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  • Hang Zhou, Yuwei Wang, Fuqiang Wang, Hao Deng, Yongchen Song, Changping Li, Zheng Ling
    Chinese Chemical Letters. 2020, 31(6): 1665-1669.

    Recent studies have shown impressive transport behaviors of water and ions within lamellar MXene membranes, which endows great promise in developing advanced separation application based high performance MXene membranes. However, most of the researches focused on modification of MXene nanoflakes and optimizing interlayer distance, leaving the impact of membrane fabrication process marginal. In this work, we studied the water flux of membranes made by vacuum filtration using delaminated MXene nanoflakes as the building-blocks. Our results show that the water permeability is extremely sensitive to the process, especially at the drying process, loading and deposit rate of nanoflakes (the feeding concentration). We find that the voids from less ordered stack rather than in-plane defects and interlayer galleries contribute to the large water permeability. The voids can be effectively avoided via deposition of MXene nanoflakes at a slow rate. Manipulating the stack of MXene nanoflakes during vacuum filtration and drying are critical for development of MXene membranes with desired performance for water permeation.

  • Shu Zhang, Xibo Pei, Yiyuan Xue, Jingyuan Xiong, Jian Wang
    Chinese Chemical Letters. 2020, 31(6): 1654-1659.

    The carbon quantum dots (CQDs) and their functionalized materials are promising in biomedical field because of their unique properties; meanwhile, a growing concern has been raised about the potential toxicity of these modified materials in biosystem. In this study, we synthesized original CQDs and two common functionalized CQDs including N-doped CQDs (NCQDs) and folic acid-modified CQDs (FA-CQDs), and compared the toxicity and biocompatibility with each other in vitro and in vivo. L929, C6 and normal cell MDCK were selected to detect the adverse reaction of these materials in vitro. No acute toxicity or obvious changes were noted from in vitro cytotoxicity studies with the dose of these CQD materials increasing to a high concentration at 1 mg/mL. Among these materials, the FA-CQDs show a much lower toxicity. Moreover, in vivo toxicity studies were performed on the nude mice for 15 days. The experimental animals in 10 or 15 mg/kg groups were similar with animals treated by phosphate buffer solution (PBS) after 15 days. The results of the multifarious biochemical parameters also suggest that the functionalized products of CQDs do not influence the biological indicators at feasible concentration. Our findings in vitro and in vivo through toxicity tests demonstrate that CQDs and their modified materials are safe for future biological applications.

  • Cao Cao, Yan Shi, Xiaohui Wu, Liqun Zhang
    Chinese Chemical Letters. 2020, 31(6): 1660-1664.

    Poly(N, N-dimethyl acrylamide)-block-poly(styrene)-block-poly(N, N-dimethyl acrylamide) (PDMAc-b-PSt-b-PDMAc) amphiphilic triblock copolymer micro/nano-objects were synthesized through reversible addition-fragmentation chain transfer (RAFT) dispersion polymerization of St mediated with poly(N, N-dimethyl acrylamide) trithiocarbonate (PDMAc-TTC-PDMAc) bi-functional macromolecular RAFT agent. It is found that the morphology of the PDMAc-b-PSt-b-PDMAc copolymer micro/nano-objects like spheres, vesicles and vesicle with hexagonally packed hollow hoops (HHHs) wall can be tuned by changing the solvent composition. In addition, vesicles with two sizes (600 nm, 264 nm) and vesicles with HHHs features were also synthesized in high solid content systems (30 wt% and 40 wt%, respectively). Besides, as compared with typical AB diblock copolymers (A is the solvophilic, stabilizer block, and B is the solvophobic block), ABA triblock copolymers tend to form higher order morphologies, such as vesicles, under similar conditions. The finding of this study provides a new and robust approach to prepare block copolymer vesicles and other higher order micelles with special structure via PISA.

  • Yu Xin, Sheng Peng, Junxing Chen, Zujin Yang, Jianyong Zhang
    Chinese Chemical Letters. 2020, 31(6): 1448-1461.

    Porous materials play an important role in chemical catalysis, separation and other industrial applications. High-efficiency preparation of porous materials has become an active research area. Conventional synthesis of porous materials has been dominated by one-pot solution processing conditions carried out by bulk mixing under conventional electric heating via hydrothermal, solvothermal or ionothermal reactions where high temperatures and pressures are the standard. Continuous flow synthesis has many key advantages in terms of efficient mass and heat transfer, precise control of residence times, improved opportunities for automation and feedback control of synthesis, scaling-up reactions and improved safety parameters compared to above mentioned conventional batch scale synthetic methods. In this review, continuous flow synthesis of various crystalline porous materials such as metal-organic frameworks (MOFs), covalent-organic frameworks (COFs), porous organic cages and zeolites is discussed. Combination of microfluidic methods with other techniques are also shown including various heating ways and various methods of substrate adding.

  • Fan Yu, Laichun Wang, Qiuju Xing, Dengke Wang, Xunheng Jiang, Guangchao Li, Anmin Zheng, Fanrong Ai, Jian-Ping Zou
    Chinese Chemical Letters. 2020, 31(6): 1648-1653.

    Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride (g-C3N4). Herein, g-C3N4 with yellow (Y-GCN) and brown (C-GCN) were prepared by using the fresh urea and the urea kept for five years, respectively, for the first time. Experimental results show that the H2 production rate of the C-GCN is 39.06 μmol/h, which is about 5 times of the Y-GCN. Meantime, in terms of apparent quantum efficiency (AQE) at 420 nm, C-GCN has a value of 6.3% and nearly 7.3 times higher than that of Y-GCN (0.86%). The results of XRD, IR, DRS, and NMR show, different from Y-GCN, a new kind of functional group of —N=CH— was firstly in-situ introduced into the C-GCN, resulting in good visible light absorption, and then markedly improving the photocatalytic performance. DFT calculation also confirms the effect of the —N=CH— group band structure of g-C3N4. Furthermore, XPS results demonstrate that the existence of —N=CH— groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles, and then improves the charge separation and photocatalytic performance. The present work demonstrates a good example of "defect engineering" to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.

  • Jing Zheng, Dandan Song, Hong Chen, Jingli Xu, Njud S. Alharbi, Tasawar Hayat, Min Zhang
    Chinese Chemical Letters. 2020, 31(5): 1109-1113.

    The exploitation of multifunctional nanocomposites is highly desired in environmental monitoring, biosensors, and medical diagnosis. In this paper, a simple approach has been proposed to fabricate MoS2 decorated N-doped carbon nanotubes (NCNTs@MoS2) hybrid composites as efficient peroxidase-like mimics. The combination of the MoS2 and N-doped carbon nanotubes (NCNTs) brings about an enhanced synergistic effect, leading to remarkably decent intrinsic peroxidase-mimic activities than that of the single components. Due to the high catalytic efficiency of the resultant NCNTs@MoS2 hybrid nanotubes as peroxidase-like mimics, a convenient colorimetric approach for the sensitive determination of H2O2 and ascorbic acid have been developed with a detection limit of about 0.14 μmol/L and 0.12 μmol/L, respectively. The work offers a new strategy for the fabrication of peroxidase-like nanomaterials with excellent catalytic activity, which indicates great promising applications in sensitive detections in real samples.

  • Young-Youb Kim, Yongbin Bang, Dayoung Lee, Mingyu Kang, Yoon-Kyu Song
    Chinese Chemical Letters. 2020, 31(5): 1137-1140.

    Here, we use two important biomaterials, protein and DNA, to construct self-assembled linear nanostructures through Watson-Crick base-paring of DNAs. We apply a simple magnetic separation method to purify traptavidin-DNA conjugates, and demonstrate synthesis of linear arrays of traptavidinDNA conjugates via the step-growth polymerization approach with pre-determined DNA sequences. Using the traptavidin-DNA array as a template, we assemble gold nanoparticles to form linear plasmonic nanostructures in a programmable manner. The traptavidin-DNA conjugates thus provide a convenient platform for one-dimensional assembly of biotinylated nanomaterials for many biomedical applications from drug delivery to bio-sensing.

  • Kaijie Wang, Qing Kong, Xiaoqiang Chen, Juyoung Yoon, K.M. K. Swamy, Fang Wang
    Chinese Chemical Letters. 2020, 31(5): 1087-1090.

    A new simple bifunctional chemosensor 1 based on rhodamine was synthesized by hydrazide and formylformic acid, which could detect Cu2+ and Hg2+ via different detecting methods in CH3CN-HEPES buffer solution (20 mmol/L, pH 7.4) (1:9, v/v) respectively. When sensor 1 bound with Cu2+, it showed a colorimetric change, while a selective enhancement in fluorescence occurred upon 1 binding with Hg2+, resulting from the spirolatam-ring opening process. The binding modes of 1 with Cu2+ and Hg2+ were investigated based on UV, fluorescence change, ESI-Mass and Job's Plot data. Moreover, sensor 1 could selectively detect target ion in a mixed solution of Cu2+ and Hg2+, and the two metal ions do not interfere with each other in the process of detecting Cu2+ or Hg2+ with 1.

  • Yuxuan Chen, Bowen Li, Xiaohong Chen, Min Wu, Yongtao Ji, Guping Tang, Yuan Ping
    Chinese Chemical Letters. 2020, 31(5): 1153-1158.

    We herein propose a co-delivery approach where small interference RNA (siRNA) and anticancer chemotherapeutic drug are simultaneously loaded into a single delivery carrier for the combined treatment of breast cancer and metastasis prevention. The co-delivery vector is composed of chondroitin sulfate (CS)-coated β-cyclodextrin-polyethylenemine polymer, which is capable of loading paclitaxel (PTX) and siRNA simultaneously to form therapeutic nanocomplexes. The nanocomplex, termed as CPPTX-siCD146-CS, is demonstrated to have strong active targeting ability towards CD44-overexpresing breast cancer cells. Moreover, the co-delivery of PTX and siRNA not only effectively inhibits cancer cells proliferation and induces apoptosis, but also well prevents metastasis. Importantly, CP-PTX-siCD146-CS nanocomplexes exhibit stronger cytotoxic effects and anti-metastatic effects on MBA-MD-231 breast cancer cells, in comparison with PTX or siCD146 mono-treatment. The current study defines a potential therapeutic strategy for the combined breast cancer treatment and metastasis prevention from a codelivery perspective.

  • Huibin Yang, Huitang Qi, Zesheng Hao, Xusheng Shao, Tian Liu, Qing Yang, Xuhong Qian
    Chinese Chemical Letters. 2020, 31(5): 1271-1275.

    Insect chitinase and N-acetyl-β-D-hexosaminidases (Hex) are potential targets for developing new pesticides. Here, a series of thiazolylhydrazones I (with substituted group R1 at N3) and II (with substituted group R1 at N2) were designed, synthesised and evaluated as competitive inhibitors of OfHex1 and OfChi-h, from the agricultural pest Ostrinia furnacalis. Derivatives I-3d and II-3d, with phenoxyethyl group at R1, demonstrated the best inhibitory activities against OfHex1 and OfChi-h. Molecular docking analysis indicated that the branched conformation compound II-3d (Ki=1.5 μmol/L) formed more hydrogen bonds with OfHex1 than the stretched conformation compound I-3d (Ki=5.9 μmol/L). The differences in compounds' binding conformations with OfChi-h explained differences in inhibitory activity of compounds I-3d (Ki=1.9 μmol/L) and II-3d (Ki=4.1 μmol/L). This work suggests a novel scaffold for developing specific Hex and Chi-h inhibitors.

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