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  • 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.

  • Jihong Zhang, Yuchen Wang, Hongjuan Wang, Dichang Zhong, Tongbu Lu
    Chinese Chemical Letters. 2022, 33(4): 2065-2068.

    Metal-organic frameworks (MOFs) as a type of crystalline heterogeneous catalysts have shown potential application in photocatalytic CO2 reduction. However, MOF catalysts with high efficiency and selectivity are still in pursuit. Herein, by a bimetallic strategy, the catalytic performance of a Co-MOF for photocatalytic CO2 reduction was enhanced. Specifically, the Co-MOF based on 4, 5-dicarboxylic acid (H3IDC) and 4, 4ʹ-bipydine (4, 4ʹ-bpy) can catalyze CO2 reduction to CO, with high efficiency but relatively low selectivity. After replacement of 2/3 Co(Ⅱ) with Ni(Ⅱ) within Co-MOF, the resulted isostructural Co1Ni2-MOF not only retains high efficiency for photocatalytic CO2 reduction, but also shows enhanced CO selectivity. The CO evolution rate reaches 1160 µmol g−1 h−1 and the CO selectivity reaches as high as 94.6%. The enhanced photocatalytic CO2 reduction performance is supported by theoretical calculation results. This case demonstrates that bimetallic strategy is an effective mean to optimize the catalytic performance of MOF catalysts for photochemical CO2 reduction.

  • 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.

  • Yi-Teng Yan, Gang Wu, Si-Chong Chen, Yu-Zhong Wang
    Chinese Chemical Letters. 2022, 33(4): 2151-2154.

    Herein, we presented a novel biodegradable copolymer via the chain extending reaction of poly(p-dioxanone)-co-poly(2-(2-hydroxyethoxy) benzoate) (PPDO-co-PDHB) prepolymer with hexamethylene diisocyanate (HDI) as a chain extender. The structures and molecular weight of PPDO-co-PDHB prepolymer and PPDO-co-PDHB-PU chain-extended copolymer are characterized via hydrogen nuclear magnetic resonance spectroscopy (1H NMR) and viscosity test. The relationship between the molecular structures and properties of the chain-extended copolymers is established. The PPDO-co-PDHB-PU copolymers possess a better thermal stability comparing with the PPDO homopolymer. The study of mechanical properties shows that the elongation-at-break of PPDO-co-PDHB-PU is much higher than that of PPDO. The investigation of hydrolytic degradation behaviors indicates the degradation rate of PPDO can be controlled by adjusting the PDHB compositions, and proves that chain-extended copolymers exhibit an excellent hydrolytic stability being better than that of PPDO.

  • Qiao Song, Yan Liu, Linlin Cai, Xinyu Cao, Shan Qian, Zhouyu Wang
    Chinese Chemical Letters. 2022, 33(4): 2212-2212.
  • Chengdu Qi, Yanni Wen, Yijie Zhao, Yinhao Dai, Yanping Li, Chenmin Xu, Shaogui Yang, Huan He
    Chinese Chemical Letters. 2022, 33(4): 2125-2128.

    The difficulty in Fe(Ⅲ)/Fe(Ⅱ) conversion in the Fe(Ⅲ)/peroxymonosulfate (PMS) process limits its efficiency and application. Herein, l-cysteine (Cys), a green natural organic ligand with reducing capability, was innovatively introduced into Fe(Ⅲ)/PMS to construct an excellent Cys/Fe(Ⅲ)/PMS process. The Cys/Fe(Ⅲ)/PMS process, at room temperature, can degrade a variety of organic contaminants, including dyes, phenolic compounds, and pharmaceuticals. In subsequent experiments with acid orange 7 (AO7), the AO7 degradation efficiency followed pseudo-first-order kinetic which exhibited an initial "fast stage" and a second "slow stage". The rate constant values ranged depending on the initial Cys, Fe(Ⅲ), PMS, and AO7 concentrations, reaction temperature, and pH values. In addition, the presence of Cl, NO3, and SO42− had negligible impact while HCO3 and humic acid inhibited the degradation of AO7. Furthermore, radical scavenger experiments and methyl phenyl sulfoxide (PMSO) transformation assay indicated that sulfate radical, hydroxyl radical, and ferryl ion (Fe(Ⅳ)) were the dominant reactive species involved in the Cys/Fe(Ⅲ)/PMS process. Finally, based on the results of gas chromatography-mass spectrometry, several AO7 degradation pathways, including N=N cleavage, hydroxylation, and ring opening were proposed. This study provided a new insight to improve the efficiency of Fe(Ⅲ)/PMS process by accelerating Fe(Ⅲ)/Fe(Ⅱ) cycle with Cys.

  • Yaqi Hou, Qianxiao Wang, Shuli Wang, Miao Wang, Xuemei Chen, Xu Hou
    Chinese Chemical Letters. 2022, 33(4): 2155-2158.

    Carbon nanotube-based (CNT-based) interfacial evaporation material is one of the most potential materials for solar desalination. Here, we studied the evaporation rate of the CNT-based membranes with different hydrophilic and hydrophobic chemical modified surfaces using molecular dynamic simulations. We found that the hydrogen bonding density among water molecules at the interface is a key factor in enhancing the evaporation rate. For a hydrophilic CNT-based membrane, the strong interactions between the membrane outer surface and the water molecules can destroy the water-water hydrogen bonding interactions at the interface, resulting in the reduction of the hydrogen bonding density, leading to an enhancement effect in evaporation rate. We also found that there is an optimal thickness for evaporation membrane. These findings could provide some theoretical guidance for designing and exploring advanced CNT-based systems with more beneficial performance in water desalination.

  • Tianyi Zhou, Yanlu Mu, Jianyang Wu, Bing Zhong, Chengkai Yang, Qian Wang, Wen Liu, Henghui Zhou, Peng Jiang
    Chinese Chemical Letters. 2022, 33(4): 2165-2170.

    Metal skeletons, such as Nickel Foam (NF) has attracted worldwide interests as stable host for lithium metal anode because of its high stability, large specific surface area and high conductivity. However, most metal skeletons have lithophobic surface and uneven current distribution that result in sporadic lithium nucleation and uncontrolled dendrites growth. Herein, we describe a sequential immersing strategy to generate interwoven Nickel(Ⅱ)-dimethylglyoxime (Ni-DMG) nanowires at NF to obtain composite skeleton (NDNF), which can be used as an stable host for Li metal storage. The Ni-DMG has proved effective to realize uniform lithium nucleation and dendrite-free lithium deposition. Combing with the three dimensional (3D) hierarchical porous structure, the composite host shows a significantly improved coulombic efficiency (CE) than pristine commercial nickel foam. Moreover, the corresponding Li||Li symmetrical cells can run more than 700 h with low voltage hysteresis 22 mV at 1.0 mA/cm2, and Li@NDNF||LiFePO4 full-cell exhibits a high capacity retention of 82.03% at 1.0 C during 630 cycles. These results proved the effectiveness of metal-organic complexes in governing Li metal growth and can be employed as a new strategy for dendrite-free Li metal anode and safe Li metal batteries (LMBs).

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