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学者姓名：沈杰
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Abstract ：
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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Artificial photoresponsive transport systems are particularly intriguing because they offer the potential for precise spatio-temporal control, rapid response times and minimal toxicity associated with the light. We report here a controllable, photoresponsive, ion-transporting carrier, achieving controllability through a photoregulated β-cyclodextrin (β-CD)-azobenzene host-guest complex. In this complex, a lipid-anchored β-CD serves as the launch base, tightly immobilizing through host-guest interactions the otherwise freely moving trans-transporter derived from a crown ether-modified trans-azobenzene motif, but rapidly releasing most of it upon 365 nm UV irradiation that converts transporter to its cis-configuration. The launched cis-transporter functions well as a highly efficient potassium transporter, delivering a low EC50 value of 1.51 μM and a drastic transport activity enhancement by ~ 400% relative to the base-bound trans-transporter (EC50 = 7.46 μM), with on-off activities repeatedly regulated by light. In the absence of the base, the on-off activities between cis- and trans-transporters however differ by only 80% (1.35 μM vs 2.45 μM). © The Author(s) 2025.
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| GB/T 7714 | Li, Z. , Yuan, L. , Chang, W. et al. A controllable photoresponsive potassium transporter [J]. | Nature Communications , 2025 , 16 (1) . |
| MLA | Li, Z. et al. "A controllable photoresponsive potassium transporter" . | Nature Communications 16 . 1 (2025) . |
| APA | Li, Z. , Yuan, L. , Chang, W. , Liu, J. , Shen, J. , Zeng, H. . A controllable photoresponsive potassium transporter . | Nature Communications , 2025 , 16 (1) . |
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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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The microenvironment of diabetic wounds is exceptionally complex, characterized notably by persistent bacterial infections and the excessive production of reactive oxygen species (ROS). Traditional treatment methods often fall short of achieving ideal results. Consequently, there is an urgent need to develop and implement more advanced and efficient treatment strategies to effectively address the complexity and recalcitrance of diabetic wounds. This study pioneers a novel approach by fabricating a silk fibroin-based nonwoven dressing (SF-Ag-HCA) under neutral conditions, integrating silver ions with dihydrocaffeic acid-modified silk fibroin. Uniquely, this dressing achieves dual functionality: exceptional antibacterial efficacy against common pathogens (E. coli, S. aureus, P. aeruginosa) and robust ROS-scavenging capabilities, effectively mitigating oxidative stress and promoting immune homeostasis. The SF-Ag-HCA dressing not only surpasses conventional materials in regulating the wound microenvironment but also accelerates re-epithelialization and collagen deposition. Animal studies further validate its superior performance in healing diabetic and infected wounds compared to commercial alternatives. This innovative dressing represents a significant advancement in wound care, offering an integrated, cost-effective solution tailored for complex chronic wound management.
Keyword ：
antibacterial antibacterial diabetic wound healing diabetic wound healing reactive oxygen species reactive oxygen species silk non-woven fabrics silk non-woven fabrics
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| GB/T 7714 | Zhou, Zhao-Xi , Chen, Yanbin , Li, Jingyi et al. Silk Nonwoven Fabric-Based Dressing with Antibacterial and ROS-Scavenging Properties for Modulating Wound Microenvironment and Promoting Diabetic Wound Healing [J]. | ADVANCED HEALTHCARE MATERIALS , 2025 , 14 (11) . |
| MLA | Zhou, Zhao-Xi et al. "Silk Nonwoven Fabric-Based Dressing with Antibacterial and ROS-Scavenging Properties for Modulating Wound Microenvironment and Promoting Diabetic Wound Healing" . | ADVANCED HEALTHCARE MATERIALS 14 . 11 (2025) . |
| APA | Zhou, Zhao-Xi , Chen, Yanbin , Li, Jingyi , Shen, Jie , Zeng, Huaqiang . Silk Nonwoven Fabric-Based Dressing with Antibacterial and ROS-Scavenging Properties for Modulating Wound Microenvironment and Promoting Diabetic Wound Healing . | ADVANCED HEALTHCARE MATERIALS , 2025 , 14 (11) . |
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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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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 , 12 (11) : 3409-3416 . |
| MLA | Fan, Jisen et al. "Dibenzo-12-crown-4 group as a pore-forming enhancer for anion transport" . | ORGANIC CHEMISTRY FRONTIERS 12 . 11 (2025) : 3409-3416 . |
| 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 , 12 (11) , 3409-3416 . |
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Water transport across biological membranes is essential for life, facilitated by water channel proteins like aquaporins (AQPs). Drawing inspiration from these natural systems, artificial water channels (AWCs) have emerged as transformative tools for advancing industrial and environmental applications. Herein, we report the design and comprehensive characterization of a groundbreaking class of AWCs, derived from unprecedented butterfly-shaped aromatic folding synthons, carefully engineered to emulate the functional attributes of natural AQPs. These foldamers, with their intricate helical architectures, exhibit exceptional water transport performance. Remarkably, the highest-performing AWC achieves an ultrafast water transport rate of 2.6 × 1010 H2O s−1 per channel—2.4 times the efficiency of AQP1—without the need for lipid anchors to preserve its functional orientation within phospholipid bilayers, while effectively excluding salts such as NaCl and KCl, along with protons. This work presents an ideal bio-inspired, high-performance artificial alternative to natural systems, demonstrating the remarkable potential of foldamer-based AWCs as next-generation solutions for tackling critical challenges in water purification and desalination. © 2025 Wiley-VCH GmbH.
Keyword ：
Artificial water channels Artificial water channels Proton rejection Proton rejection Salt rejection Salt rejection Supramolecular chemistry Supramolecular chemistry Water desalination Water desalination
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| GB/T 7714 | Shen, J. , Zhang, Y. , Jin, Y. et al. Butterfly-Shaped Folding Synthons for Designing Superselective and Ultrapermeable Artificial Water Channels [J]. | Angewandte Chemie - International Edition , 2025 . |
| MLA | Shen, J. et al. "Butterfly-Shaped Folding Synthons for Designing Superselective and Ultrapermeable Artificial Water Channels" . | Angewandte Chemie - International Edition (2025) . |
| APA | Shen, J. , Zhang, Y. , Jin, Y. , Zhou, Z.-X. , Xu, Y. , Chang, W. et al. Butterfly-Shaped Folding Synthons for Designing Superselective and Ultrapermeable Artificial Water Channels . | Angewandte Chemie - International Edition , 2025 . |
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Artificial ion channels with specific organelle-targeting capabilities have been scarcely investigated. Here, we report the first-in-class mitochondria-targeting anion channels derived from a structurally simple tetrabenzylphosphonium framework, in stark contrast to its phenyl-based counterpart, which lacks anion transport activity. Structural and computational analyses underscore the critical role of the methylene (CH2) linkers in the benzyl groups. These CH2 units reduce positive charge delocalization to enhance sigma-hole-anion interactions, while also enabling H-atoms from both the CH2 linkers and aromatic rings to cooperatively form multiple C & horbar;H & ctdot;anion H & horbar;bonds. In further conjunction with the rigid benzene rings, they help create sufficient spatial voids to accommodate anion translocation, collectively facilitating and energizing the anion transport process. Among the series studied, those bearing methyl and tert-butyl substituents exhibit the highest transport activity via a channel mechanism, with a conductance value as high as 26.5 +/- 0.8 pS. Furthermore, leveraging the cationic nature of the quaternary phosphonium center, this family of anion channels readily achieves targeted mitochondrial localization, demonstrating potent anticancer activity, with IC50 values ranging from 1.42 to 3.04 mu M across three cancer cell lines.
Keyword ：
Artificial anion channels Artificial anion channels Chloride transport Chloride transport Self-assembly Self-assembly Supramolecular chemistry Supramolecular chemistry Tetrabenzylphosphonium Tetrabenzylphosphonium
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| GB/T 7714 | Gou, Fei , Huangfu, Xinlei , Wang, Qiuting et al. Dual-Function Tetrabenzylphosphonium Groups as Mitochondria-Targeting Artificial Anion Channels [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (36) . |
| MLA | Gou, Fei et al. "Dual-Function Tetrabenzylphosphonium Groups as Mitochondria-Targeting Artificial Anion Channels" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 36 (2025) . |
| APA | Gou, Fei , Huangfu, Xinlei , Wang, Qiuting , Yang, Zihong , Yuan, Xiyu , Chang, Wenju et al. Dual-Function Tetrabenzylphosphonium Groups as Mitochondria-Targeting Artificial Anion Channels . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (36) . |
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Artificial proton channels exhibiting high selectivity remain largely unexplored, with only two such systems recently reported. Inspired by the DNA duplex's iconic helical structure, we present here a novel strategy for designing a molecular-scale staircase configuration. The resulting molecular staircase (MS), predominantly linear in shape, consists of pyridine units linked by hydrazide groups, with backbone rigidity enhanced by intramolecular H-bonding. This MS incorporates up to five proton-transporting motifs, demonstrating remarkable efficacy as a proton-conducting channel within lipid bilayer membranes. Our findings indicate that the MS exhibits high proton transport activity (EC50 of 0.31 mol%, relative to lipids) and significant selectivity for protons, with selectivity values of 160.3 for K+, 90.5 for Na+, and 3.5 for Cl⁻. These results underscore the potential of the MS and its variants as a highly selective and efficient proton channel, advancing the field of artificial ion transport systems. © 2025 Wiley-VCH GmbH.
Keyword ：
Molecular staircase Molecular staircase Proton channels Proton channels Proton transport Proton transport Transmembrane transport Transmembrane transport
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| GB/T 7714 | Xu, J. , Chen, Y. , Wang, J. et al. A Molecular Staircase Built from Hydrazide-Linked Pyridines as an Artificial Proton Channel [J]. | Angewandte Chemie - International Edition , 2025 . |
| MLA | Xu, J. et al. "A Molecular Staircase Built from Hydrazide-Linked Pyridines as an Artificial Proton Channel" . | Angewandte Chemie - International Edition (2025) . |
| APA | Xu, J. , Chen, Y. , Wang, J. , Chang, W. , Shen, J. , Zeng, H. . A Molecular Staircase Built from Hydrazide-Linked Pyridines as an Artificial Proton Channel . | Angewandte Chemie - International Edition , 2025 . |
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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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