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  • Yanru Zhu, Minghuan Yang, Zhen Zhang, Zhe An, Jian Zhang, Xin Shu, Jing He
    Chinese Chemical Letters. 2022, 33(4): 2069-2072.

    Supported NiCu bimetallic catalysts have been produced in-situ on commercial Al2O3 by using layered double hydroxides as precursors. The resulting catalysts show a uniform Ni and Cu distribution, thus providing good activity and selectivity in the reforming reaction of n-heptane. The catalytic performance has been found to depend on the Cu/Ni ratio, revealing the synergic catalysis between homogeneously dispersed Ni and Cu sites. The good catalysis of NiCu bimetallic catalysts makes it possible to partly or even completely replace Pt with NiCu bimetallic catalysts.

  • Juan Wang, Yuwei Sheng, Ying Yang, Xiaoxia Dai, Changjun You
    Chinese Chemical Letters. 2022, 33(4): 2077-2080.

    N6-methyldeoxyadenosine (6mdA) modification is considered as a new epigenetic mark that may play important roles in various biological processes. However, it remains unclear about the effect of 6mdA on DNA replication in human cells. Herein, we combined next-generation sequencing with shuttle vector technology to explore how 6mdA affects the efficiency and accuracy of DNA replication in human cells. Our results showed that 6mdA neither blocked DNA replication nor induced mutations in human cells. Moreover, we found that the depletion of translesion synthesis DNA polymerase (Pol) κ, Pol η, Pol ι or Pol ζ did not significantly change the biological consequences of 6mdA during replication in human cells. The negligible impact of 6mdA on DNA replication is consistent with its potential role in epigenetic gene expression.

  • Chun-Lan Xie, Duo Zhang, Kai-Qiang Guo, Qing-Xiang Yan, Zheng-Biao Zou, Zhi-Hui He, Zhen Wu, Xiao-Kun Zhang, Hai-Feng Chen, Xian-Wen Yang
    Chinese Chemical Letters. 2022, 33(4): 2057-2059.

    A novel meroterpenoid, named meroterpenthiazole A (1), was isolated from the deep-sea-derived Penicillium allii-sativi. Its structure was established by extensive spectroscopic and computational methods. Meroterpenthiazole A bears a rare benzothiazole moiety in nature. Compound 1 significantly inhibited retinoid X receptor (RXR)-α transcriptional effect (KD = 12.3 µmol/L) through a novel binding mechanism.

  • Hui Zhao, Rakesh Kumar Gupta, Wei Zhang, Jiong Jia, Qun Yu, Zhiyong Gao, Guilin Zhuang, Dacheng Li, Xingpo Wang, Chen Ho Tung, Di Sun
    Chinese Chemical Letters. 2022, 33(4): 2047-2051.

    The construction of all-carbon molecule frameworks remains challenging. Herein, we report a facile and efficient one-pot synthesis of a novel all-carbon stair containing dimerized pentalene core using inexpensive cyclopropyl alkyne catalyzed by in situ generated Cu(I) from the comproportionation reaction of Cu(II) salt and Cu powder under mild reaction conditions. The reaction proceeds via sequential acetylenic coupling, followed by cyclization and [2 + 2] cycloaddition to directly produce pentalene dimer, which is difficult to access by other established methods. Different mechanistic paths were studied for the pentalene formation using density functional theory, suggesting that the reaction also proceeds through acetylenic coupling followed by cyclization and [2 + 2] cycloaddition. Based on the activation energy barriers, Path 1 has the rate-determining step of 38.63 kcal/mol, which is the most thermodynamically preferred one among the four paths.

  • Yue Zhao, Xiaoxing Fang, Min Bai, Jin Zhang, Huahang Yu, Feng Chen, Yongxi Zhao
    Chinese Chemical Letters. 2022, 33(4): 2101-2104.

    Exosomal microRNA (miRNA) is an ideal candidate of noninvasive biomarker for the early diagnosis of cancer. Sensitive and accurate sensing of abnormal exosomal miRNA plays essential role for clinical promotion due to its close correlation with tumor proliferation and progression. Herein, a microfluidic surface-enhanced Raman scattering (SERS) sensor was proposed for an on-line detection of exosomal miRNA based on rolling circle amplification (RCA) and tyramine signal amplification (TSA) strategy. The microfluidic chip consists of a magnetic enrichment chamber, a serpentine fluidic mixer and a plasmonic SERS substrate functionalized with capture probes. The released miRNA activates the capture probe, triggers RCA reaction, and generates a large number of single-stranded DNA products to drive the catalysis of nanotags deposition via TSA, producing numerous phot spotsq to enhance the SERS signals. In merit of the microfluidics chip and nucleic acid-tyramine cascade amplification, the developed SERS sensor significantly improves the sensitivity for the exosomal miRNA assay, resulting in a limit of detection (LOD) as low as 1 pmol/L and can be successfully applied in the analysis of exosomes secreted from breast tumor cells, which demonstrates the potential utility in practical applications.

  • 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.

  • Longjie Li, Kejun Dong, Xinyu Wang, Meizhou Zhang, Jun Li, Andreas K. Nussler, Xianjin Xiao, Hongbo Wang, Yuzhou Wu
    Chinese Chemical Letters. 2022, 33(4): 2052-2056.

    Point mutations can be used as biomarkers to perform diagnosis for diseases. In this study, a nanorobot for low-abundance point mutation enrichment was constructed using DNA origami. The novel design achieved limits of detection of 0.1% and 1% for synthesized DNA samples and clinical gene samples, respectively. Resettability was a key property of this method, which also involved a simpler process, lower cost and shorter detection duration than traditional enrichment methods. This novel DNA nanorobot may enable the detection of tumor markers, potentially facilitating early cancer diagnosis.

  • Xiaoting Huo, Lei Wang, Wuzhen Qi, Na Rong, Yingjia Liu, Siyuan Wang, Hong Duan, Jianhan Lin
    Chinese Chemical Letters. 2022, 33(4): 2091-2095.

    Foodborne pathogenic bacteria have been considered as a major risk factor for food safety. It is of great significance to carry out in-field screening of pathogenic bacteria to prevent the outbreaks of foodborne diseases. In this study, a portable lab-on-a-disc platform with a microfluidic disc was developed for rapid and automatic detection of Salmonella typhimurium using a nickel nanowire (NiNW) net for effective separation of target bacteria, horseradish peroxidase nanoflowers (HRP NFs) for efficient amplification of biological signals, and a self-developed smartphone APP for accurate analysis of colorimetric images. First, the microfluidic disc was preloaded with reagents and samples and centrifuged to form one bacterial sample column, one immune NiNW column, one HRP NF column, two washing buffer columns and one tetramethylbenzidine (TMB) column, which were separated by air gaps. Then, a rotatable magnetic field was specifically developed to assemble the NiNWs into a net, which was automatically controlled by a stepped motor to successively pass through the sample column for specific capture of target bacteria, the HRP NF column for specific label of target bacteria, the washing columns for effective removal of sample background and non-specific binding NFs, and the TMB column for colorimetric determination of target bacteria. The color change of TMB from colorless to blue was finally analyzed using the smartphone APP to quantitatively determine the target bacteria. This lab-on-a-disc platform could detect Salmonella typhimurium from 5.6×101 CFU/20 μL to 5.6×105 CFU/20 μL in 1 h with a lower detection limit of 56 CFU/20 μL. The recovery of target bacteria in spiked chicken samples ranged from 97.5% to 101.8%. This portable platform integrating separation, labeling, washing, catalysis and detection onto a single disc is featured with automatic operation, fast reaction, and small size and has shown its potential for in-field detection of foodborne pathogens.

  • Gaorong Wu, Xiaobo Xu, Shuai Wang, Lu Chen, Binghan Pang, Tao Ma, Yafei Ji
    Chinese Chemical Letters. 2022, 33(4): 2005-2008.

    A novel method for metal-free C-H borylation of 2-(N-methylanilino)-5-fluoropyridines and 2-benzyl-5-fluoropyridines has been reported. The 5-fluoropyridine directed borylation reaction exhibited high efficiency and site exclusivity. The useful protocol could be executed on a gram-scale easily and the borylated products showed good derivatization applications. Moreover, the practicality of the strategy was expanded by the fact that the directing group could be removed in an acceptable yield.

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