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学者姓名:沈杰
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H-bonded helically folded aromatic foldamers rely on the precise formation of H-bonds between each helicity codon and its neighboring codons to maintain their structure. We report here for the first time that the phenyl group, referred to as a non-helicity codon due to its inability to form H-bonds, does not necessarily disrupt the helical structure. Specifically, we modified our recently reported pyridine-based aquapentamers by sequentially replacing each of the five pyridine residues with a phenyl group, creating a series of five hybrid pentamers. The phenyl groups, unable to form H-bonds with the adjacent N-H bonds of the amides, introduce H-bond defects along the helical backbone. Despite these defects, three out of five pentamers still adopt a helical structure and function as highly selective and ultra-fast abiotic water channels, with the most efficient channel achieving a water transport rate of 1.8 x 109 H2O s-1 per channel-approximately 30% of aquaporin Z's capacity.
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GB/T 7714 | Cao, Gaiping , Yang, Zihong , Zhao, Huaiqing et al. Superfast and highly selective water transport by hybrid aquapentamers incorporating a non-helicity codon [J]. | ORGANIC CHEMISTRY FRONTIERS , 2025 , 12 (5) : 1603-1611 . |
MLA | Cao, Gaiping et al. "Superfast and highly selective water transport by hybrid aquapentamers incorporating a non-helicity codon" . | ORGANIC CHEMISTRY FRONTIERS 12 . 5 (2025) : 1603-1611 . |
APA | Cao, Gaiping , Yang, Zihong , Zhao, Huaiqing , Shen, Jie , Chang, Wenju , Liu, Zhiwei et al. Superfast and highly selective water transport by hybrid aquapentamers incorporating a non-helicity codon . | ORGANIC CHEMISTRY FRONTIERS , 2025 , 12 (5) , 1603-1611 . |
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In subzero environments, sluggish electrochemical kinetics and unstable electrode/electrolyte interphases hinder progress in lithium metal batteries (LMBs), emphasizing the need for advanced electrolytes to ensure stability in harsh environments. Herein, we proposed a balanced "cocktail optimized" electrolyte by manipulating solvated and anionic species. The dual salt/dual solvent electrolyte simultaneously achieves low bulk impedance and low interfacial impedance, while also demonstrating improved Li reversibility and oxidation stability. The tailored solvation structure encourages the breakdown of anions, leading to the formation of inorganic-rich interphases at both the cathode and Li-anode, which enables a uniform plating-stripping of Li while maintaining exceptional voltage resilience on the cathode. Moreover, NO3 - ions preferentially adsorb onto the cathode surface within the inner Helmholtz plane, shielding the easily-oxidized non-solvating solvent molecules, a phenomenon referred to as the "shielding effect", thus inhibiting side oxidation reactions. Consequently, the anion-derived interface chemistry contributes to the dendrite-free Li deposition with a high CE of 99.45%, a stable cycling of Li||NCM523 battery with 85% capacity retention after 150 cycles, and a superior low-temperature discharge performance at -30 degrees C with a capacity retention of 68.2%. This work sheds light on an encouraging electrolyte strategy for stable LMBs in a wide-temperature range.
Keyword :
Cocktail electrolyte Cocktail electrolyte Dual salt/dual solvent electrolyte Dual salt/dual solvent electrolyte Lithium metal batteries Lithium metal batteries Low-temperature Low-temperature Strong-weak coupling Strong-weak coupling
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GB/T 7714 | Liu, Yongchuan , Shen, Jie , Hu, Guolin et al. Stable low-temperature lithium metal batteries with dendrite-free ability enabled by electrolytes with cooperative Li plus -solvation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 503 . |
MLA | Liu, Yongchuan et al. "Stable low-temperature lithium metal batteries with dendrite-free ability enabled by electrolytes with cooperative Li plus -solvation" . | CHEMICAL ENGINEERING JOURNAL 503 (2025) . |
APA | Liu, Yongchuan , Shen, Jie , Hu, Guolin , Fang, Guihuang , Chen, Yuanqiang , Zhang, Xiangxin et al. Stable low-temperature lithium metal batteries with dendrite-free ability enabled by electrolytes with cooperative Li plus -solvation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 503 . |
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自由基在有机化学中扮演着至关重要的角色,与碳正离子、碳负离子、卡宾等高能活性中间体共同构筑了有机化学的基石.氧中心自由基,作为自由基家族中一类特殊且重要的活性中间体,其独特性质不仅赋予其引发一系列有机反应的能力,更在医疗健康与环境保护等领域引发了广泛而深入的研究.本文旨在深入剖析并重点介绍四种氧中心自由基——三重态氧气(·O2·)、羟基自由基(HO·)、超氧自由基阴离子(O2-·)以及烷氧类自由基(RO·)的物理化学本质特性和多样化的合成策略,并进一步阐述其在有机合成领域中的具体应用实例与广泛影响.
Keyword :
氧中心自由基 氧中心自由基 活性中间体 活性中间体 绿色化学 绿色化学 自由基 自由基
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GB/T 7714 | 胡雨潇 , 黄冰冰 , 常文举 et al. 氧中心自由基 [J]. | 大学化学 , 2025 , 40 (2) : 216-227 . |
MLA | 胡雨潇 et al. "氧中心自由基" . | 大学化学 40 . 2 (2025) : 216-227 . |
APA | 胡雨潇 , 黄冰冰 , 常文举 , 沈杰 . 氧中心自由基 . | 大学化学 , 2025 , 40 (2) , 216-227 . |
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Dysregulation of anion transport is implicated in a range of diseases, including congenital myotonia, cystic fibrosis, and hereditary renal lithiasis. While natural anion channels exhibit highly complex and intricate structures, the development of structurally simpler artificial channels holds promise for advancing the understanding of anion transport mechanisms and offering novel therapeutic approaches. Among emerging strategies, the use of side chain-side chain interactions to construct artificial anion channels has shown significant potential, particularly through the application of flexible hydrocarbon side chains to facilitate pore formation. Building on this concept, we introduce a novel scaffold-the dibenzo-12-crown-4 group-which unexpectedly acts as a pore-forming enhancer, rather than a cation transporter. By strengthening side chain-side chain interactions, this group promotes the formation of sizable pores within lipid bilayers, selectively and efficiently transporting anions, rather than cations. Notably, channel A10 exhibits a remarkable high Cl-/K+ selectivity ratio of 17 while showcasing a distinct hierarchy in anion conductivity: ClO4- > I- > NO3- > Br- > Cl-.
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GB/T 7714 | Fan, Jisen , Xu, Yingxue , Shen, Jie et al. Dibenzo-12-crown-4 group as a pore-forming enhancer for anion transport [J]. | ORGANIC CHEMISTRY FRONTIERS , 2025 . |
MLA | Fan, Jisen et al. "Dibenzo-12-crown-4 group as a pore-forming enhancer for anion transport" . | ORGANIC CHEMISTRY FRONTIERS (2025) . |
APA | Fan, Jisen , Xu, Yingxue , Shen, Jie , Chang, Wenju , Zeng, Huaqiang . Dibenzo-12-crown-4 group as a pore-forming enhancer for anion transport . | ORGANIC CHEMISTRY FRONTIERS , 2025 . |
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Artificial gated ion channels are still rare, particularly when compared to their many ungated counterparts. In this work, we introduce a photoresponsive azobenzene group and an ion-binding crown ether group into a doubly amidated monopeptide scaffold having a capacity to self-assemble into a one-dimensionally aligned, doubly H-bonded columnar structure. While the directionally aligned crown ethers provide the structural basis for transporting K+ ions with high selectivity, the similarly aligned azobenzene groups offer the system light modulation, concurrently with surprisingly enhanced ion transport properties with respect to its parent molecule having an octyl side chain. Upon 365 nm UV irradiation to convert trans-azobenzene to its cis-form, the ion transport activity drops drastically by >60% (from 0.98 to 2.60 mol% relative to lipids) in the EC50 value, with fractional ion transport activity-derived K+/Na+ selectivity substantially decreasing by >70% (from 23.6 to 6.3). The activity and selectivity are fully restored after alternating exposure to visible light at 455 nm.
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GB/T 7714 | Zeng, Landley Ziluo , Li, Zhongyan , Xu, Ying et al. A light-regulated, exceptionally active and selective artificial potassium channel [J]. | ORGANIC CHEMISTRY FRONTIERS , 2024 , 11 (21) : 6150-6158 . |
MLA | Zeng, Landley Ziluo et al. "A light-regulated, exceptionally active and selective artificial potassium channel" . | ORGANIC CHEMISTRY FRONTIERS 11 . 21 (2024) : 6150-6158 . |
APA | Zeng, Landley Ziluo , Li, Zhongyan , Xu, Ying , Shen, Jie , Gong, Bing , Chang, Wenju . A light-regulated, exceptionally active and selective artificial potassium channel . | ORGANIC CHEMISTRY FRONTIERS , 2024 , 11 (21) , 6150-6158 . |
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This review is the first to focus on transmembrane transporters derived from aromatic foldamers, with most studies reported over the past decade. These foldamers have made significant strides in mimicking the essential functions of natural ion channel proteins. With their aromatic backbones rigidified by intramolecular hydrogen bonds or differential repulsive forces, this innovative family of molecules stands out for its structural diversity and functional adaptability. They achieve efficient and selective ion and molecule transport across lipid bilayers via carefully designed helical structures and tunable large cavities. Recent developments in this field highlight the transformative potential of foldamers in therapeutic applications and biomaterial engineering. Key advances include innovative molecular engineering strategies that enable highly selective ion transport by fine-tuning structural and functional attributes. Specific modifications to macrocyclic or helical foldamer structures have allowed precise control over ion selectivity and transport efficiency, with notable selectivity for K+, Li+, H+ and water molecules. Although challenges remain, future directions may focus on more innovative molecular designs, optimizing synthetic methods, improving membrane transport properties, integrating responsive designs that adapt to environmental stimuli, and fostering interdisciplinary collaborations. By emphasizing the pivotal role of aromatic foldamers in modern chemistry, this review aims to inspire further development, offering new molecular toolboxes and strategies to address technological and biological challenges in chemistry, biology, medicine, and materials science.
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GB/T 7714 | Zhang, Danyang , Chang, Wenju , Shen, Jie et al. Aromatic foldamer-derived transmembrane transporters [J]. | CHEMICAL COMMUNICATIONS , 2024 , 60 (92) : 13468-13491 . |
MLA | Zhang, Danyang et al. "Aromatic foldamer-derived transmembrane transporters" . | CHEMICAL COMMUNICATIONS 60 . 92 (2024) : 13468-13491 . |
APA | Zhang, Danyang , Chang, Wenju , Shen, Jie , Zeng, Huaqiang . Aromatic foldamer-derived transmembrane transporters . | CHEMICAL COMMUNICATIONS , 2024 , 60 (92) , 13468-13491 . |
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In sharp contrast to numerous artificial potassium channels developed over the past decade, the study of artificial lithium-transporting channels has remained limited. We demonstrate here the use of an interesting class of polymers with intrinsic microporosity (PIM) for constructing artificial lithium channels. These PIM-derived lithium channels show exceptionally efficient (gamma(+)(Li)>40 pS) and highly selective transport of Li+ ions, with selectivity factors of>10 against both Na+ and K+. By simply adjusting the initial reaction temperature, we can tune the transport property in a way that PIMs synthesized at initial reaction temperatures of 60 degrees C and 80 degrees C exhibit improved transport efficiency and selectivity, respectively, in the dioleoyl phosphatidylcholine membrane.
Keyword :
Lithium Ion Channels Lithium Ion Channels Lithium Transport Lithium Transport Microporous Polymers Microporous Polymers Supramolecular Chemistry Supramolecular Chemistry Transmembrane Transport Transmembrane Transport
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GB/T 7714 | Gou, Fei , Wang, Qiuting , Yang, Zihong et al. Artificial Lithium Channels Built from Polymers with Intrinsic Microporosity [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 64 (7) . |
MLA | Gou, Fei et al. "Artificial Lithium Channels Built from Polymers with Intrinsic Microporosity" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 7 (2024) . |
APA | Gou, Fei , Wang, Qiuting , Yang, Zihong , Chang, Wenju , Shen, Jie , Zeng, Huaqiang . Artificial Lithium Channels Built from Polymers with Intrinsic Microporosity . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 64 (7) . |
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Membrane-active molecular machines represent a recently emerging, yet important line of expansion in the field of artificial transmembrane transporters. Their hitherto demonstrated limited types (molecular swing, ion fishers, shuttlers, rotors, etc.) certainly call for new inspiring developments. Here, we report a very first motorized ion-transporting carrier-type transporter, i.e., a modularly tunable, light-powered propeller-like transporter derived from Feringa's molecular motor for consistently boosting transmembrane ion transport under continuous UV light irradiation. Based on the EC50 values, the molecular propeller-mediated ion transport activities under UV light irradiation for 300 s are 2.31, 1.74, 2.29, 2.80, and 2.92 times those values obtained without irradiation for Li+, Na+, K+, Rb+, and Cs+ ions, respectively, with EC50 value as low as 0.71 mol % for K+ ion under light irradiation.
Keyword :
ion transport ion transport molecularmachine molecularmachine molecular motor molecular motor molecular propeller molecular propeller supramolecular chemistry supramolecular chemistry
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GB/T 7714 | Deng, Shaowen , Li, Zhongyan , Yuan, Lin et al. Light-Powered Propeller-like Transporter for Boosted Transmembrane Ion Transport [J]. | NANO LETTERS , 2024 , 24 (35) : 10750-10758 . |
MLA | Deng, Shaowen et al. "Light-Powered Propeller-like Transporter for Boosted Transmembrane Ion Transport" . | NANO LETTERS 24 . 35 (2024) : 10750-10758 . |
APA | Deng, Shaowen , Li, Zhongyan , Yuan, Lin , Shen, Jie , Zeng, Huaqiang . Light-Powered Propeller-like Transporter for Boosted Transmembrane Ion Transport . | NANO LETTERS , 2024 , 24 (35) , 10750-10758 . |
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For compounds each containing a phenylalanine moiety with its two ends amidated to have a 15-crown-5 unit and an alkyl chain, a simple tuning of the alkyl chain length delivered a K+-selective channel with a record-high K+/Na+ selectivity of 20.1.
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GB/T 7714 | Jin, Lei , Sun, Chang , Li, Zhongyan et al. A K+-selective channel with a record-high K+/Na+ selectivity of 20.1 [J]. | CHEMICAL COMMUNICATIONS , 2023 , 59 (24) : 3610-3613 . |
MLA | Jin, Lei et al. "A K+-selective channel with a record-high K+/Na+ selectivity of 20.1" . | CHEMICAL COMMUNICATIONS 59 . 24 (2023) : 3610-3613 . |
APA | Jin, Lei , Sun, Chang , Li, Zhongyan , Shen, Jie , Zeng, Huaqiang . A K+-selective channel with a record-high K+/Na+ selectivity of 20.1 . | CHEMICAL COMMUNICATIONS , 2023 , 59 (24) , 3610-3613 . |
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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 & ANGS; 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.
Keyword :
Foldamers Foldamers H-Bonds H-Bonds Lithium Channels Lithium Channels Organic Nanotubes Organic Nanotubes Supramolecular Chemistry Supramolecular Chemistry
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GB/T 7714 | Shen, Jie , Deepa, R. , Li, Zhongyan et al. Sulfur-Containing Foldamer-Based Artificial Lithium Channels [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (39) . |
MLA | Shen, Jie et al. "Sulfur-Containing Foldamer-Based Artificial Lithium Channels" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 39 (2023) . |
APA | Shen, Jie , Deepa, R. , Li, Zhongyan , Oh, Hyeonji , Behera, Harekrushna , Joshi, Himanshu et al. Sulfur-Containing Foldamer-Based Artificial Lithium Channels . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (39) . |
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