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  • Xiang Yuan, Zhenyuan Li, Ziming Feng, Jianshuang Jiang, Yanan Yang, Peicheng Zhang
    Chinese Chemical Letters. 2021, 32(12): 4058-4062.

    Three matrine-derived alkaloids, alopecuroidine A (1), alopecuroidine B (2a) and alopecuroidine C (2b) were isolated from the seeds of Sophora alopecuroides. Their structures were elucidated by extensive spectroscopic analyses and X-ray diffraction. Three compounds possess an unprecedented rearranged fused 7/6/5/6 tetracyclic skeleton with a diazacycloheptane structure. Their plausible biosynthetic pathway was also proposed. The anti-proliferative activities of compounds 1 and 2a were examined by the MTT assay. Compound 1 inhibited the viability of human lung cancer A549 cells, having a half maximal inhibitory concentration (IC50) of 7.58 ± 2.47 µmol/L at 72 h. The flow cytometric analysis suggested that 1 inhibited A549 cell growth by inducing apoptosis and cell-cycle arrest. Additionally, 1 induced the loss of mitochondrial membrane potential, elevated intracellular reactive oxygen species, increased the Bax/Bcl-2 ratio, stimulated cleaved-caspase-3 and P53 protein levels, and suppressed the pro-caspase-3 level. Thus, 1 appeared to induce A549 cells apoptosis through a mitochondria-mediated apoptotic pathway.

  • Shiqi Cheng, Zhao Chen, Ya Yin, Yue Sun, Shenghua Liu
    Chinese Chemical Letters. 2021, 32(12): 3718-3732.

    Photophysical properties of organic and organometallic luminophors are closely related with their molecular packings, enabling the exploitation of stimuli-responsive functional luminescent molecules. Mechanochromic molecules, which can change their luminescence characteristics after mechanical stimulus, have received an increasing interest due to their promising applications in multifunctional sensors and molecular switches. During the past two decades, the development of gold(I) chemistry has been attracting the attention of plenty of researchers. Indeed, a variety of gold(I) complexes with fascinating photophysical behaviors have been discovered. This review focuses on the research progress in the different types of mechanoluminochromic gold(I) complexes, including mono-, bi- and multi-nuclear gold(I) systems. Their interesting luminescence behaviors of these gold(I)-containing luminogens upon mechanical stimulus and the proposed mechanisms of their observed mechanochromic luminescence are summarized systematacially. Moreover, this review will put forward an outlook about the possible opportunities and challenges in this significative scientific field.

  • Lingling Yao, Defeng Zhu, Lei Wang, Jie Liu, Yicheng Zhang, Pinhua Li
    Chinese Chemical Letters. 2021, 32(12): 4033-4037.

    A visible-light-induced chemoselective reactions of quinoxalin-2(1H)-ones with alkylboronic acids in the presence of air (O2) and N2 atmosphere was developed under transition-metal free conditions, providing 3-alkylquinoxalin-2(1H)-ones and 3, 4-dihydroquinoxalin-2(1H)-ones, respectively. The overall strategy accommodates a broad scope of substituted quinoxalin-2(1H)-ones and alkylboronic acids with good to excellent product yields.

  • Ningning Li, Yi Liu, Xiaoyu Ji, Jiaxin Feng, Kai Wang, Jiayue Xie, Guanglu Lei, Xianghong Liu, Xiangxin Guo, Jun Zhang
    Chinese Chemical Letters. 2021, 32(12): 3787-3792.

    The application of Si as the anode materials for lithium-ion batteries (LIBs) is still severely hindered by the rapid capacity decay due to the structural damage caused by large volume change (> 300%) during cycling. Herein, a three-dimensional (3D) aerogel anode of Si@carbon@graphene (SCG) is rationally constructed via a polydopamine-assisted strategy. Polydopamine is coated on Si nanoparticles to serve as an interface linker to initiate the assembly of Si and graphene oxide, which plays a crucial role in the successful fabrication of SCG aerogels. After annealing the polydopamine is converted into N-doped carbon (N-carbon) coatings to protect Si materials. The dual protection from N-carbon and graphene aerogels synergistically improves the structural stability and electronic conductivity of Si, thereby leading to the significantly improved lithium storage properties. Electrochemical tests show that the SCG with optimized graphene content delivers a high capacity (712 mAh/g at 100 mA/g) and robust cycling stability (402 mAh/g at 1 A/g after 1500 cycles). Furthermore, the full cell using SCG aerogels as anode exhibits a reversible capacity of 187.6 mAh/g after 80 cycles at 0.1 A/g. This work provides a plausible strategy for developing Si anode in LIBs.

  • Tongxia Jin, Mengyu Cui, Dan Wu, Weiping Zhu, Yufang Xu, Xuhong Qian
    Chinese Chemical Letters. 2021, 32(12): 3899-3902.

    Glutathione (GSH) plays a critical role in maintaining cellular redox homeostasis in biological system. Mitochondrion is a pivotal organelle for cellular aerobic respiration and its disorder is associated with impaired redox balance, leading to cell death. In this work, we designed and synthesized a non-invasive "off-on" mitochondrial-targeting fluorescent probe QZ for the detection of GSH in living cells. Based on the mechanism of native chemical ligation (NCL) and fluorescence resonance energy transfer (FRET), a rhodamine B derivative, QZ was prepared, by choosing aromatic thioester bond as the selective reaction site. QZ exhibited excellent detection capability for GSH over Cys and Hcy. Upon addition of GSH to QZ solution, a remarkably enhanced fluorescence was observed with a limit of detection of 2.98 μmol/L. Furthermore, QZ was found to possess the specific mitochondrial localization ability in cell imaging experiments. Moreover, with exogenous and endogenous stimulations, QZ could image GSH in living cells.

  • Chi Zhang, Jingjing Jin, Ke Liu, Xuejuan Ma, Xinfeng Zhang
    Chinese Chemical Letters. 2021, 32(12): 3931-3935.

    Chemiluminescence (CL) has been widely used for bioanalysis owing to its high sensitivity, low background and simplicity. However, most of the CL systems need acidic/alkaline conditions or organic solvent to enhance their luminescent efficiency, and the non-physiological conditions can usually lead to the misfunction of biomolecules during biosensing. Herein, we report a highly luminous CL system under physiological conditions based on carbon dots-bis(2-carbopentyloxy-3, 5, 6-trichlorophenyl) oxalate (CDs-CPPO) micelles, and further used it in biosensing application. In the CL system, the amphiphilic surfactant packed CPPO and hydrophobic CDs together to form CDs-CPPO micelles. Such micelles solution not only isolated the CPPO from water to prevent its hydrolysis but also made the close proximity between CPPO and CDs, thus significantly enhancing the CDs quantum yield. The CL quantum yield was calculated to be 5.26 × 10−4 einsteins/mol, about 200-fold higher than that of the most commonly used luminol CL system. The oxidases (e.g., glucose oxidase) were tested to be susceptible to the organic solvent and non-physiological pH. Hence, the CL system was used for the detection of oxidase substrates (exemplified by glucose) in serum samples, and the limit of detection was as low as 8.4 nmol/L. The highly luminous CL system that can work under physiological conditions is promising for biosensing applications

  • Hui Yu, Xiang Wu, Qiaoqiao Mu, Zhihe Wei, Yindong Gu, Xuzhou Yuan, Yongtao Lu, Zhao Deng, Yang Peng
    Chinese Chemical Letters. 2021, 32(12): 3833-3836.

    The development of robust photocatalytic systems is key to harvest the solar power for hydrogen production. In the current study, a series of aluminum-based porphyrinic metal organic frameworks (Al-TCPP) with various morphologies of bulk, carambola-like and nanosheets are synthesized with modulated layer thickness. Morphology-dependent photocatalytic activities in hydrogen production are witnessed and inversely correlate to the thickness of the Al-TCPP micro-platelets or nanosheets. Particularly, the exfoliated metal organic layers (MOLs) of Al-TCPP demonstrated a high hydrogen yield rate of 1.32 × 104 µmol h−1 g−1 that is 21-fold of that from the bulk catalyst, as well as an exceptional TON of 6704 that seldom seen in literature. Through comprehensive photochemical characterizations, the remarkable photocatalytic performance of Al-TCPP-MOL is attributed to the great charge separation efficiency and transfer kinetics endowed by the ultrathin 2D morphology with extended active surface area.

  • Huimin Yan, Huning Yang, Jipeng Luo, Nan Yin, Zhicheng Tan, Quan Shi
    Chinese Chemical Letters. 2021, 32(12): 3825-3832.

    n-Alkanes have been widely used as phase change materials (PCMs) for thermal energy storage applications because of their exceptional phase transition performance, high chemical stability, long term cyclic stability and non-toxicity. However, the thermodynamic properties, especially heat capacity, of n-alkanes have rarely been comprehensively investigated in a wide temperature range, which would be insufficient for design and utilization of n-alkanes-based thermal energy storage techniques. In this study, the thermal properties of n-alkanes (C18H38-C22H46), such as thermal stability, thermal conductivity, phase transition temperature and enthalpy were systematically studied by different thermal analysis and calorimetry methods, and compared with previous results. Thermodynamic property of these n-alkanes was studied in a wide temperature range from 1.9 K to 370 K using a combined relaxation (Physical Property Measurement System, PPMS), differential scanning and adiabatic calorimetry method, and the corresponding thermodynamic functions, such as entropy and enthalpy, were calculated based on the heat capacity curve fitting. Most importantly, the heat capacities and related thermodynamic functions of n-heneicosane and n-docosane were reported for the first time in this work, as far as we know. This research work would provide accurate and reliable thermodynamic properties for further study of n-alkanes-based PCMs for thermal energy storage applications.

  • Fang Hu, Yao Gu, Fuhan Cui, Guihong Song, Kai Zhu
    Chinese Chemical Letters. 2021, 32(12): 3793-3798.

    Ammonium vanadate has been considered as a competitive high-performance cathode material for aqueous Zn-ion batteries. However, it still suffers from insufficient rate capability and poor cyclability due to the low electronic conductivity. Herein, (NH4)2V6O16·0.9H2O nanobelts with reduced graphene oxide (RGO) modification are synthesized by one-step hydrothermal reaction. Benefiting from the addition of RGO, an excellent electrochemical performance of (NH4)2V6O16·0.9H2O@RGO nanobelts can be obtained. The (NH4)2V6O16·0.9H2O@RGO displays a high-rate capacity and a high energy density of 386 Wh/kg at 72 W/kg. In particular, after 1000 cycles at 5 A/g, the capacity remains at 322 mAh/g with 92.8% capacity retention. In addition, the key reaction mechanisms of reversible Zn2+insertion/extraction in (NH4)2V6O16·0.9H2O@RGO are clarified.

  • Tong Guo, Xiuli Liu, Zhikun Zhang, Yiqun Luo, Tong Li, Lan Li, Huixue Wang, Yong Huang, Jian He, Qiaoying Chen, Yongxiang Zhao, Lu Gan, Liping Zhong
    Chinese Chemical Letters. 2021, 32(12): 3962-3966.

    Oncolytic virus is an emerging anti-cancer strategy. However, extracellular matrix (ECM), as a physical barrier, limits virus spread within the tumor. To overcome the obstacle, we constructed a recombinant Newcastle disease virus (NDV) expressing matrix metalloproteinase (MMP8) (NDV-MMP8) using with reverse genetic technology. In vitro, NDV-MMP8 was identified and verified by WB and ELISA. Cell viability was detected by CCK-8 assay. In vivo, we established two liver cancer xenograft models. NDV-MMP8 was injected into the tumor to observe the tumor volume and survival of mice. The changes in extracellular matrix were observed by Masson's trichrome staining. Virus expression in tumor tissues was detected by immunofluorescence assay. The virus titer in tumor tissues was detected by TCID50. Histopathological changes were detected by hematoxylin and eosin (HE) and terminal deoxynucleotidyl transferase dUTP nick end labeling (TUNEL) staining. Intratumoral administration of NDV-MMP8 can effectively degrade ECM, promote the spread of the virus within the tumor, and reduce tumor growth rate. Therefore, the method of increasing intratumoral virus accumulation by degradation of the ECM to enhance the oncolytic effect has great potential for clinical application.

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