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  • Shunshun Jiang, Ji Zhang, Jing Wang, Shan-Tao Zhang
    Chinese Chemical Letters. 2024, 35(7): 108955-.

    The rapid development of high-power and pulsed-power techniques inspires extensive investigates on high-performance ceramic-based capacitors. However, the low recoverable energy density (Wrec) hampers their wider applications. Herein, the non-stoichiometric Bi0.5Na0.5TiO3-based ceramics were designed and studied. The proper introduction of oxygen vacancies facilitated activating defect dipole, giving rise to reduced remanent polarization. Consequently, the optimal composition exhibited an exceptional high Wrec of 8.3 J/cm3, a high efficiency of 85%, and excellent anti-fatigue and thermal reliability. This work provides an efficient approach to explore ceramic capacitors with high capacitive energy storage performances.

  • Luyu Zhang, Zirong Dong, Shuai Yu, Guangyue Li, Weiwen Kong, Wenjuan Liu, Haisheng He, Yi Lu, Wei Wu, Jianping Qi
    Chinese Chemical Letters. 2024, 35(7): 109101-.

    This research aims to develop a non-invasive strategy for small interfering RNA (siRNA) nasal delivery based on ionic liquids (ILs) and cationic lipid (2,3-dioleoyloxy-propyl)-trimethylammonium-chloride (DOTAP). Other than the classical role of penetration enhancer, ILs also acted as superior solvents to simultaneously load siRNA and DOTAP, forming siRNA-DOTAP-ILs (siRNA-DILs) formulations. During nasal mucosa penetration, DOTAP and ILs components self-assembled into cationic lipid nanocomplexes to load siRNA for enhanced in situ transfection. The siRNA-DILs demonstrated resistance against RNase, significant mucosa penetration, prolonged nasal retention, and satisfying gene-silencing efficacy at lower dosage. Meanwhile, DILs were also able to deliver KCa3.1-targeted siRNA effectively for the treatment of allergic rhinitis in rat model by nasal route. Thus, DILs have great potentials to deliver biological macromolecules across nasal mucosa by in situ dynamic self-assembly.

  • Yu Deng, Yan Liu, Yonghui Deng, Jinsheng Cheng, Yidong Zou, Wei Luo
    Chinese Chemical Letters. 2024, 35(7): 108898-.

    Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment, and thus it is distinctly meaningful to monitor benzene series with quickly, real-time and efficient technique. Herein, novel sulfur-doped mesoporous WO3 materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering, which possessed highly crystallized frameworks, high specific surface area (40.9–63.8 m2/g) and uniform pore size (~18 nm). Benefitting from abundant oxygen vacancy and defects via S-doping, the tailored mesoporous S/mWO3 exhibited excellent benzene sensing performance, including high sensitivity (50 ppm vs. 48), low detection limit (ca. 500 ppb), outstanding selectivity and favorable stability. In addition, the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces. It provides brand-new approach to design sensitive materials with multiple reaction sites.

  • Jingting Wang, Yuanyuan Chen, Linlin Han, Shasha Xia, Xingyao Zhang, Peng Xue, Yuejun Kang, Jian Ming, Zhigang Xu
    Chinese Chemical Letters. 2024, 35(7): 109029-.

    Anti-inflammatory drugs targeting inflammatory bowel disease (IBD) have attracted considerable attention but still face low therapeutic outcomes and frequent side effects. Astaxanthin (ATX), a natural ketone, possesses potent antioxidant and anti-inflammatory properties. However, it faces problems such as poor water solubility, photothermal instability, and low bioavailability. Here, we employed a supramolecular encapsulation strategy to create a nanoscale oral delivery system for ATX (referred to as FC-ATX NPs) by coupling fucoidan (FUC) with chitosan oligosaccharides (COS). The obtained FC-ATX NPs exhibited a particular "bean pod" structure with uniform size, good encapsulation efficiency, excellent physical and chemical stability, pH-triggered intestinal targeted slow-release properties, and potent antioxidant capacity. In vitro cell culture experiments showed that FC-ATX NPs promoted cellular uptake and scavenged excessive intracellular reactive oxygen species (ROS). In mouse models of colitis, FC-ATX NPs enhanced the drug absorption of intestinal epithelial cells and effectively accumulated at the site of inflammation. This work provides an efficient approach to enhance the bioavailability of ATX and has excellent application potential as an oral targeted delivery system for colitis therapy.

  • Xian-Fa Jiang, Chongyun Shao, Zhongwen Ouyang, Zhao-Bo Hu, Zhenxing Wang, You Song
    Chinese Chemical Letters. 2024, 35(7): 109011-.

    Qubit, as the basic unit of quantum operations, has at least two quantum states for superposition. Diamond itself has no superimposable quantum states, but after injecting N atoms, the resulted nitrogen-vacancy centers form excellent-performance qubits. For the same purpose, we can also obtain qubits by modifying the matrix without effective quantum states. HKUST-1 ({Cu3(BTC)2(H2O)3}, BTC = 1,3,5-benzene-tricarboxylate) with S = 0 ground state is electron paramagnetic resonance (EPR) silent, so it is not a qubit candidate. However, the spontaneously hydrolyzed HKUST-1 produces dilute uncoupled Cu ions with S = 1/2. In this paper, we utilized the hydrolysis products of HKUST-1 to obtain qubits and assembled a core-shell structural HKUST-1@ZIF-8 by ZIF-8 ({Zn(mim)2}, mim = 2-methylimidazole) coated over HKUST-1 for controlling the hydrolysis. The experimental results clearly show that the qubits come from hydrolyzed Cu ions. Furthermore, the dilute uncoupled Cu ions in this assembly can effectively reduce the decoherence of qubits. The EPR studies show that the T2 of this compound is 1067 ns at 10 K.

  • Xiaoning Li, Quanyu Shi, Meng Li, Ningxin Song, Yumeng Xiao, Huining Xiao, Tony D. James, Lei Feng
    Chinese Chemical Letters. 2024, 35(7): 109021-.

    Mercury ion (Hg2+), as one of the most toxic heavy metal ions, accumulates easily in the environment, which can generate potential hazards to the ecosystem and human health. To effectively detect and remove Hg2+, we fabricated four types of carbon dots (CDs) using carboxymethyl nanocellulose as a carbon source doped with different elements using a hydrothermal method. All the CDs exhibited a strong fluorescence emission, excitation-dependent emission and possessed good water dispersibility. Moreover, the four fluorescent CDs were used for Hg2+ recognition in aqueous solution, where the CDs-N exhibited better sensitivity and selectivity for Hg2+ detection, with a low limit of detection of 8.29 × 10−6 mol/L. It was determined that the fluorescence quenching could be ascribed to a photoinduced charge-transfer processes between Hg2+ and the CDs. In addition, the CDs-N were used as a smart invisible ink for anti-counterfeiting, information encryption and decryption. Furthermore, the CDs-N were immersed into a cellulose (CMC)-based hydrogel network to prepare fluorescent hydrogels capable of simultaneously detecting and adsorbing Hg2+. We anticipate that this research will open possibilities for a green method to synthesize fluorescent CDs for metal ion detection and fluorescent ink production.

  • Ping Sun, Yuanqin Huang, Shunhong Chen, Xining Ma, Zhaokai Yang, Jian Wu
    Chinese Chemical Letters. 2024, 35(7): 109005-.

    Indole is a biologically active compound formed by the fusion of benzene and pyrrole, and it is widely found in natural products and drugs. Due to the unique structure and properties of indole, its derivatives often exhibit distinctive physiological activities, which has led to widespread attention in the field of pesticide development. Analyzing the design strategies and structure-activity relationships (SARs) of compounds is a crucial step in developing novel pesticides. This review mainly summarizes indole compounds with plant growth regulating, antiviral, fungicidal, herbicidal, and insecticidal activities, with the aim of providing new insights into the discovery and mechanism of action of novel indole-based pesticides.

  • Zixi Zou, Jingyuan Wang, Yian Sun, Qian Wang, Da-Hui Qu
    Chinese Chemical Letters. 2024, 35(7): 108972-.

    Dynamic assembly on time scale is common in biological systems but rare for artificial materials, especially for smart luminescent materials. Programming molecular assembly in a spatio-temporal manner and resulting in white-light-including multicolor fluorescence with time-dynamic features remains challenging. Herein, controlling molecular assembly on time scale is achieved by integrating a pH-responsive motif to a transient alkaline solution which is fabricated by activators (NaOH) and deactivators (esters), leading to automatic assembly on time scale and time-dependent multicolor fluorescence changing from blue to white and yellow. The kinetics of the assembly process is dependent on the ester hydrolysis process, which can be controlled by varying ester concentrations, temperature, initial pH, stirring rate and ester structures. This dynamic fluorescent system can be further developed for intelligent fluorescent materials such as fluorescent ink, three-dimension (3D) codes and even four-dimension (4D) codes, exhibiting a promising potential for information encryption.

  • Jingqi Xin, Shupeng Han, Meichen Zheng, Chenfeng Xu, Zhongxi Huang, Bin Wang, Changmin Yu, Feifei An, Yu Ren
    Chinese Chemical Letters. 2024, 35(7): 109165-.

    Tumor microenvironment (TME)-activatable probes have been proven to effectively increase signal-to-background ratios (SBRs) and improve the success rate of complete tumor resection. However, many fluorescence probes have to be loaded into a nanocarrier for tumor targeted delivery, which consequently encounters poor drug loading, heterogeneous composition and non-encapsulated drug aggregates occurred during nanoformulation fabrications. Herein, a nitroreductase (NTR)-activated "OFF-ON" near-infrared fluorescence nanoprobe, named NanoBodipy, was synthesized by the spontaneous self-assembling of NTR-responsive dye-polyethylene glycol (PEG) amphiphilic polymer in water. The NTR-responsive dye acted as the hydrophobic segment in the amphiphilic polymer, yielding a homogeneous composition and a high loading of 12.2 wt% (according to calculation) in the synthesized NanoBodipy. The synthesized NanoBodipy can efficiently accumulate in tumors via the enhanced permeability and retention (EPR) effect, enabling non-invasive tumor-targeted fluorescence imaging and guiding complete tumor resection. Once the synthesized NanoBodipy entered the tumor cells, they dissociated and were activated by overexpressed NTR. With the real-time fluorescence guide of NanoBodipy, complete tumor resection surgery was performed successfully.

  • Shuangliang Xie, Yuyue Chen, Qing He, Liang Chen, Jikun Yang, Shiqing Deng, Yimei Zhu, He Qi
    Chinese Chemical Letters. 2024, 35(7): 108871-.

    Relaxor ferroic dielectrics have garnered increasing attention in the past decade as promising materials for energy storage. Among them, relaxor antiferroelectrics (AFEs) and relaxor ferroelectrics (FEs) have shown great promise in term of high energy storage density and efficiency, respectively. In this study, a unique phase transition from relaxor AFE to relaxor FE was achieved for the first time by introducing strong-ferroelectricity BaTiO3 into NaNbO3-BiFeO3 system, leading to an evolution from AFE R hierarchical nanodomains to FE polar nanoregions. A novel medium state, consisting of relaxor AFE and relaxor FE, was identified in the crossover of 0.88NaNbO3–0.07BiFeO3–0.05BaTiO3 ceramic, exhibiting a distinctive core-shell grain structure due to the composition segregation. By harnessing the advantages of high energy storage density from relaxor AFE and large efficiency from relaxor FE, the ceramic showcased excellent overall energy storage properties. It achieved a substantial recoverable energy storage density Wrec ~ 13.1 J/cm3 and an ultrahigh efficiency η ~ 88.9%. These remarkable values shattered the trade-off relationship typically observed in most dielectric capacitors between Wrec and η. The findings of this study provide valuable insights for the design of ceramic capacitors with enhanced performance, specifically targeting the development of next generation pulse power devices.

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