the three Au25(SR)18 clusters stems from different affinities with reactants and the extent of intramolecular charge migration during the reactions, which are closely associated with the valence occupancies of the clusters varied by one electron. The stability difference in the three clusters is attributed to their different equilibria, which are established between the AuSR dissociation and polymerization influenced by one electron. 相似文献
995.
Dr. Xiaocui Guo Prof. Feng Li Chunxia Liu Yi Zhu Nannan Xiao Dr. Zi Gu Prof. Dan Luo Prof. Jianhui Jiang Prof. Dayong Yang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20832-20839
The design of controllable dynamic systems is vital for the construction of organelle-like architectures in living cells, but has proven difficult due to the lack of control over defined topological transformation of self-assembled structures. Herein, we report a DNA based dynamic assembly system that achieves lysosomal acidic microenvironment specifically inducing topological transformation from nanoparticles to organelle-like hydrogel architecture in living cells. Designer DNA nanoparticles are constructed from double-stranded DNA with cytosine-rich stick ends (C-monomer) and are internalized into cells through lysosomal pathway. The lysosomal acidic microenvironment can activate the assembly of DNA monomers, inducing transformation from nanoparticles to micro-sized organelle-like hydrogel which could further escape into cytoplasm. We show how the hydrogel regulates cellular behaviors: cytoskeleton is deformed, cell tentacles are significantly shortened, and cell migration is promoted. 相似文献
996.
Dr. Yao Xiao Yan-Fang Zhu Dr. Wei Xiang Dr. Zhen-Guo Wu Yong-Chun Li Jing Lai Shi Li Dr. Enhui Wang Zu-Guang Yang Chun-Liu Xu Prof. Ben-He Zhong Prof. Xiao-Dong Guo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(4):1507-1511
Demands for large-scale energy storage systems have driven the development of layered transition-metal oxide cathodes for room-temperature rechargeable sodium ion batteries (SIBs). Now, an abnormal layered-tunnel heterostructure Na0.44Co0.1Mn0.9O2 cathode material induced by chemical element substitution is reported. By virtue of beneficial synergistic effects, this layered-tunnel electrode shows outstanding electrochemical performance in sodium half-cell system and excellent compatibility with hard carbon anode in sodium full-cell system. The underlying formation process, charge compensation mechanism, phase transition, and sodium-ion storage electrochemistry are clearly articulated and confirmed through combined analyses of in situ high-energy X-ray diffraction and ex situ X-ray absorption spectroscopy as well as operando X-ray diffraction. This crystal structure engineering regulation strategy offers a future outlook into advanced cathode materials for SIBs. 相似文献
997.
Two new 1D helical coordination polymers based on polyoxometalate were synthesized by self-assembly of Keggin-type POMs and copper salts in the presence of triangular N-heterocyclic derivatives or long-chain N-containing carboxylate ligand, that are, (H3O)[{Cu(H2tpim)2}{SiMo12O40}] · 0.5H2O [Htpim = 2,4,5-tri(4-pyridyl)-imidazole] ( 1 ) and [Cu2(Hcpp)3(cpp)(H2O)][PMo12O40] · 2H2O [Hcpp = 1-(4-cyanobenzyl)-3–2-yl)pyrazole] ( 2 ). Their structures were determined by single-crystal X-ray diffraction and further characterized by elemental analyses and TG analyses. Compounds 1 and 2 exhibit (1D→2D) interdigitated architectures assembled from 1D helical chains. In compound 1 , the achiral 2D interdigitated nets containing left- and right-handed helixes are further interdigitated with each other to form a 3D supramolecular framework. In compound 2 , adjacent 2D interdigitated layers with opposite chirality are further extended by supramolecular interactions into a 3D supramolecular network, in which non-coordinating Keggin-type POMs as guests are encapsulated. 相似文献
998.
Integration of MnOx into the carbon matrix proves a viable strategy to improve the electrochemical performance of MnOx materials. Mn3O4 nanoparticle-decorated N-doped carbon composites (Mn3O4@N-doped carbon) were facilely prepared from a non-porous eight-fold interpenetrated ZnII-based MOF, which involves first synthesis of bimetallic Mn/Zn-MOF in one-pot reaction followed by direct pyrolysis at 1000 °C. In 0.1 m KOH solution, the optimal Mn3O4@N-doped carbon exhibits decent oxygen reduction activity with the onset potential (Eonset) of 0.94 V (vs. RHE) and half-wave potential (E1/2) of 0.81 V (vs. RHE), excellent methanol tolerance as well as good durability. 相似文献
999.
Dr. Xi-Sha Zhang Yan-Ying Huang Jing Zhang Dr. Wei Meng Dr. Qian Peng Ruirui Kong Zhenwei Xiao Dr. Jie Liu Miaofei Huang Dr. Yuanping Yi Liangliang Chen Qingrui Fan Dr. Gaobo Lin Dr. Zitong Liu Dr. Guanxin Zhang Dr. Lang Jiang Prof. Dr. Deqing Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3557-3561
Polycyclic aromatic hydrocarbons with hexagons/pentagons or hexagons/heptagons have been intensively investigated in recent years, but those with simultaneous presence of hexagons, pentagons and heptagons remain rare. In this paper, we report dicyclohepta[ijkl,uvwx]rubicene ( DHR ), a non-benzenoid isomer of dibenzo[bc,kl]coronene with two pentagons and two heptagons. We developed an efficient and scalable synthetic method for DHR by using Scholl reaction and dehydrogenation. Crystal structure of DHR shows that the benzenoid rings, two pentagons and two heptagons are coplanar. The bond lengths analysis and the ICSS(1)zz and LOL-π calculations indicate that the incorporation of two formal azulene moieties has an effect on the conjugated structure. The π-electrons of benzenoid and pentagon rings are more delocalized. Cyclic voltammetry studies indicate that DHR shows multiple oxidation and reduction potentials. Interestingly, DHR exhibits unusual S0 to S2 absorption and abnormal anti-Kasha S2 to S0 emission. Moreover, crystals of DHR exhibit semiconducting behaviour with hole mobility up to 0.082 cm2 V−1 s−1. 相似文献
1000.
Shan Jin Manman Zhou Xi Kang Xiaowu Li Wenjun Du Xiao Wei Shuang Chen Dr. Shuxin Wang Prof. Manzhou Zhu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):3919-3923
The high-dimensional (that is, three-dimensional (3D)) assembly of nanomaterials is an effective means of improving their properties; however, achieving this assembly at the atomic level remains challenging. Herein, we obtained a novel nanocluster, [Au8Ag57(Dppp)4(C6H11S)32Cl2]Cl (Dppp=1,3-bis(diphenylphosphino)propane) showing a 3D octameric assembly mode involving the kernel penetration of eight complete icosahedral Au@Ag10Au2 units for the first time. The atomically precise structure was determined by single-crystal X-ray diffraction, and further confirmed by thermogravimetric analysis, X-ray photoelectron spectroscopy, and electrospray ionization mass spectrometry measurements. Furthermore, ligand-induced transformation prompted the conversion of [Au8Ag57(Dppp)4(C6H11S)32Cl2]Cl, with complete octameric fusion into [Au8Ag55(Dppp)4(C6H11S)34][BPh4]2, with incomplete octameric fusion. These observations will hopefully facilitate further research on the assembly of M13 nanobuilding blocks. 相似文献