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  • Changli Wang, Xinran Li, Wenping Yang, Yuxia Xu, Huan Pang
    Chinese Chemical Letters. 2021, 32(9): 2909-2913.

    Metal-organic frameworks (MOFs) with porous crystal structures have attracted extensive attention in application of energy storage and conversion, owing to their regularity, porosity, large specific surface area, etc. In this work, Co-MOF-74 microflower has been successfully prepared via a controllable solvent regulation strategy. Through modulating the polarity of the solvent, crystals grow in certain preferred orientation and Co-MOF-74 with various morphologies were obtained. Thereinto, the energy storage performance of Co-MOF-74 microflower was measured in both three-electrode system and asymmetric supercapacitor device (specific capacitance of 164.2 F/g at 0.5 A/g in the three-electrode system and 62.5 F/g at 1 A/g in the asymmetric supercapacitor device). This can be attributed to the preferred crystal orientation resulting in a regular and uniform microflower, which is of great significance to electronic interfacial exchange and ion transfer during electrochemical reactions.

  • Qingjiang Yu, Kecheng Jiang, Cuiling Yu, Xianjin Chen, Chuanjian Zhang, Yi Yao, Bin Jiang, Huijin Long
    Chinese Chemical Letters. 2021, 32(9): 2659-2678.

    In comparison with lithium-ion batteries (LIBs) with liquid electrolytes, all-solid-state lithium batteries (ASSLBs) have been considered as promising systems for future energy storage due to their safety and high energy density. As the pivotal component used in ASSLBs, composite solid polymer electrolytes (CSPEs), derived from the incorporation of inorganic fillers into solid polymer electrolytes (SPEs), exhibit higher ionic conductivity, better mechanical strength, and superior thermal/electrochemical stability compared to the single-component SPEs, which can significantly promote the electrochemical performance of ASSLBs. Herein, the recent advances of CSPEs applied in ASSLBs are presented. The effects of the category, morphology and concentration of inorganic fillers on the ionic conductivity, mechanical strength, electrochemical window, interfacial stability and possible Li+ transfer mechanism of CSPEs will be systematically discussed. Finally, the challenges and perspectives are proposed for the future development of high-performance CSPEs and ASSLBs.

  • He Qi, Liyan Jiang, Qiong Jia
    Chinese Chemical Letters. 2021, 32(9): 2629-2636.

    The analysis of endogenous glycoproteins and glycopeptides in human body fluids is of great importance for screening and discovering disease biomarkers with clinical significance. However, the presence of interfering substances makes the direct quantitative detection of low-abundance glycoproteins and glycopeptides in human body fluids one of the great challenges in analytical chemistry. Magnetic solid phase extraction (MSPE) has the advantages of easy preparation, low cost and good magnetic responsiveness. Magnetic adsorbents are the core of MSPE technology, and magnetic adsorbents based on different functional materials are widely used in the quantitative analysis of glycoproteins and glycopeptides in human body fluids, making it possible to analyze glycoproteins and glycopeptides with low abundance as well as multiple types, which provides a technical platform for screening and evaluating glycoproteins and glycopeptides in body fluids as disease biomarkers. In this paper, we focus on the recent advances in the application of MSPE technology and magnetic adsorbents for the separation and enrichment of glycoproteins and glycopeptides in human body fluids, and the future trends and application prospects in this field are also presented.

  • Mamitiana Roger Razanajatovo, Wenyan Gao, Yaran Song, Xuan Zhao, Qina Sun, Qingrui Zhang
    Chinese Chemical Letters. 2021, 32(9): 2637-2647.

    In recent years, lanthanum-based nanomaterials (La-NMs) are selected as an efficient nano-adsorbent for phosphate removal because La3+ has a strong affinity with oxygen-donor atoms from phosphate. Additionally, there are a broad interest and literature base for the effect of different synthesis optimization and environmental parameters on the adsorption performance of La-NMs. A considerable amount of research has also investigated the regeneration and application of La-NMs to real wastewater in a laboratory scale. Based on the literature survey, it was found that La-NMs are often produced via co-precipitation and hydrothermal methods. Moreover, phosphate's adsorption process and behavior onto La-NMs are described well with the pseudo-second-order model and Langmuir model. The interaction mechanism between phosphate and La-NMs are dominated by ligand exchange, surface complexation and electrostatic attraction. Furthermore, phosphate could easily desorb from La-NMs due to the weak H-bonding interaction between phosphate and the H-bond acceptor groups on the surface of La-NMs. Despite the wealth of literature available in this area, there is a lack of systematic review to evaluate the gaps in the use of La-NMs to eliminate phosphate in water. In this review, we mainly summarize and discuss the role and the effect of the synthesis techniques on the physicochemical properties and the adsorption behavior of La-NMs. The possible adsorption mechanism, regeneration efficiency, and the application of La-NMs to the real environmental samples are also presented and highlighted.

  • Tao Zhong, Zhida Chen, Jitao Yi, Gui Lu, Jiang Weng
    Chinese Chemical Letters. 2021, 32(9): 2736-2750.

    Since the sulfur(VI) fluoride exchange reaction (SuFEx) was introduced by Sharpless and co-workers in 2014, this new-generation click chemistry has emerged as an efficient and reliable tool for creating modular intermolecular connections. Sulfonyl fluorides, one of the most important sulfur(VI) fluoride species, have attracted enormous attention in diverse fields, ranging from organic synthesis and material science, to chemical biology and drug discovery. This review aims to introduce seminal and recent progresses on the synthetic methods of sulfonyl fluorides, which include aromatic, aliphatic, alkenyl, and alkynyl sulfonyl fluorides. While not meant to be exhaustive, the purpose is to give a timely overview and insight in this field, and stimulate the development of more efficient synthetic methods of sulfonyl fluorides.

  • Jingjing Wang, Xue Liu, Ziyan Wu, Feng Li, Tingting Qin, Siyuan Zhang, Weiguang Kong, Lantao Liu
    Chinese Chemical Letters. 2021, 32(9): 2777-2781.

    Silver-catalyzed decarboxylative C-H alkylation of cyclic aldimines with abundant aliphatic carboxylic acids has been realized under mild reaction conditions generating the corresponding products in moderate to good yields (32%-91%). In addition, a gram-scale reaction, late-stage modification of drug, synthetic transformation of the product, and further application of the catalytic strategy were also performed. Preliminary studies indicate that the reaction undergoes a radical process.

  • Yujie Dai, Yiming Ding, Linlin Li
    Chinese Chemical Letters. 2021, 32(9): 2715-2728.

    With high catalytic activity and stability, nanozymes have huge advantage in generating or eliminating the reactive oxygen species (ROS) due to their intrinsic enzyme-mimicking abilities, therefore attracting wide attention in ROS-related disease therapy. To better design nanozyme-based platforms for ROS-related biological application, we firstly illustrate the catalytic mechanism of different activities, and then introduce different strategies for using nanozymes to augment or reduce ROS level for the applications in cancer therapy, pathogen infection, neurodegeneration, etc. Finally, the challenges and future opportunities are proposed for the development and application of nanozymes.

  • Peng Yang, Yuxuan Ye, Zidu Yan, Qiang Li, Kun Zhang, Yezhi Yang, Qiuyue Zhang, Hang Yin, Dongsheng Xia, Fei Pan
    Chinese Chemical Letters. 2021, 32(9): 2823-2827.

    As a novel wastewater treatment strategy, the intimate coupling of photocatalysis and biodegradation (ICPB) has been attracted attention, which is ascribed to its combination of the advantages of photocatalytic reactions and biological treatment. The selection of carriers is important since it affects the stability of the system and the removal efficiency of pollutants. In this study, a novel ICPB system was successfully constructed by loading photocatalytic materials (i.e., TiO2, N-TiO2, and Ag-TiO2) and microbes onto non-woven cotton fabric. The photocatalysts were characterized by scanning electron microscope-energy dispersive spectrometer (SEM-EDS), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). This system exhibited good performance in degrading tetracycline (TC) in water. The results showed that Ag-TiO2-ICPB had the maximum removal efficiency of tetracycline (94.7%) in 5 h, which was 16.5% higher than the photocatalysis alone. After five cycles, 82.9% of tetracycline could be still degraded through Ag-TiO2-ICPB. SEM spectrum showed microbes on the material changed little before and after the reactions. This result implied the materials were stable, and then beneficial for degrading of pollutants continuously. The intermediates were detected through ultraperformance liquid chromatography-mass spectrometer (UPLC-MS) and the plausible degradation pathways were proposed. Electron paramagnetic resonance (EPR) analysis showed OH and O2 were the main reactive oxygen species for TC degradation. In conclusion, the ICPB system with non-woven cotton fabric as a carrier has certain application prospects for antibiotic-containing wastewater.

  • Huan Li, Hang Liu, Yan Zhang, Na Yang, Lixia Xiong, Zhengming Li, Baolei Wang
    Chinese Chemical Letters. 2021, 32(9): 2893-2898.

    Diamide compounds such as chlorantraniliprole, a famous anthranilic diamide insecticide targeting the insect ryanodine receptor (RyR), have received continuous attention in pesticide research during the past 15 years owing to their excellent insecticidal potentials. With the aim of discovering new heterocyclic pesticides used for crop protection, based on the structural information of compound M from the reported pharmacophore-based virtual screening for RyR insecticides and diamide compound, a series of new heterocyclic mono-, di-, and tri-amide derivatives containing piperazine moiety have been synthesized in this paper. The new compounds were identified and confirmed by melting point, 1H NMR, 13C NMR and HRMS. Compound M was firstly validated for insecticidal activities, and the new synthesized compounds were all made comprehensive insecticidal evaluations against diamondback moth and oriental armyworm. The bioassay results showed that some of the compounds exhibit favorable insecticidal potentials, particularly some novel piperazine-containing heterocyclic mono-/di-/tri-amide derivatives such as 8g, 14a, 15a, 15g, 15i, 15j, 15k, 15l, and 15m could be used as new insecticidal leading structures for further study (e.g., towards diamondback moth, 15i-15m LC50: 0.0022−0.0081 mg/L). The structure-activity relationships of the compounds discussed in detail provide useful guidance for further design and development of new insecticides.

  • Yonghui Qiao, Zhihao Wei, Tingting Qin, Rufeng Song, Zhiqiang Yu, Qi Yuan, Juan Du, Qingbing Zeng, Lanlan Zong, Shaofeng Duan, Xiaohui Pu
    Chinese Chemical Letters. 2021, 32(9): 2877-2881.

    Tumor drug resistance and systemic side effects of chemotherapeutic drugs are the main reasons for the failure of cancer treatment. In recent years, it was found that some natural active ingredients can reverse MDR and regulate body immunity to enhance the efficacy and reduce toxicity of chemotherapeutic drugs. In this paper, a new nanosuspensions, HCPT and QUR hybrid nanosuspensions (HQ-NPs), was prepared by the microprecipitation-high pressure homogenization method to reverse tumor drug resistance, reduce toxicity, and increase therapeutic efficacy. The in vitro investigation results showed that HQ-NPs had a unique shape (particle size was about 216.3±5.9 nm), changed crystalline, and different dissolution rates compared with HCPT-NPs and QUR-NPs, which is attributed to the strong intermolecular forces between HCPT and QUR as indicated by the results of the molecule dock. It was verified that the HQ-NPs could double the retention of HCPT in cells and enhance the cytotoxicity to A549/PTX cells in vitro tests compared with HCPT-NPs. We also found that HQ-NPs can significantly enhance the accumulation of HCPT in tumor sites, improve the antitumor activity of HCPT, and protect the immune organs and other normal tissues (P < 0.01), compared with HCPT-NPs. Therefore, hybrid nanosuspensions can offer promising potential as the drug delivery system for HCPT and QUR to increase the therapeutic efficacy and reduce the toxicity of HCPT.

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