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  • Yongxing Sun, Kaijun Quan, Jia Chen, Hui Li, Xin Li, Zuguang Li, Hongdeng Qiu
    Chinese Chemical Letters. 2023, 34(9): 108166-.

    In this study, two novel spherical/hollow metal-organic frameworks were successfully synthesized, and further modified by a mild non-covalent modification strategy with dopamine and 1, 4-benzenedithiol (BDT) as polymeric monomers to obtain pBDT@PDA-Ni-MOF and pBDT@PDA-Ni/Co-MOF, respectively. The results showed that the above MOFs possessed extremely fast adsorption rates and ideal adsorption capacities for sulfonamides (SAs) and the modified MOFs exhibited enhanced adsorption capacities for SAs owing to a large number of additional functional groups. Then, benefit of their regular morphology and size, a facile syringe-assisted dispersive solid phase extraction (S-DSPE) method was developed for efficient detection of SAs, which will provide a powerful tool for monitoring trace level of SAs in aqueous environment.

  • Jiajia Yuan, Xiaoya Fan, Jiacheng Yang, Xinfeng Zhang
    Chinese Chemical Letters. 2023, 34(9): 108155-.

    Developing multiplex sensing technique is of great significance for fast sample analysis. However, the broad emissions of most chemiluminescence (CL) luminophores make the multiplex CL analysis be difficult. In this work, a simple and sensitive CL analytical method has been developed for the simultaneous determination of Tb3+ and Eu3+ thanking to their narrow band emission. The technique was based on a mixed CL system of periodate (IO4)-hydrogen peroxide (H2O2)-rare earth complexes, in which the reactive oxygen species (ROSs) especially singlet oxygen (1O2) can transfer its energy to the complex of Tb3+/Eu3+-ethylenediaminetetraacetic acid disodium salt (EDTA) and then produce the characteristic emissions of Tb3+ and Eu3+ without cross-interference. The further experiment found that the CL emissions of Tb3+ and Eu3+ could be catalyzed by the gold nanoparticles (AuNPs) via enhancing the yield of 1O2. The CL intensities of Tb3+ (at 490 nm) and Eu3+ (at 620 nm) increased linearly with concentration of Tb3+ and Eu3+. After the optimization of the CL sensing conditions, the limits of detection (LOD) were 5.0 × 10−9 mol/L and 8.0 × 10−7 mol/L for Tb3+ and Eu3+, respectively. Finally, the method has been applied for measuring the contents of Tb3+ and Eu3+ in leaching solution of mine sample and Tb3+/Eu3+-contained nanomaterials with satisfactory results. The present system provides a new CL technique for multiplex sensing with simplicity and high sensitivity.

  • Qi Li, Zi-Lu Wang, Yun-He Xu
    Chinese Chemical Letters. 2023, 34(9): 108150-.

    Herein, copper-catalyzed 1,4-protosilylation and 1,4-protoborylation of enynic orthoesters have been developed. The enynic orthoesters as precursors of unstable enynic esters were applied to produce the functionalized 2, 3-allenoate products. Meanwhile, the asymmetric 1,4-protosilylation of enynic orthoesters with PhMe2Si-Bpin was also studied. The chiral monopyridine imidazoline ligand was efficient to provide the asymmetric 1,4-protosilylation products with high enantioselectivity.

  • Xianxu Chu, Yueyu Liao, Lu Wang, Junru Li, Hui Xu
    Chinese Chemical Letters. 2023, 34(9): 108285-.

    Transition metal sulfides are demonstrated to play an increasingly important role in boosting the deployment of ecofriendly electrocatalytic energy conversion technologies. It is also widely recognized that the introduction of vacancies is now becoming an important and valid approach to promote the electrocatalytic performance. In this review, the significance of sulfur vacancies on the enhancement of catalytic performance via four main functionalities, including tuning the electronic structure, tailoring the active sites, improving the electrical conductivity, and regulating surface reconstruction, is comprehensively summarized. Many effective strategies for the sulfur vacancy engineering, such as plasma treatment, heteroatom doping, and chemical reduction are also comprehensively provided. Subsequently, recent achievements in sulfur vacancy fabrication on various hotspot electrocatalytic reactions are also systematically discussed. Finally, a summary of the recent progress and challenges of this interesting field are organized, which hopes to guide the future development of more efficient metal sulfide electrocatalysts.

  • Zexu Fang, Ying Gu, Xinran Dong, Gen Zhang, Lin Li, Xiaoguang Zhou, Chungui Tian
    Chinese Chemical Letters. 2023, 34(9): 108128-.

    Hydrogenation reactions play crucial roles on chemical synthesis and pollutant elimination. The improvement of the ability to activate reactants and increase of the contact probability between the catalysts and reactants are positive to improve the catalytic performance. Herein, we have reported the design of two-dimensional porous Ni-Ni3N-NiMoN heterojunction sheets (2D Mo-Ni based nanosheets) for efficient catalytic hydrogenation of the aromatic nitro-compounds. The heterojunction interfaces provide plentiful active sites to improve the activating ability of the catalyst on the reactants. Additionally, the 2D porous structure facilitates not only the contact of catalytic sites with reactants but also mass transfer and diffusion, both of which are favorable to accelerating the hydrogenation process. As a result, the optimized sample of 2D Mo-Ni sheet exhibits good activity for the hydrogenation of aromatic nitro-compounds by converting 0.2 mmol/L (30 mL) of p-nitrophenol to p-aminophenol within 45 s with good recyclability. The activation energy and the reaction rate at 25 ℃ is 31.11 kJ/mol and 0.0796 s-1, respectively, both of which surpass most of reported non-noble metal catalysts and rivals with most noble metal-based catalysts. The combination of late and early transition metals provides an innovative way to obtain outstanding catalysts for the hydrogenation.

  • Zhe Wang, Lingyu Zhang, Zhen Lei, Liyuan Zheng, Liqin Huang, Shuang Liu, Yuexiang Lu
    Chinese Chemical Letters. 2023, 34(9): 108146-.

    Uranium is the main fuel of nuclear power and elimination uranium from nuclear wastewater is significant both in environmental protection and fuel recycle. Here we report for the first time the synthesis of carbon dots/polyurethane (CDs/PU) composite materials for the photoinduced elimination of uranium from water. Irradiated with visible light, CDs/PU could eliminate uranium efficiently with the generation of (UO2)O2·2H2O as solid products in air. The further investigated mechanism showed that the addition of CDs/PU could produce more H2O2 under visible light, which reacted with uranyl ions to form (UO2)O2·2H2O. Importantly, the sponge-like CDs/PU could be easily removed from water with high reusability as the elimination efficiency remained above 95% after 5 cycles. CDs/PU also displayed good selectivity in the presence of other metal ions. Our work affords exciting strategies for developing photocatalysts and eliminating uranium from water.

  • Meifang Wang, Ping'an Ma, Jun Lin
    Chinese Chemical Letters. 2023, 34(9): 108300-.

    The cancer cells realize their proliferation and metastasis activities based on the special redox adaptation to increased reactive oxygen species (ROS) level, which inversely makes them sensitive to external interference with their redox state. In view of this, in recent decades, researchers have made great efforts to construct a series of novel nanoplatform-based ROS-mediated cancer therapies through increasing ROS generation and inhibiting the ROS elimination. Besides, the multidrug resistance and thermoresistance of tumor are closely related to tumor redox state. Recently, numerous works have shown that ROS regulation in cancer cells can intervene in the expression, function and stability of related proteins to achieve reversal of tumor resistance. In this review, the recent researches about ROS-regulating nanoagents on cancer therapy and tumor resistance alleviation have been well summarized. Finally, the challenges and research directions of ROS-regulating nanoagents for future clinical translation are also discussed.

  • Lihua Chu, Hao Yan, Wanfeng Xie, Yuxin Shi, Muhammad Hilal, Changxu Sun, Ze Li, Meicheng Li
    Chinese Chemical Letters. 2023, 34(8): 108512-.

    High-performance and low-cost gas sensors are highly desirable and involved in industrial production and environmental detection. The combination of highly conductive MXene and metal oxide materials is a promising strategy to further improve the sensing performances. In this study, the hollow SnO2 nanospheres and few-layer MXene are assembled rationally via facile electrostatic synthesis processes, then the SnO2/Ti3C2Tx nanocomposites were obtained. Compared with that based on either pure SnO2 nanoparticles or hollow nanospheres of SnO2, the SnO2/Ti3C2Tx composite-based sensor exhibits much better sensing performances such as higher response (36.979), faster response time (5 s), and much improved selectivity as well as stability (15 days) to 100 ppm C2H5OH at low working temperature (200 ℃). The improved sensing performances are mainly attributed to the large specific surface area and significantly increased oxygen vacancy concentration, which provides a large number of active sites for gas adsorption and surface catalytic reaction. In addition, the heterostructure interfaces between SnO2 hollow spheres and MXene layers are beneficial to gas sensing behaviors due to the synergistic effect.

  • Peikun Xin, Shuyan Han, Jun Huang, Conglai Zhou, Jiayuan Zhang, Xinru You, Jun Wu
    Chinese Chemical Letters. 2023, 34(8): 108125-.

    As a representative of chronic wounds, the long-term high levels of oxidative stress and blood sugar in chronic diabetic wounds lead to serious complications, making them the biggest challenge in the research on wound healing. Many edible natural biomaterials rich in terpenes, phenols, and flavonoids can act as efficient antioxidants. In this study, okra extract was selected as the main component of a wound dressing. The okra extracts obtained via different methods comprehensively maintained the bioactivity of multiple molecules. The robust antioxidant properties of okra significantly reduced intracellular reactive oxygen species production, thereby accelerating the wound healing process. The results showed that okra extracts and their hydrogel dressings increased cell migration, angiogenesis, and re-epithelization of the chronic wound area, considerably promoting wound remodeling in diabetic rats. Therefore, okra-based hydrogels are promising candidates for skin regeneration and wider tissue engineering applications.

  • Zesi Wang, Jiao Li, Jiao Chen, Zifeng Cao, Hui Li, Yaopeng Cao, Quanquan Li, Mengyao She, Ping Liu, Shengyong Zhang, Jianli Li
    Chinese Chemical Letters. 2023, 34(8): 108507-.

    Thiophenol (PhSH) is an important raw material for organic synthesis, while its high toxicity to organisms makes it an environmental pollutant. Therefore, it is crucial to accurately detect PhSH and explore its metabolic process in the living system. Herein, a near-infrared (NIR) fluorescent probe TEM-FB was developed for sensing PhSH with a turn-on fluorescent signal at 719 nm and a large Stokes shift (198 nm) based on generating the intramolecular charge transfer (ICT) process. TEM-FB shows high specificity and significant sensitivity towards PhSH (detection limit: 10 nmol/L) via the aromatic nucleophilic substitution mechanism. Furthermore, it was successfully applied to image PhSH in multiple cell lines and in zebrafish. Notably, we revealed the oxidative stress process caused by PhSH and demonstrated that the hydrogen peroxide (H2O2) in cells would alleviate the poisonousness from exogenous PhSH for the first time. This work provides a promising bioimaging tool for monitoring PhSH in living systems and visualizing the process of oxidative stress induced by PhSH.

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