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51.
Prof. Dr. Jie Shen Deepa R Zhongyan Li Hyeonji Oh Harekrushna Behera Dr. Himanshu Joshi Prof. Dr. Manish Kumar Prof. Dr. Aleksei Aksimentiev Prof. Dr. Huaqiang Zeng 《Angewandte Chemie (International ed. in English)》2023,62(39):e202305623
Unlike many other biologically relevant ions (Na+, K+, Ca2+, Cl−, etc) and protons, whose cellular concentrations are closely regulated by highly selective channel proteins, Li+ ion is unusual in that its concentration is well tolerated over many orders of magnitude and that no lithium-specific channel proteins have so far been identified. While one naturally evolved primary pathway for Li+ ions to traverse across the cell membrane is through sodium channels by competing with Na+ ions, highly sought-after artificial lithium-transporting channels remain a major challenge to develop. Here we show that sulfur-containing organic nanotubes derived from intramolecularly H-bonded helically folded aromatic foldamers of 3.6 Å in hollow cavity diameter could facilitate highly selective and efficient transmembrane transport of Li+ ions, with high transport selectivity factors of 15.3 and 19.9 over Na+ and K+ ions, respectively. 相似文献
52.
Yaxin Zeng Prof. Dr. Ying Xia 《Angewandte Chemie (International ed. in English)》2023,62(32):e202307129
Direct synthesis of gem-difluorinated carbocyclic molecules represents a longstanding challenge in organic chemistry. Herein, a Rh-catalyzed [3+2] cycloaddition reaction between readily available gem-difluorinated cyclopropanes (gem-DFCPs) and internal olefins has been developed, enabling the efficient synthesis of gem-difluorinated cyclopentanes with good functional group compatibility, excellent regioselectivity and good diastereoselectivity. The resulting gem-difluorinated products can undergo downstream transformations to access various mono-fluorinated cyclopentenes and cyclopentanes. This reaction demonstrates the use of gem-DFCPs as a type of “CF2” C3 synthon for cycloaddition under transition metal catalysis, which provides potential strategy for synthesizing other gem-difluorinated carbocyclic molecules. 相似文献
53.
Dr. Yinxiang Zeng Zhihao Pei Dr. Yan Guo Dr. Deyan Luan Prof. Xiaojun Gu Prof. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2023,62(45):e202312145
Constructing multifunctional interphases to suppress the rampant Zn dendrite growth and detrimental side reactions is crucial for Zn anodes. Herein, a phytic acid (PA)-ZnAl coordination compound is demonstrated as a versatile interphase layer to stabilize Zn anodes. The zincophilic PA-ZnAl layer can manipulate Zn2+ flux and promote rapid desolvation kinetics, ensuring the uniform Zn deposition with dendrite-free morphology. Moreover, the robust PA-ZnAl protective layer can effectively inhibit the hydrogen evolution reaction and formation of byproducts, further contributing to the reversible Zn plating/stripping with high Coulombic efficiency. As a result, the Zn@PA-ZnAl electrode shows a lower Zn nucleation overpotential and higher Zn2+ transference number compared with bare Zn. The Zn@PA-ZnAl symmetric cell exhibits a prolonged lifespan of 650 h tested at 5 mA cm−2 and 5 mAh cm−2. Furthermore, the assembled Zn battery full cell based on this Zn@PA-ZnAl anode also delivers decent cycling stability even under harsh conditions. 相似文献
54.
Dr. Hongshuang Guo Dr. Chen Liang Dr. Tero-Petri Ruoko Dr. Henning Meteling Dr. Bo Peng Dr. Hao Zeng Prof. Arri Priimagi 《Angewandte Chemie (International ed. in English)》2023,62(43):e202309402
Shape-changing polymeric materials have gained significant attention in the field of bioinspired soft robotics. However, challenges remain in versatilizing the shape-morphing process to suit different tasks and environments, and in designing systems that combine reversible actuation and self-healing ability. Here, we report halogen-bonded liquid crystal elastomers (LCEs) that can be arbitrarily shape-programmed and that self-heal under mild thermal or photothermal stimulation. We incorporate halogen-bond-donating diiodotetrafluorobenzene molecules as dynamic supramolecular crosslinks into the LCEs and show that these relatively weak crosslinks are pertinent for their mechanical programming and self-healing. Utilizing the halogen-bonded LCEs, we demonstrate proof-of-concept soft robotic motions such as crawling and rolling with programmed velocities. Our results showcase halogen bonding as a promising, yet unexplored tool for the preparation of smart supramolecular constructs for the development of advanced soft actuators. 相似文献
55.
Mengjiao Zhuansun Yue Liu Ruihu Lu Fan Zeng Zhanyou Xu Ying Wang Prof. Yaoyue Yang Prof. Ziyun Wang Prof. Gengfeng Zheng Prof. Yuhang Wang 《Angewandte Chemie (International ed. in English)》2023,62(41):e202309875
Advancing the performance of the Cu-catalyzed electrochemical CO2 reduction reaction (CO2RR) is crucial for its practical applications. Still, the wettable pristine Cu surface often suffers from low exposure to CO2, reducing the Faradaic efficiencies (FEs) and current densities for multi-carbon (C2+) products. Recent studies have proposed that increasing surface availability for CO2 by cation-exchange ionomers can enhance the C2+ product formation rates. However, due to the rapid formation and consumption of *CO, such promotion in reaction kinetics can shorten the residence of *CO whose adsorption determines C2+ selectivity, and thus the resulting C2+ FEs remain low. Herein, we discover that the electro-kinetic retardation caused by the strong hydrophobicity of quaternary ammonium group-functionalized polynorbornene ionomers can greatly prolong the *CO residence on Cu. This unconventional electro-kinetic effect is demonstrated by the increased Tafel slopes and the decreased sensitivity of *CO coverage change to potentials. As a result, the strongly hydrophobic Cu electrodes exhibit C2+ Faradaic efficiencies of ≈90 % at a partial current density of 223 mA cm−2, more than twice of bare or hydrophilic Cu surfaces. 相似文献
56.
Yunpeng Zhong Xuesong Xie Prof. Zhiyuan Zeng Prof. Bingan Lu Prof. Gen Chen Prof. Jiang Zhou 《Angewandte Chemie (International ed. in English)》2023,62(40):e202310577
Aqueous rechargeable zinc-ion batteries (ARZBs) are impeded by the mutual problems of unstable cathode, electrolyte parasitic reactions, and dendritic growth of zinc (Zn) anode. Herein, a triple-functional strategy by introducing the tetramethylene sulfone (TMS) to form a hydrated eutectic electrolyte is reported to ameliorate these issues. The activity of H2O is inhibited by reconstructing hydrogen bonds due to the strong interaction between TMS and H2O. Meanwhile, the preferentially adsorbed TMS on the Zn surface increases the thickness of double electric layer (EDL) structure, which provides a shielding buffer layer to suppress dendrite growth. Interestingly, TMS modulates the primary solvation shell of Zn2+ ultimately to achieve a novel solvent co-intercalation ((Zn-TMS)2+) mechanism, and the intercalated TMS works as a “pillar” that provides more zincophilic sites and stabilizes the structure of cathode (NH4V4O10, (NVO)). Consequently, the Zn||NVO battery exhibits a remarkably high specific capacity of 515.6 mAh g−1 at a low current density of 0.2 A g−1 for over 40 days. This multi-functional electrolytes and solvent co-intercalation mechanism will significantly propel the practical development of aqueous batteries. 相似文献
57.
Mingjie Zeng Changyue Yu Yibing Wang Jingjing Wang Jiang Wang Hong Liu 《Angewandte Chemie (International ed. in English)》2023,62(22):e202300424
We report a ligand-controlled CoII-catalyzed C(sp3)−C(sp3) coupling hydroalkylation for direct and β-selective synthesis of 2-deoxy-C-glycosides from glycals. This reaction proceeds by a radical pathway for alkyl halide activation and is β-selective through ligand control. This approach may inspire the development of further stereoselective coupling reactions with potential application in the field of carbohydrates. 相似文献
58.
Linlong Dai Yuheng Liu Qing Xu Meifang Wang Dr. Qiaohong Zhu Prof. Dr. Peiyuan Yu Prof. Dr. Guofu Zhong Prof. Dr. Xiaofei Zeng 《Angewandte Chemie (International ed. in English)》2023,62(7):e202216534
Diaryl ethers are widespread in biologically active compounds, ligands and catalysts. It is known that the diaryl ether skeleton may exhibit atropisomerism when both aryl rings are unsymmetrically substituted with bulky groups. Despite recent advances, only very few catalytic asymmetric methods have been developed to construct such axially chiral compounds. We describe herein a dynamic kinetic resolution approach to axially chiral diaryl ethers via a Brønsted acid catalyzed atroposelective transfer hydrogenation (ATH) reaction of dicarbaldehydes with anilines. The desired diaryl ethers could be obtained in moderate to good chemical yields (up to 79 %) and high enantioselectivities (up to 95 % ee) under standard reaction conditions. Such structural motifs are interesting precursors for further transformations and may have potential applications in the synthesis of chiral ligands or catalysts. 相似文献
59.
Jiahui Zeng Yu Fu Yue Wu Shanshan Wang Wenxiang Zhang Prof. Heping Ma 《Angewandte Chemie (International ed. in English)》2023,62(42):e202310235
Xe is an ideal anesthetic gas, but it has not been widely used in practice due to its high cost and low output. Closed-circuit Xe recovery and recycling is an economically viable method to ensure adequate supply in medical use. Herein, we design an innovative way to recover Xe by using a stable fluorinated metal-organic framework (MOF) NbOFFIVE-1-Ni to eliminate CO2 from moist exhaled anesthetic gases. Unlike other Xe recovery MOFs with low Xe/CO2 selectivity (less than 10), NbOFFIVE-1-Ni could achieve absolute molecular sieve separation of CO2/Xe with excellent CO2 selectivity (825). Mixed-gas breakthrough experiments assert the potential of NbOFFIVE-1-Ni as a molecular sieve adsorbent for the effective and energy-efficient removal of carbon dioxide with 99.16 % Xe recovery. Absolute CO2/Xe separation in NbOFFIVE-1-Ni makes closed-circuit Xe recovery and recycling can be easily realized, demonstrating the potential of NbOFFIVE-1-Ni for important anesthetic gas regeneration under ambient conditions. 相似文献
60.
Yiding Wang Lei Shen Helin Wang Yixin Luo Prof. Dr. Qingle Zeng 《European journal of organic chemistry》2023,26(7):e202200942
Ring-opening addition reaction of activated vinyl cyclopropanes with N-tosylhydrazones in the presence of palladium(0) and triphenylphosphine affords N-tosylhydrazone butenylmalonate compounds. Aromatic aldehyde-derived N-tosylhydrazones produced terminal and internal N-allylated products, in which the terminal products are the main. While ketone-derived tosylhydrazones produced only terminal addition products. The transformation relationship of the terminal and internal N-allylated products in the reaction was also observed. A reasonable mechanism is proposed based on preliminary experimental results. 相似文献