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  • Ran Li, Can-Can Zhang, Dan Wang, Yan-Fang Hu, Yong-Long Li, Wei Xie
    Chinese Chemical Letters. 2021, 32(9): 2846-2850.

    Gold nanoparticles (Au NPs) are nanoscale sources of light and electrons, which are highly relevant for their extensive applications in the field of photocatalysis. Although a number of research works have been carried out on chemical reactions accelerated by the energetic hot electrons/holes, the possibility of reaction pathway change on the plasmonic Au surfaces has not been reported so far. In this proof-of-concept study, we find that Au NPs change the reaction pathway in photooxidation of alkyne under visible light irradiation. This reaction produces benzil (-CO-CO-) without the presence of Au NPs. In contrast, as indicated by surface-enhanced Raman spectroscopic (SERS) results, the C-C triple bonds (-C≡C-) adsorbed on Au NPs are converted into carboxyl (-COOH) and acyl chloride (-COCl) groups. The plasmonic Au NPs not only provide energetic charge carriers but also activate the reactant molecules as conventional heterogeneous catalysts. This study discloses the second role of plasmonic NPs in photocatalysis and bridges the gap between plasmon-driven and conventional heterogeneous catalysis.

  • 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.

  • Yongbin Zhang, Yu Zhang, Yongkang Yue, Jianbin Chao, Fangjun Huo, Caixia Yin
    Chinese Chemical Letters. 2021, 32(9): 2873-2876.
  • Hongen Cao, Ruonan Ma, Sainan Chu, Juqun Xi, Lei Yu, Rong Guo
    Chinese Chemical Letters. 2021, 32(9): 2761-2764.

    Selenium doped carbon (Se/C), an easily fabricated material, was found to be bio-active and it can serve as an adjuvant to enhance the immune effect of Tween 80/Brij 30 (T80/B30) vesicles and Tween 80/polymer cationic surfactant PN320 (T80/PN320) mixed micelles. The synergistic effect of the combination of T80/B30 vesicles and T80/PN320 mixed micelles with Se/C on nasal mucosal immunity was studied in this work, which might provide theoretical basis for developing the related new adjuvant for nasal immunization of recombinant protein, peptide and split protein vaccine. Since both selenium and carbon were bio-compatible elements, Se/C might be safe for practical applications, and this was also reflected by the low hemolytic activity of the materials. This work not only reports an efficient protocol for adjuvant development, but also significantly expands the application scope of selenium chemistry.

  • 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.

  • 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).

  • Sheng Guo, Huiling Tang, Liming You, Huali Zhang, Jun Li, Kun Zhou
    Chinese Chemical Letters. 2021, 32(9): 2828-2832.

    A mesoporous cobalt aluminate (CoAl2O4) spinel is synthesized through a combustion method and adopted for the activation of peroxymonosulfate (PMS) to degrade organic pollutants. Multiple characterization procedures are conducted to investigate the morphology and physicochemical properties of the CoAl2O4 spinel. Due to its mesoporous structure, large surface area, and high electrical conductivity, the obtained CoAl2O4 exhibits remarkable catalytic activity for Rhodamine B (RhB) degradation. Its RhB degradation rate is 89.0 and 10.5 times greater than those of Co3O4 and CoAl2O4 spinel prepared by a precipitation method, respectively. Moreover, the mesoporous CoAl2O4 spinel demonstrates a broad operating pH range and excellent recyclability. The influence of several parameters (catalyst amount, PMS concentration, initial pH, and coexisting inorganic anions) on the oxidation of RhB is evaluated. Through quenching tests and electron paramagnetic resonance experiments, sulfate radicals are identified as the predominant reactive species in RhB degradation. This paper provides new insights for the development of efficient, stable, and reusable cobalt-based heterogeneous catalysts and promotes the application of persulfate activation technology for the treatment of refractory organic wastewater.

  • 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.

  • Nan Hao, Yu Qiu, Jinwen Lu, Xu Han, Yaqi Li, Jing Qian, Kun Wang
    Chinese Chemical Letters. 2021, 32(9): 2861-2864.

    All-inorganic perovskite quantum dots (QDs) have attracted great interests due to its outstanding properties. But their poor stability in polar solvents seriously hampered wide applications in analytical chemistry. In this work, strong, stable and flexibly regulated the electrochemiluminescence (ECL) emission form CsPbBr3 QDs was successfully obtained and applied in the analysis of polar solvents through the unique structure of closed bipolar electrode (BPE). To demonstrate the feasibility, it was successfully used in the detection of tetracycline (Tc) aqueous solution. CsPbBr3 QDs was immersed into organic solution in anode microcell of closed BPE while Tc aqueous solution was added into cathode microcell. The two microcells were physically separated and would not interfere with each other. But the bio-recognition event between aptamer and Tc in cathode microcell would induce the ECL signal change in anode microcell through the electrons conducted by BPE as the bridge. The ECL emission can be flexibly regulated by environmental factors of both polar and non-polar solvents and the interface status of the BPE. Compared with traditional methods to overcome the intrinsic instability in polar medium, the reported method does not need any further surface modifications, has no limitations on the targets and can provide wide development space for further deep research, which may open a new direction for the ECL sensing of CsPbBr3 QDs.

  • 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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