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  • Zhang-Ye Han, Hong-Kai Li, Qian-Qian Zhu, Rongrong Yuan, Hongming He
    Chinese Chemical Letters. 2021, 32(9): 2865-2868.

    Porous organic frameworks (POFs) are excellently stable porous materials, which can be employed as host platforms to support metal nanoparticles as functional composites for various applications. Herein, a novel POF is successfully prepared via Friedel-Crafts reaction. Silver nanoparticles (Ag NPs) are embedded in the prepared POF to generate an Ag@POF composite, which not only possesses high surface area, outstanding physicochemical stability and outstretched π-conjugation skeleton, but also exhibits preferable electrochemical stability and conductivity. This composite is able to immobilize a mass of aptamer strands to fabricate an intriguing electrochemical aptasensor. Electrochemical impedance spectroscopy (EIS) is a commonly used technology to analyze the electrochemical signal variation. The Ag@POF-based biosensor shows the excellent electrochemical detection behavior through analyzing EIS. For instance theophylline as a research mode, the Ag@POF based electrochemical aptasensor reveals ultra-sensitiveness, high selectivity, remarkable stability, good repeatability and simple operability even in various real samples. Notably, this aptasensor has the sensitive detection performance with the limit of detection of 0.191 pg/mL (1.06 pmol/L) in a wide concentration range of 5.0 × 10-4 – 5.0 ng/mL (2.78 × 10-3 – 27.8 nmol/L).

  • Xingyu Cui, Xia Xing, Xinrui Wang, Wenying Shi, Chao Lu
    Chinese Chemical Letters. 2021, 32(9): 2869-2872.

    Pressure-related sensing materials in mechanochromic luminescent materials have received wide attention. However, at present, most piezochromic luminescence (PCL) materials have problems such as aggregation-caused quenching (ACQ) effect due to the presence of powder form, complicated preparation methods and fluorescence quenching effect under high pressure. To solve these problems, we employ three components containing carbon dots (CDs), layered double hydroxides (LDHs) and polyvinyl alcohol (PVA) to construct the CDs-LDHs/PVA film. The LDHs can provide a rigid environment for CDs and improve the luminescent efficiency of CDs. The film shows high sensitivity, stability and reversibility. Moreover, the compressed film can recover to its original state by heating. Therefore, the PCL film with dual emission (fluorescence and phosphorescence) characteristic is constructed, which boosts the sensitivity of pressure-sensing.

  • Yongbin Zhang, Yu Zhang, Yongkang Yue, Jianbin Chao, Fangjun Huo, Caixia Yin
    Chinese Chemical Letters. 2021, 32(9): 2873-2876.
  • 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.

  • Zongju Zhang, Jiugang Hu, Shijun Liu, Xin Hao, Lin Li, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji
    Chinese Chemical Letters. 2021, 32(9): 2882-2886.

    Zero-dimensional carbon dots have emerged as important nanofillers for the separation membrane due to their small specific size and rich surface functional groups. This study proposed a strategy based on hydrophobic carbon dots (HCDs) to regulate water channels for an efficient forward osmosis (FO) membrane. Thin-film composite (TFC) membranes with superior FO performance are fabricated by introducing HCDs as the nanofiller in the polyacrylonitrile support layer. The introduction of HCDs promotes the formation of the support layer with coherent finger-like hierarchical channels and micro-convex structure and an integrated polyamide active layer. Compared to the original membrane, TFC-FO membrane with 10 wt% HCDs exhibits high water flux (15.47 L m−2h−1) and low reverse salt flux (2.9 g m−2h−1) using 1 mol/L NaCl as the draw solution. This improved FO performance is attributed to the lower structural parameters of HCDs-induced water channels and alleviated internal concentration polarization. Thus, this paper provides a feasible strategy to design the membrane structure and boost FO performance.

  • Huijun Li, Sancan Han, Bowen Lyu, Ting Hong, Shibo Zhi, Ling Xu, Fengfeng Xue, Liman Sai, Junhe Yang, Xianying Wang, Bin He
    Chinese Chemical Letters. 2021, 32(9): 2887-2892.

    Carbon dots (CDs) are metal-free fluorescent materials that can be used in optical and electronic devices, but few studies have focused on one-step synthesis routes for CDs with tunable color and high photoluminescence quantum yield (PLQY). Herein, CDs with tunable light emission were synthesized using a novel amide-assisted solvothermal approach. The as-prepared CDs were well dispersed and homogeneous, with average diameters of approximately 2.0–4.0 nm, depending on the dopants. Owing to the surface states with different ratios of nitrogen- and oxygen-related species, different CDs can exhibit blue, green, red, or white emission with relatively high PLQYs of 61.6%, 41.3%, 29.1% and 19.7%, respectively. XPS measurements, in conjunction with DFT calculations, indicate that nitrogen substitution (pyridinic/pyrrolic nitrogen) dominates the blue emission, while introducing oxygen functional groups lowered the LUMO energy level, which resulted in redder emission. In addition, the CDs are demonstrated as a bioimaging probe in bothin vitro and in vivo assays, and the white light CDs have been demonstrated to be potential fluorescent materials for white-light-emitting diode (WLED).

  • 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.

  • Xiaoyu Liu, Yongzheng Fang, Pengcheng Liang, Jiahao Xu, Bo Xing, Kai Zhu, Yuyu Liu, Jiujun Zhang, Jin Yi
    Chinese Chemical Letters. 2021, 32(9): 2899-2903.

    Zinc metal has aroused increasing interest as anode material of Zn-based batteries for their energy storage application. However, the uneven Zn stripping/plating processes induce severe dendrite growth, leading to low Coulombic efficiency and safety hazards. Herein, a surface-tuned two-dimensional (2D) MXene Ti3C2T scaffold as a robust skeleton is developed to facilitate the uniform Zn stripping/plating. The Ti3C2T with high electrical conductivity and unique structure provides fast ionic-transport paths, promising even Zn2+ stripping/plating processes. With suppressed Zn dendrite growth and uniform nucleation, the proposed 2D Ti3C2T scaffold for Zn metal anode delivers a low voltage hysteresis of 63 mV and long lifespan over 280 h. This surface-tuned engineering strategy demonstrates the potential application of Zn anode with MXene skeleton for next-generation Zn-based batteries.

  • Yanhong Chang, Jing Li, Yilin Chang, Yixiao Zhang, Jianqi Zhang, Kun Lu, Xiangnan Sun, Zhixiang Wei
    Chinese Chemical Letters. 2021, 32(9): 2904-2908.

    With the emergence of non-fullerene acceptors (NFAs), the power conversion efficiencies (PCEs) of all-small-molecule organic solar cells (ASM-OSCs) have been significantly improved. However, due to the strong crystallinities of small molecules, it is much more challenging to obtain the ideal phase separation morphology and efficient charge transport pathways for ASM-OSCs. Here, a high-efficiency ternary ASM-OSC has been successfully constructed based on H11/IDIC-4F system by introduction of IDIC with a similar backbone as IDIC-4F but weak crystallinity. Notably, the addition of IDIC has effectively suppressed large-scale phase aggregation and optimized the morphology of the blend film. More importantly, the molecular orientation has also been significantly adjusted, and a mixed face-on and edge-on orientation has formed, thus establishing a more favorable three-dimensional (3D) charge pathways in the active layer. With these improvements, the enhanced short-circuit current density (JSC) and fill factor (FF) of the ternary system have been achieved. In addition, because of the high lowest unoccupied molecular orbital (LUMO) energy level of IDIC as well as the alloyed structure of the IDIC and IDIC-4F, the promoted open circuit voltage (VOC) of the ternary system has also been realized.

  • 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.

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