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  • Wanting Hu, Dan Gao, Zhaochen Su, Rui Qian, Yu Wang, Qionglin Liang
    Chinese Chemical Letters. 2022, 33(4): 2096-2100.

    Colorectal cancer (CRC) is still the leading cause of cancer death worldwide, but the clinical effect of drug therapy such as irinotecan is not an ideal way at present. In recent years, probiotics have attracted much attention, and the combination of probiotics may play an important role in the prevention and treatment of CRC. This work proposed a cellular chip-MS system, to study the synergistic effects of probiotic Lactobacillus rhamnosus GG (L.GG) and irinotecan on HCT116 cells by cell viability and on-line mass spectrometry (MS) analysis. The double-layer chip sandwiched with a polycarbonate membrane can co-culture HCT116 cells and L.GG. And the solid phase microextraction chip can be used for desalination and concentration. Finally, the extracted chemicals were entered the electrospray ionization quadrupole time-of-flight MS to detect irinotecan metabolites. The results showed that with the increasing concentration of co-cultured L.GG, the percentage of living HCT116 cells decreased, but the relative amount of metabolized SN-38 by HCT116 cells increased. Therefore, the microfluidic system can be used to detect and monitor the synergistic effect of irinotecan-L.GG combination on HCT116 cells. In summary, our study provided experimental evidence for the first time with potential applications of irinotecan-L.GG combination in CRC treatment, and the cellular chip-MS system as a powerful tool can be used in the experiments of probiotics as new drugs.

  • Meng-Yuan Chen, Zhu Gui, Ke-Ke Chen, Jiang-Hui Ding, Jin-Gang He, Jun Xiong, Jia-Le Li, Jie Wang, Bi-Feng Yuan, Yu-Qi Feng
    Chinese Chemical Letters. 2022, 33(4): 2086-2090.

    Alcohol consumption is a critical risk factor contributing to a verity of human diseases. The incidence of alcohol use disorder increases across adolescence in recent years. Accumulating line of evidence suggests that alcohol-induced changes of DNA cytosine methylation (5-methyl-2'-deoxycytidine, 5mC) in genomes play an important role in the development of diseases. However, systemic investigation of the effects of adolescent alcohol exposure on DNA and RNA modifications is still lacked. Especially, there hasn't been any report to study the effects of alcohol exposure on RNA modifications. Similar to DNA modifications, RNA modifications recently have been identified to function as new regulators in modulating numbers of biological processes. In the current study, we systematically investigated the effects of alcohol exposure on both DNA and RNA modifications in peripheral blood of adolescent rats by liquid chromatography-electrospray ionization-tandem mass spectrometry (LC-ESI-MS/MS) analysis. The developed LC-ESI-MS/MS method enabled the sensitive and accurate determination of 2 DNA modifications and 12 RNA modifications. As for the alcohol exposure experiments, the adolescent rats were intraperitoneally injected with ethanol with an interval of one day for a total 14 days. The quantification results by LC-ESI-MS/MS analysis showed that adolescent alcohol exposure could alter both DNA and RNA modifications in peripheral blood. Specifically, we observed an overall decreased trend of RNA modifications. The discovery of the significant alteration of the levels of DNA and RNA modifications under alcohol exposure indicates that alcohol consumption may increase the risk of the incidence and development of diseases through dysregulating DNA and RNA modifications.

  • Tian Wang, Jianjun Zhou, Wenjuan Wang, Yunqing Zhu, Junfeng Niu
    Chinese Chemical Letters. 2022, 33(4): 2121-2124.

    In this study, Ag0.23/(S1.66-N1.91/TiO2-x) single-atom photocatalyst was synthesized by in-situ photo-reducing of silver on S, N-TiO2-x nanocomposite and used to degrade bisphenol A (BPA) through heterogeneous activation of potassium peroxymonosulfate (PMS) under visible-light illumination. The structure, physicochemical property, morphology, and electronic property were evalutated by X-ray diffraction (XRD), Raman spectrum, X-ray photoelectron spectra (XPS), high-resolution transmission electron microscopy (HR-TEM), UV–vis diffuse reflectance spectra (UV-vis DRS), electron paramagnetic resonance (EPR) spectrum. Ag0.23/(S1.66-N1.91/TiO2-x) single-atom photocatalyst exhibited 2.4 times higher activity for the synergetic degradation of BPA than that of its counterpart, and 48.73% mineralization rate of BPA also achieved. It was ascribed to the uniformly-dispersed metallic Ag atoms as the active site for accelerating the migration rate of photo-generated carrier for generation of high reactive radicals. The EPR experiments indicated that SO4•‒ and OH was jointly involved in BPA degradation.

  • Mengjuan Yang, Hao Cheng, Yuqiu Xu, Mengzhen Li, Yong Ai
    Chinese Chemical Letters. 2022, 33(4): 2143-2146.

    Owing to the diversity of structure and potential applications in the field of electrics, sensors, and light-emitting diodes, lead halide perovskites have attracted great attention in recent years. Especially those lead halide perovskites with non-centrosymmetric crystal structures usually exhibit nonlinear optical (NLO) characteristics, which may endow them photoelectricity switching functionality. In this work, a lead-based hybrid organic-inorganic perovskite (HOIP) material, trimethyliodomethylammonium lead trichloride (TMIM·PbCl3), is obtained on the basis of tetramethylammonium lead chloride through halogen substitution on the cation part. It shows dual-phase-transition behavior around 345 and 358 K, which is significantly improved. TMIM·PbCl3 crystallizes in the chiral space group, P212121, and shows a well-defined second harmonic generation (SHG) response, and good switching endurance, which makes it an excellent candidate for SHG switching material. This work highlights the importance of halogen substitution for crystal engineering and may pave way for the further exploration of the optoelectronic devices.

  • Siyi Rong, Pengcheng Su, Shizheng Chen, Miaomiao Jia, Wanbin Li
    Chinese Chemical Letters. 2022, 33(4): 2134-2138.

    Metal-organic frameworks (MOFs) show great potential for various applications, but many of them suffer from the drawbacks of hydrolysis propensity and poor processability. Herein, we employ polymers of intrinsic microporosity (PIMs) with hydrophobic pores to decorate MOFs toward substantially improved water stability and shapeability. Through simple PIM-1 decoration, the sub-5 nm polymer layers can be uniformly deposited on MOF surfaces with almost no deterioration in porosity. Owing to the existence of superhydrophobic coating and the obstruction of water entrance into MOFs, the PIM-1 coated CuBTC exhibits impressive water resistance and excellent pore preservation ability after exposure in water, even in acidic and alkaline solutions. Moreover, polymer decoration improves the processability of MOFs, while various MOF/PIM-1 bulk wafers and oil-water separators can be obtained straightforwardly.

  • Xiaoyue Zhang, Yong Yang, Lijun Xiong, Tianyu Wang, Zheng Tang, Panjie Li, Nan Yin, Aiwu Sun, Jinyou Shen
    Chinese Chemical Letters. 2022, 33(4): 2111-2116.

    Developing photocatalyst with high activity, superior stability and prominent selectivity for CO2 conversion is of great importance for the target of carbon neutralization. Herein, 3D dahlia-like NiAl-LDH/CdS heterosystem is developed through in-situ decoration of exfoliated CdS nanosheets on the scaffold of NiAl-LDH and the on-spot self-assembly. The formation of a hierarchical architecture collaborating with well-defined 2D/2D interfacial interaction is constructed by optimizing the ratio of CdS integrated in the formation of the heterojunction. The light-harvesting capacity of NiAl-LDH/CdS is improved by this unique scaffold, and the charge transfer between NiAl-LDH and CdS is effectively facilitated by virtue of the unique 2D/2D interface. As a result, the 3D hierarchical NiAl-LDH/CdS heterosystem presents 12.45µmol g−1 h−1 of CO production (3.3 and 1.6 folds of pristine NiAl-LDH and CdS) with 96% selectivity and superior stability. This 3D hierarchical design collaborating with 2D/2D interfacial interaction provides a new avenue to develop ideal catalysts for artificial photosynthesis.

  • Shuo Liu, Xinyu Tian, Xiansheng Zhang, Chongzhi Xu, Lili Wang, Yanzhi Xia
    Chinese Chemical Letters. 2022, 33(4): 2205-2211.

    Conductive hydrogels have attracted considerable attention owing to their potential for use as electronic skin and sensors. However, the loss of the inherent elasticity or conductivity in cold environments severely limits their working conditions. Generally, organic solvents or inorganic salts can be incorporated into hydrogels as cryoprotectants. However, their toxicity and/or corrosive nature as well as the significant water loss during the solvent exchange present serious difficulties. Herein, a liquid-like yet non-toxic polymer-polyethylene glycol (PEG) was attempted as one of the components of solvent for hydrogels. In the premixed PEG-water hybrid solvent, polyacrylamide (PAAm) was in situ polymerized, overcoming the inevitable water loss induced by the high osmotic pressure of the PEG solution and achieving tailored water capacity. Interestingly, the mechanical strength ("soft-to-rigid" transition) and anti-freezing properties of organohydrogels can be simultaneously tuned over a very wide range through adjusting PEG content. This was due to that with increasing PEG in solvent, the PAAm chains transformed from stretching to curling conformation, while PEG bonded with water molecules via hydrogen bonds, weakening the crystallization of water at subzero temperature. Additionally, a highly conductive Ti3C2Tx-MXene was further introduced into the organohydrogels, achieving a uniform distribution triggered by the attractive interaction between the rich functional groups of the nanofillers and the polymer chains. The nanocomposite hydrogels demonstrate high electrical conductivity and strain sensitivity, along with a wide working temperature window. Such a material can be used for monitoring human joint movement even at low temperature and has potential applications in wearable strain sensors.

  • Daoshan Yang, Qiuli Yan, Enjie Zhu, Jian Lv, Wei-Min He
    Chinese Chemical Letters. 2022, 33(4): 1798-1816.

    The development of green and convenient methods for C–S bond formation has received significant attention because C–S bond widely occurs in many important pharmaceutical and biological compounds. Recently, visible-light photoredox catalysis has been established as an efficient and general tool for the construction of C–C and C-heteroatom bonds. In this review, we have focused on the research on recent advances in C–S bond formation via visible-light photoredox catalysis, and the growing opportunities they present to the construction of complex chemical scaffolds for applications encompassing bioactive molecules synthesis, synthetic methodology development, and sulfur-containing drugs. We hope that this review will provide chemists with a synthetic tool that will open the door to further development of organsulfur chemistry

  • Hongdou Zhang, Jun Xu, Yani Ouyang, Xiaoguang Yue, Chenxin Zhou, Zhigang Ni, Wanmei Li
    Chinese Chemical Letters. 2022, 33(4): 2036-2040.

    Herein, an efficient molecular oxygen-mediated method for the selective hydroxyalkylation and alkylation of quinoxalin-2(1H)-ones with alkylboronic acids under transition-metal free conditions has been developed. This strategy demonstrates a broad scope of quinoxalin-2(1H)-ones and alkylboronic acids, giving 3-hydroxyalkylquinoxalin-2(1H)-ones and 3-alkylquinoxalin-2(1H)-ones in moderate-to-good yield. Control experiments reveal that a radical pathway is involved.

  • Jiayi Zhu, Ai Ouyang, Zhuanglin Shen, Zhihao Pan, Samya Banerjee, Qianling Zhang, Yantao Chen, Pingyu Zhang
    Chinese Chemical Letters. 2022, 33(4): 1907-1912.

    Metal-based compounds with excellent photo-physical properties show good photochemotherapeutic performance. But, low in-depth tissue penetration of light limits their effectivity for deeply buried tumors. Encouraged by the sonosensitizing ability of the traditional organic photosensitizers, here, we developed AuNPs@Ir1 as a sonosensitizer by hybridizing an organometallic Ir(Ⅲ) complex (Ir1) with ultrasmall gold nanoparticles (AuNPs) for efficient tumor sonodynamic therapy (SDT) for the first time. AuNPs@Ir1 rapidly entered the cancer cells, produced 1O2, and catalytically oxidized NADH to NAD+ under ultrasound (US) irradiation, thus resulted in cancer cells oncosis. Because of efficient passive retention in tumors post intravenous injection, AuNPs@Ir1 further efficiently inhibited the growth of tumors in-vivo under US stimulation without long-term toxicity to other organs. Overall, this work presents the excellent US triggered in-vitro and in-vivo anticancer profile of the novel AuNPs@Ir1. It is expected to increase the scope of SDT for metal-based anticancer drugs.

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