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71.
Ye Qian Mi Wei Deng Chaohui He Prof. Dr. Osman Eksik Yi Ping Zheng De Kun Yao Dr. Xian Bin Liu Yan Hong Yin Ye Sheng Li Prof. Dr. Bao Yu Xia Prof. Dr. Zi Ping Wu 《Angewandte Chemie (International ed. in English)》2023,62(12):e202218621
Solid-state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3-dioxolane electrolytes to fabricate integrated solid-state lithium batteries. The in situ polymerization and formation of solid-state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high-performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □−1 and high lithium-ion diffusion efficiency of 2.5×10−11 cm2 s−1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life. 相似文献
72.
Kang Sun Yunyang Qian Prof. Dr. Hai-Long Jiang 《Angewandte Chemie (International ed. in English)》2023,62(15):e202217565
Photocatalytic water splitting and carbon dioxide (CO2) reduction provide promising solutions to global energy and environmental issues. In recent years, metal-organic frameworks (MOFs), a class of crystalline porous solids featuring well-defined and tailorable structures as well as high surface areas, have captured great interest toward photocatalytic water splitting and CO2 reduction. In this review, the semiconductor-like behavior of MOFs is first discussed. We then summarize the recent advances in photocatalytic water splitting and CO2 reduction over MOF-based materials and focus on the unique advantage of MOFs for clarifying the structure-property relationship in photocatalysis. In addition, some representative characterization techniques have been presented to unveil the photocatalytic kinetics and reaction intermediates in MOF-based systems. Finally, the challenges, and perspectives for future directions are proposed. 相似文献
73.
Tianchen Qin Prof. Dr. Dezhou Guo Juanjuan Xiong Xingyu Li Lei Hu Weishan Yang Zijie Chen Yulun Wu Dr. Honghe Ding Dr. Jun Hu Qian Xu Dr. Tao Wang Prof. Dr. Junfa Zhu 《Angewandte Chemie (International ed. in English)》2023,62(43):e202306368
The electrical and mechanical properties of graphene-based materials can be tuned by the introduction of nanopores, which are sensitively related to the size, morphology, density, and location of nanopores. The synthesis of low-dimensional graphene nanostructures containing well-defined nonplanar nanopores has been challenging due to the intrinsic steric hindrance. Herein, we report the selective synthesis of one-dimensional (1D) graphene nanoribbons (GNRs) containing periodic nonplanar [14]annulene pores on Ag(111) and two-dimensional (2D) porous graphene nanosheet containing periodic nonplanar [30]annulene pores on Au(111), starting from a same precursor. The formation of distinct products on the two substrates originates from the different thermodynamics and kinetics of coupling reactions. The reaction mechanisms were confirmed by a series of control experiments, and the appropriate thermodynamic and kinetic parameters for optimizing the reaction pathways were proposed. In addition, the combined scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations revealed the electronic structures of porous graphene structures, demonstrating the impact of nonplanar pores on the π-conjugation of molecules. 相似文献
74.
Rémi Lavernhe Dr. Qian Wang Prof. Dr. Jieping Zhu 《Angewandte Chemie (International ed. in English)》2023,62(22):e202303537
Transition-metal-catalyzed [4+2] heteroannulation of α,β-unsaturated oximes and their derivatives with alkynes has been developed into a powerful strategy for the synthesis of pyridines. It nevertheless lacks regioselectivity when unsymmetrically substituted alkynes are used. We report herein the unprecedented synthesis of polysubstituted pyridines by a formal [5+1] heteroannulation of two readily accessible building blocks. A copper-catalyzed aza-Sonogashira cross-coupling between β,γ-unsaturated oxime esters and terminal alkynes affords ynimines, which, without isolation, undergo an acid-catalyzed domino reaction involving ketenimine formation, 6π-electrocyclization and aromatization to afford pyridines. Terminal alkynes served as a one-carbon donor to the pyridine core in this transformation. Di- through pentasubstituted pyridines are accessible with complete regioselectivity and excellent functional-group compatibility. The first total synthesis of anibamine B, an indolizinium alkaloid with potent antiplasmodial activity, was accomplished featuring this reaction as a key step. 相似文献
75.
Dr. Wenjun Zhan Lingling Xu Zhiyu Liu Xiaoyang Liu Dr. Ge Gao Tiantian Xia Xiaotong Cheng Dr. Xianbao Sun Prof. Dr. Fu-Gen Wu Prof. Dr. Qian Yu Prof. Dr. Gaolin Liang 《Angewandte Chemie (International ed. in English)》2023,62(32):e202306427
Staphylococcus aureus (S. aureus) is able to hide within host cells to escape immune clearance and antibiotic action, causing life-threatening infections. To boost the therapeutic efficacy of antibiotics, new intracellular delivery approaches are urgently needed. Herein, by rational design of an adamantane (Ada)-containing antibiotic-peptide precursor Ada-Gly-Tyr-Val-Ala-Asp-Cys(StBu)-Lys(Ciprofloxacin)-CBT ( Cip-CBT-Ada ), we propose a strategy of tandem guest-host-receptor recognitions to precisely guide ciprofloxacin to eliminate intracellular S. aureus. Via guest-host recognition, Cip-CBT-Ada is decorated with a β-cyclodextrin-heptamannoside ( CD-M ) derivative to yield Cip-CBT-Ada/CD-M , which is able to target mannose receptor-overexpressing macrophages via multivalent ligand-receptor recognition. After uptake, Cip-CBT-Ada/CD-M undergoes caspase-1 (an overexpressed enzyme during S. aureus infection)-initiated CBT-Cys click reaction to self-assemble into ciprofloxacin nanoparticle Nano-Cip . In vitro and in vivo experiments demonstrate that, compared with ciprofloxacin or Cip-CBT-Ada , Cip-CBT-Ada/CD-M shows superior intracellular bacteria elimination and inflammation alleviation efficiency in S. aureus-infected RAW264.7 cells and mouse infection models, respectively. This work provides a supramolecular platform of tandem guest-host-receptor recognitions to precisely guide antibiotics to eliminate intracellular S. aureus infection efficiently. 相似文献
76.
Mengdi Lv Yue Zheng Jian Wu Zhengqi Shen Binglian Guo Guojing Hu Yuanlei Huang Jingyue Zhao Prof. Yong Qian Prof. Zhi Su Prof. Chao Wu Prof. Xuling Xue Prof. Hong-Ke Liu Prof. Zong-Wan Mao 《Angewandte Chemie (International ed. in English)》2023,62(48):e202312897
Ferroptosis is a form of programmed cell death driven by iron-dependent lipid peroxidation (LPO) with the potential for antitumor immunity activation. In this study, a nonferrous cyclopentadienyl metal-based ferroptosis inducer [Ir(Cp*)(Bet)Cl]Cl ( Ir-Bet ) was developed by a metal-ligand synergistic enhancement (MLSE) strategy involving the reaction of [Ir(Cp*)Cl]2Cl2 with the natural product Betulin. The fusion of Betulin with iridium cyclopentadienyl (Ir-Cp*) species as Ir-Bet not only tremendously enhanced the antiproliferative activity toward cancer cells, but also activated ferritinophagy for iron homeostasis regulation by PI3K/Akt/mTOR cascade inhibition with a lower dosage of Betulin, and then evoked an immune response by nuclear factor kappa-B (NF-κB) activation of Ir-Cp* species. Further immunogenic cell death (ICD) occurred by remarkable ferroptosis through glutathione (GSH) depletion, glutathione peroxidase 4 (GPX4) deactivation and ferritinophagy. An in vivo vaccination experiment demonstrated desirable antitumor and immunogenic effects of Ir-Bet by increasing the ratio of cytotoxic T cells (CTLs)/regulatory T cells (Tregs). 相似文献
77.
Yao Qian Dr. Xiangyu Guo Prof. Yunfang Wang Prof. Zheng Ouyang Prof. Xiaoxiao Ma 《Angewandte Chemie (International ed. in English)》2023,62(52):e202312275
Spatial lipidomics based on mass spectrometry imaging (MSI) is a powerful tool for fundamental biology studies and biomarker discovery. But the structure-resolving capability of MSI is limited because of the lack of multiplexed tandem mass spectrometry (MS/MS) method, primarily due to the small sample amount available from each pixel and the poor ion usage in MS/MS analysis. Here, we report a mobility-modulated sequential dissociation (MMSD) strategy for multiplex MS/MS imaging of distinct lipids from biological tissues. With ion mobility-enabled data-independent acquisition and automated spectrum deconvolution, MS/MS spectra of a large number of lipid species from each tissue pixel are acquired, at no expense of imaging speed. MMSD imaging is highlighted by MS/MS imaging of 24 structurally distinct lipids in the mouse brain and the revealing of the correlation of a structurally distinct phosphatidylethanolamine isomer (PE 18 : 1_18 : 1) from a human hepatocellular carcinoma (HCC) tissue. Mapping of structurally distinct lipid isomers is now enabled and spatial lipidomics becomes feasible for MSI. 相似文献
78.
Bingchu Tian Dr. Yanbo Shang Yi Tu Dr. Jun Hu Dr. Dong Han Qian Xu Prof. Shangfeng Yang Prof. Yifan Ye Dr. Honghe Ding Dr. Yu Li Prof. Junfa Zhu 《Chemphyschem》2023,24(20):e202300400
The interfacial electronic structure of perovskite layers and transport layers is critical for the performance and stability of perovskite solar cells (PSCs). The device performance of PSCs can generally be improved by adding a slight excess of lead iodide (PbI2) to the precursor solution. However, its underlying working mechanism is controversial. Here, we performed a comprehensive study of the electronic structures at the interface between CH3NH3PbI3 and C60 with and without the modification of PbI2 using in situ photoemission spectroscopy measurements. The correlation between the interfacial structures and the device performance was explored based on performance and stability tests. We found that there is an interfacial dipole reversal, and the downward band bending is larger at the CH3NH3PbI3/C60 interface with the modification of PbI2 as compared to that without PbI2. Therefore, PSCs with PbI2 modification exhibit faster charge carrier transport and slower carrier recombination. Nevertheless, the modification of PbI2 undermines the device stability due to aggravated iodide migration. Our findings provide a fundamental understanding of the CH3NH3PbI3/C60 interfacial structure from the perspective of the atomic layer and insight into the double-edged sword effect of PbI2 as an additive. 相似文献
79.
Dr. Shuai Zhao Bin-Wei Lu Ning Bao Zi-Jian Yin Dr. Mingcheng Qian Lin Cao Min Geng Ye Lin Prof. Dr. Xin Chen 《European journal of organic chemistry》2023,26(2):e202201239
A palladium-catalyzed oxidative amidation of conjugated olefin with 2-pyridone is described. A series of E-Enamides were synthesized in a highly stereocontrolled manner. The reaction also accommodates other cyclic and acyclic amides. Z-Enamides were predominantly prepared for primary amides probably due to the presence of an intramolecular hydrogen bond. Gram-scale synthesis of enamide and the following oxidative annulation with diphenylacetylene demonstrates the synthetic utility of this reaction. 相似文献
80.
Bing-Chang Tan Qian Wang Long-Long Jiang Ying Song Prof. Xin-Tao Wu Prof. Tian-Lu Sheng 《欧洲无机化学杂志》2023,26(12):e202300003
To investigate the effect of ligand remote (>10 Å) substituents on the bridging metal center on the metal-to-metal charge transfer (MMCT) properties in cyanidometa-bridged complexes, a series of new cyanidometal-bridged complexes and their one-electron and two-electron oxidation products have been synthesized and well characterized (namely, trans-[Cp(dppe)Fe−NC−(L)Ru(PPh3)−CN−Fe(dppe)Cp][PF6]n (n=2, 3, 4) (L=dmptpy, 1[PF6]n ; L=meoptpy, 2[PF6]n ; L=t-Buptpy, 3[PF6]n ) (Cp=1,3-cyclopentadiene, dppe=1,2-bis(diphenylphosphino)ethane, PPh3=triphenylphosphine, dmptpy=4′-(4-dimethylaminophenyl)-2,2′,6′,2′′-terpyridine, meoptpy=4′-(4-methoxyphenyl)-2,2′,6′,2′′-terpyridine, t-Buptpy=4′-(4-tertbutylphenyl)-2,2′,6′,2′′-terpyridine)). The investigations suggest that the cyanido-stretching (νCN) vibration energy for the complexes is unsensitive to the electron-donating ability change of the remote substituents of the cyanidometal bridging auxiliary ligand from tertbutyl, methoxy to dimethylamino group. However, the MMCT energies of the one- and two-electron oxidation complexes are still sensitive to the remote substituents of the ligand on the bridging metal center, and decreases with the increase of the electron-donating ability of the remote substituents from tertbutyl, methoxy to dimethylamino group. All one-electron and two-electron oxidation products belong to Class II mixed valence compounds according to the classification of Robin and Day. 相似文献