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  • Yue Li, Nong Lu, Qitian Lin, Haobing Wang, Zhuoming Liang, Yujuan Lu, Pingyu Zhang
    Chinese Chemical Letters. 2023, 34(1): 107653-.

    Carbon monoxide (CO) gas therapy, a novel anti-tumor technique based on the cytotoxicity from the CO released in situ, has become one of the hot topics in cancer treatment. Since the technique is oxygen-independent, it displays promising therapeutic effect for hypoxic tumor where traditional photodynamic therapy shows limited efficacy and insufficient penetration depth. To fully address these limitations of PDT, we propose a synergetic sonodynamic-CO gas releasing strategy for the therapy of hypoxic tumor. In this work, two rhenium(I) tricarbonyl complexes with different substituted ligands are investigated for US-triggered ROS generation and CO release. Our results indicated that the electron-donating NMe2-substituted complex (Re-NMe2) exhibits stronger luminescence intensity and generates more singlet oxygen (1O2) than the electron-withdrawing NO2-substituted complex (Re-NO2). In addition, Re-NMe2 displays release of CO triggered by US, thus showing high sono-cytotoxicity to tumor cells in-vitro and in-vivo. The strong ROS-generating capability combined with rapid CO-releasing feature from Re-NMe2 has made it a powerful tool for the efficient treatment of hypoxic tumor.

  • Zhaoyan Tian, Xiang Qin, Fengying Shao, Xiuxiu Li, Zhi Wang, Songqin Liu, Yafeng Wu
    Chinese Chemical Letters. 2023, 34(1): 107656-.

    The coupling of bipolar electrode (BPE) arrays and electrofluorochromic (EFC) imaging has exhibited great abilities in bioanalysis. However, the imaging resolution and analytical performance are hampered by the large size of the electrode and the rapid diffusion of EFC molecules on the electrode surface. Here, to address the challenges, bipolar nanoelectrodes (BPnE) array and in situ immobilization strategy of EFC molecules were proposed. Anodized aluminum oxide (AAO) template-assisted Au nanoelectrodes array with high density was fabricated as BPnE array for high spatial imaging resolution. By electrically polymerizing EFC molecules on the surface of single Au nanoelectrode, the rapid diffusion of EFC molecules on the electrode surface was not only avoided, but also realizing electrofluorescent imaging on an individual nanoelectrode. Using dopamine (DA) released from living PC12 cells as a model, the proposed strategy exhibited an ultra-high sensitivity for DA analysis with a detection limit of 0.45 nmol/L and the DA release amount from a single cell was calculated to be 0.13 pmol/L. Moreover, the dynamic change of DA release under the drug stimulation from living PC12 cells could also be monitored.

  • Ya-Ling Wang, Kang Chen, Hai-Ru Li, Bo Chu, Zishan Yan, Hao-Ke Zhang, Bin Liu, Shengliang Hu, Yongzhen Yang
    Chinese Chemical Letters. 2023, 34(1): 107684-.

    Developing non-conjugated luminescent polymers (NCLPs) with fluorescence and long-lived room-temperature phosphorescence is of great significance for revealing the essence of NCLPs luminescence, which has gradually attracted the attention of researchers in recent years. Herein, polymethylol (PMO) and poly(3-butene-1, 2-diol) (PBD) with polyhydroxy structures were prepared and their luminescence behaviors were investigated to reveal the clusteroluminescence (CL) mechanism. Compared with polyvinyl alcohol with non-luminescent behavior, PMO and PBD exhibit cyan-blue fluorescence with quantum yields of ca. 12% and green room-temperature phosphorescence with lifetimes of ca. 89 ms in the solid state. Both fluorescence and phosphorescence exhibit typical excitation-dependent CL behavior. Experimental and theoretical analyses show that the strong hydrogen-bonding interaction of PMO and PBD greatly promotes the formation of oxygen clusters and the through-space n-n interaction of oxygen atoms, enabling fluorescence and phosphorescence emission. Our results have enormous implications for understanding the CL mechanism of NCLPs and provide a new polymer design strategy for the rational design of novel NCLPs materials.

  • Hui Chen, Xinye Ma, Xinyu Zhang, Gui Hu, Yan Deng, Song Li, Zhu Chen, Nongyue He, Yanqi Wu, Zhihong Jiang
    Chinese Chemical Letters. 2023, 34(1): 107701-.

    The SARS-CoV-2 virus is released from an infectious source (such as a sick person) and adsorbed on aerosols, which can form pathogenic microorganism aerosols, which can affect human health through airborne transmission. Efficient sampling and accurate detection of microorganisms in aerosols are the premise and basis for studying their properties and evaluating their hazard. In this study, we built a set of sub-micron aerosol detection platform, and carried out a simulation experiment on the SARS-CoV-2 aerosol in the air by wet-wall cyclone combined with immunomagnetic nanoparticle adsorption sampling and ddPCR. The feasibility of the system in aerosol detection was verified, and the influencing factors in the detection process were experimentally tested. As a result, the sampling efficiency was 29.77%, and extraction efficiency was 98.57%. The minimum detection limit per unit volume of aerosols was 250 copies (102 copies/mL, concentration factor 2.5).

  • Huimin Chu, Haoyang Zheng, Aizhu Miao, Chunhui Deng, Nianrong Sun
    Chinese Chemical Letters. 2023, 34(1): 107716-.

    Phosphorylation plays crucial parts in lenticular biological function. Getting knowledge of region-resolved phosphoproteome contributes to better comprehending the pathogenesis. Here, we prepared the hybrid metal organic frameworks (HMOFs) for probing the region-resolved heterogeneity of phosphoproteome in human lens. 1334 phosphosites corresponding to 564 phosphoproteins, 1160 phosphosites corresponding to 316 phosphoproteins and 517 phosphosites corresponding to 205 phosphoproteins were identified in capsule, cortex and nucleus, respectively, providing the relatively extensive distribution mapping of phosphorylation in human lens for the first time. The label-free quantification experiments and principal component analysis presented differential expression of phopshoproteins in three subregions. For instance, α-crystallin, β-crystallin and fibrillin-1 closely associated with cataract and Marfan syndrome showed disparate spatial distribution. The preferential phosphoproteins in capsule, cortex and nucleus were involved in cytoskeleton organization, metabolic process and lens development in camera-type eye, respectively. This work first provided a general overview of region-resolved phosphoproteome of human lens.

  • Haixin Zhang, Jingrong Li, Jinguang Si, Chengya Dong, Qi Li, Meng Yu, Lingling Qin, Lingyu Li, Chenxu Zhao, Tao Zhang, Zhongmei Zou
    Chinese Chemical Letters. 2023, 34(1): 107743-.

    Three eudesmanolide sesquiterpene-phenol hybrids, atramacronoids A−C (1−3), featuring an unusual 6/6/5/5/6 skeleton furnished by forming an unexpected C-8−C-16 linkage, were obtained from the rhizomes of Atractylodes macrocephala. Their structures and absolute configurations were elucidated by spectroscopic data analysis, chemical calculations, combined with X-ray diffractions. The plausible biosynthetic pathways for compounds 1−3 are proposed. Surprisingly, compound 1 exhibited cytotoxicity against SGC-7901 cells by inducing cells apoptosis, which might relate to the promotion of synthesis of neutrophil elastase.

  • Fang-Fang Shen, Yuguo Wang, Leyong Wang
    Chinese Chemical Letters. 2023, 34(1): 107761-.
  • Mingjun Zhong, Qimeng Wu, Liang Ma, Jie Li, Yifan Wang, Yansong Wang, Xin Li, Yajie Zhang, Jingtao Lü, Yongfeng Wang
    Chinese Chemical Letters. 2023, 34(1): 107813-.

    Spin properties of organic molecules have attracted great interest for their potential applications in spintronic devices and quantum computing. Fe-tetraphenyl porphyrin (FeTPP) is of particular interest for its robust magnetic properties on metallic substrates. FeTPP is prepared in vacuum via on-surface synthesis. Molecular structure and spin-related transport properties are characterized by low-temperature scanning tunneling microscope and spectroscopy at 0.5 K. Density functional theory calculations are performed to understand molecular adsorption and spin distribution on Au(111). The molecular structure of FeTPP is distorted upon adsorption on the substrate. Spin excitations of FeTPP are observed on the Fe atom and high pyrrole groups in differential conductance spectra. The calculated spin density distribution indicates that the electron spin of FeTPP is mainly distributed on the Fe atom. The atomic transmission calculation indicates that electrons transport to substrate is mediated through Fe atom, when the tip is above the high pyrrole group.

  • Chinese Chemical Letters. 2023, 34(1): 107937-.
  • Zexian Li, Jianfeng Zheng, Wei-Dong Z. Li
    Chinese Chemical Letters. 2022, 33(12): 4957-4968.

    Taxol is one of the most famous diterpenoid natural products used in clinical cancer therapy. Taxol and its analogues are popular synthetic targets and have attracted worldwide attention over the past decades. Tremendous research efforts have already been made and ten groups have achieved the total synthesis of Taxol since 1994. This mini-review summarized the recent highlights of divergent strategic approaches towards the chemical synthesis of Taxol's carbocyclic framework bearing a bridged eight-membered ring.

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