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  • Bin Liu, Bo Chu, Lixun Zhu, Haoke Zhang, Wang-Zhang Yuan, Zheng Zhao, Wen-Ming Wan, Xing-Hong Zhang
    Chinese Chemical Letters. 2023, 34(5): 107909-.

    Clusteroluminescence (CL) materials, as an emerging class of luminescent materials with unique photophysical properties, have received increasing attention owing to their great theoretical significance and potential for biological applications. Although much progress has been made in the design, synthesis and application of CL materials, there is still a big challenge in the emission mechanism. So far, through-space interaction has been proposed as the preliminary mechanism of the corresponding clusterization-triggered emission (CTE) effect, but a systematic theory is still needed. This review summarizes the current mechanistic understanding of CL materials including organic/inorganic small molecules, and polymers with/without isolated aromatic structures. In addition, some strategies to achieve high quantum yield, adjustable emission color, and persistent room temperature phosphorescence in CL materials are also summarized. At last, a perspective of the mechanism and application of CL materials are demonstrated, which inspire the researchers working on the development of new kinds of functional materials.

  • Jin Li, Qinglong Qiao, Yiyan Ruan, Ning Xu, Wei Zhou, Guixin Zhang, Jingli Yuan, Zhaochao Xu
    Chinese Chemical Letters. 2023, 34(5): 108266-.

    Protein self-labeling tags achieve selective fusion and labeling of target proteins through genetic coding technology, but require exogenous fluorescent probes with fluorogenicity for protein tag binding to have the performance of wash-free fluorescence imaging in live cells. In this paper, we reported a fluorogenic probe 1 capable of ratiometric fluorescence recognition of SNAP-tag proteins. In this probe, the O6-benzylguanine derivative of 3–hydroxy-1,8-naphthalimide underwent a selective covalent linkage reaction with SNAP-tag protein. The hydroxyl group on the naphthalimide fluorophore formed a hydrogen bond with the functional group near the protein cavity. The excited state proton transfer occurred after illumination, to obtain the ratio fluorescence signal from blue emission to red emission, realizing the wash-free fluorescence imaging of the target proteins.

  • Tao Feng, Fengting Li, Xiaojun Hu, Ying Wang
    Chinese Chemical Letters. 2023, 34(5): 107862-.

    Electrocatalytic nitrate reduction to ammonia (NRA) under ambient conditions is significant for carbon-neutral synthetic fuels. Nevertheless, the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand challenge. Herein, NbWO6 nanosheets with oxygen vacancy (NbWO6-x) was demonstrated via thermal treatment and exfoliation with NH3 selectivity of 86.8% and Faradaic efficiency of 85.7% toward NRA. 1H nuclear magnetic resonance spectra coupled with 15N isotope labeling experiments proved that NH3 originated from NO3. The function of oxygen vacancy was revealed by computational studies in NRA. Moreover, the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry (DEMS). This work provides a selective NH3 generation strategy to decarbonize the energy-chemical sector, bridging the gap between batteries and biofuels.

  • Tianran Lin, Chunsuo Tian, Ying Sun, Shendong Liu, Di Wang, Li Hou, Shulin Zhao
    Chinese Chemical Letters. 2023, 34(5): 107864-.

    Information-carrying capacity has become an important factor in the development of encryption and anti-counterfeiting. Herein, a hydrogen-bonded organic framework (HOF-PyTTA) was developed as novel anti-counterfeiting ink without rare metals and a smartphone-based APP was written for encryption and anti-counterfeiting. We found that the fluorescence of HOF-PyTTA can be quenched by Fe3+ ions and recovered by the addition of ascorbic acid. And the fluorescence of HOF-PyTTA can be enhanced by the increasing concentrations of ethanol. Based on these stimulus-response properties, four anti-counterfeiting models with gradually increased security were studied. Mode one was printed by HOFs ink and decrypted by UV light. Mode two was based on HOF-PyTTA and CsPbBr3 inks (or HOF-PyTTA-Fe3+) which are used to separately print the genuine and pirated information. A decryption reagent was applied to get the genuine information. Furthermore, we successfully construct a dynamic information encryption anti-counterfeiting model using a fluorescence array in combination with an information encryption anti-counterfeiting APP. The circular array is printed by several concentrations of HOF-PyTTA ink and different RGB thresholds are set with the help of the information encryption anti-counterfeiting APP, to obtain distinct encrypted anti-counterfeiting information, thus accomplishing a high information-carrying capacity.

  • Weipan Xu, Zheng Ma, Geetika Dhanda, Jayanta Haldar, Hexin Xie
    Chinese Chemical Letters. 2023, 34(5): 107847-.

    The expression of β-lactamase, particularly metallo-β-lactamase (MBL) in bacteria has caused significant resistance to clinically important β-lactam antibiotics, including life-saving carbapenems. Antimicrobial peptides (AMPs) have emerged as promising therapeutic agents to combat antibiotic resistance. However, the cytotoxic AMPs has been one of the major concerns for their applications in clinical practice. Herein, we report a novel cephalosporin-caged AMP, which shows significantly reduced cytotoxicity, hemolytic activity, and antibacterial activity but turns highly active against bacteria upon specific hydrolysis by the antimicrobial resistance-causative β-lactamase. Further investigations demonstrate this β-lactamase-activatable AMP selectively inactivates resistant bacterial pathogens over susceptible bacteria. This strategy should be applicable to other AMPs as a potential solution for the treatment of infectious diseases caused by β-lactamase-expressing pathogenic bacteria.

  • Xin Wang, Zhichuan Wang, Zhenjian Li, Kai Sun
    Chinese Chemical Letters. 2023, 34(5): 108045-.

    The XCF3 groups (X = O, S, Se) play an increasingly important role in modern organic chemistry due to their unique electronegativity, lipophilic nature, metabolic stability, and bioavailability. Heterocyclic compounds are important scaffolds in many bioactive compounds and drugs. The incorporation of XCF3 groups into heterocyclic compounds can change their physicochemical and biological properties, which injects new vitality into the application of heterocyclic compounds in many fields such as organic chemistry, the pharmaceutical chemistry, and life sciences. In this paper, the recent progress in the synthesis of F3CX-containing heterocycles is reviewed, and the application scope and mechanism of some reactions are discussed.

  • Yefei Jiang, Zhiyong Zeng, Jianhua Yao, Ying Guan, Peipei Jia, Xiaoli Zhao, Lin Xu
    Chinese Chemical Letters. 2023, 34(5): 107966-.

    Alzheimer's disease is a neurodegenerative disease that signals for excess β-amyloid (Aβ) aggregation. Although people have made great attempts to control the aggregation of Aβ, no effective medications have been produced yet. Due to its excellent temporal and spatial selectivity, photodynamic treatment has been gradually employed and interfered in the aggregation process of Aβ, with some achievement. To enhance the research and application of photodynamic therapy in Alzheimer's disease, this paper reviews the progress of small-molecule photosensitizers in the treatment of Alzheimer's disease in recent years and outlines existing tactics and potential obstacles.

  • Ao Yu, Wangtao Long, Longtao Zhu, Yinan Zhao, Ping Peng, Fang-Fang Li
    Chinese Chemical Letters. 2023, 34(5): 107860-.

    The oxygen reduction reaction (ORR), an important process in Zn-air batteries (ZABs), shows sluggish reaction kinetics, which significantly impairs the further improvement of battery performance. Thus, rationally designing cathodic catalysts for ZABs has drawn sufficient attention. We herein synthesize and characterize Fe/N/F-tridoped CNTs (FeNFCs) by annealing the postsynthesized trifluoroacetic anhydride-modified Fe-MIL-88B-NH2 nanocrystals with melamine at high temperature in a N2 atmosphere. Benefiting from the Fe/N/F element doping, high specific surface area, and CNT structure, the FeNFC800 catalyst prepared at 800 ℃ exhibits a preferable half-wave potential of 0.829 V vs. RHE. The Zn-air battery equipped with FeNFC800 shows a high open-circuit voltage of 1.47 V, a gratifying peak power density of 196 mW/cm2, and extraordinary long-term stability, outperforming the benchmark 20% Pt/C.

  • Kaiya Wang, Minzan Zuo, Tao Zhang, Huilan Yue, Xiao-Yu Hu
    Chinese Chemical Letters. 2023, 34(5): 107848-.

    Pillar[5]arene–modified amphiphilic peptides with varying numbers of guanidiniocarbonylpyrrol (GCP) moieties have been successfully synthesized, which can self-assemble to multivalent cationic superstructures in aqueous solutions. These assembled peptides can condense DNA into various compact multimolecular aggregates to achieve successful intracellular DNA delivery and demonstrate great potential for gene transfection. Transfection efficiencies of the self-assembled superstructures have been evaluated in vitro with HeLa and HEK 293T cells. We demonstrate that GCP moiety could enhance the cell transfection ability, owing to its excellent binding towards cytomembrane. It was also found that subtle structure difference in peptides 2 and 3 could result in distinct transfection efficacy, which makes it possible to gain an in-depth understanding of their structure-activity relationship. This work presents a good example of rational structural design in achieving effective gene transfection vectors.

  • Manuel Petroselli, Yong-Qing Chen, Ming-Kai Zhao, Julius Rebek, Yang Yu
    Chinese Chemical Letters. 2023, 34(5): 107834-.

    Binding of non-activated alkyl halides (220) in water-soluble cavitand (1) through supramolecular forces is here reported, with emphasis on the role of size and polarizability of the halogen atom in the formation of intramolecular C-H hydrogen bonds in confined spaces. Rare reverse affinity in water (RI < RBr < RCl) is surprisingly observed for the more water-soluble short alkyl halides in dynamic open-ended containers. Competitive bindings and theoretical calculations confirm the unusual selectivity and the presence of C-H hydrogen bonds in non-activated systems for the first time, pointing out the importance and effect of subtle forces on molecular recognition in confined spaces.

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