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  • Gaowa Xing, Weifei Zhang, Nan Li, Qiaosheng Pu, Jin-Ming Lin
    Chinese Chemical Letters. 2022, 33(4): 1743-1751.

    Rapid on-site detection of pathogenic bacteria with high sensitivity and specificity is becoming an urgent need in public health assurance, medical diagnostics, environmental monitoring, and food safety fields. Despite being reliable and widely used, the existing methods of bacteria detection are cumbersome and time-consuming, which is not conducive to field detection. Microfluidic lab-on-a-chip technology has provided a detective tool for various analytes, due to its miniaturization, portability and low reagent consumption. Within this progress report, advances in the bacteria detection using microfluidic biosensors were discussed. Typical methods for pathogenic bacteria capture, separation and detection were introduced respectively in the first part. Then key applications of microfluidic biosensor-based rapid bacteria detection were presented. Finally, we made a conclusion and discussed possible research prospects in aspects of microfluidic biosensors for rapid detection of pathogenic bacteria.

  • Lili Wang, Long Chen, Jiping Wang, Liying Wang, Chenyu Gao, Bo Li, Yuanzheng Wang, Jun Wu, Changyun Quan
    Chinese Chemical Letters. 2022, 33(4): 1956-1962.

    A poor biocompatibility and bioactivity of invasive materials remains major problems for biomaterial-based therapy. In this study, we introduced gelatin scaffolds carrying both bone morphogenetic protein-2 (BMP-2) biomimetic peptide and vascular endothelial growth factor-165 (VEGF) that achieved controlled release, cell attachment, proliferation and differentiation. To promote osteogenesis with VEGF, we designed the BMP-2 biomimetic peptide that comprised BMP-2 core sequence oligopeptide (SSVPT), phosphoserine, and synthetic cell adhesion factor (RGDS). In vitro cell experiments, the scaffold was conducive to the adhesion and proliferation of rat bone marrow mesenchymal stem cells (rBMSCs). The micro-CT 3D reconstruction of the rat cranial bone defect model showed that bone regeneration patterns occurred from one side edge towards the center area implanted with the prepared cryogel, and tissue section staining analysis demonstrated that the scaffold with double-growth factor can synergistically accelerate bone regeneration. These findings suggested that the obtained gelatin cryogel could serve as a cell-responsive platform for biomaterial-based nonbearing bone repair.

  • Wendong Zhang, Yun Wang, Yi Wang, Yi Liang, Fan Dong
    Chinese Chemical Letters. 2022, 33(3): 1259-1262.

    A novel SrSn(OH)6 photocatalyst with large plate and particle size were synthesized via a facile chemical precipitation method. The photocatalytic activity of the SrSn(OH)6 was evaluated by the removal of NO at ppb level under UV light irradiation. Based on the ESR measurements, SrSn(OH)6 photocatalyst was found to have the ability to generate the main active species of O2•−, OH and 1O2 during the photocatalytic process. Moreover, SrSn(OH)6 photocatalyst not only exhibits high photocatalytic activity for NO removal (79.6%), but also has good stability after five cycles. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) was used to investigate the NOx transfer pathway and the intermediate products distribution during the adsorption and photocatalytic NO oxidation process. The present work not only provides an efficient material for air pollutants purification at room temperature but also in-depth understanding of the mechanism involved in the photocatalytic NO removal process.

  • Jingtian Lu, Ting Wang, Huimin Bao, Haojie Lu
    Chinese Chemical Letters. 2022, 33(3): 1343-1345.

    Herein, we developed a fractionation-free negative enriching method incorporating methylamidation, site-selective dimethylation and aldehyde resin coupling (MADMAR) for in-depth C-terminome analysis. The methylamidation blocked the free carboxyl group on proteins first, followed by LysC digestion of methylamidated proteins. Then, the site-selective dimethylation blocked the N-terminal amino group of the digested peptides without affecting the amino groups of lysine. Finally, the aldehyde resin was used to capture non-C-terminal peptides containing amino groups from lysine, while leaving the C-terminal peptides without free amino group in the supernatant for its analysis. We identified 1359 database-annotated protein C-termini from 50 µg HeLa proteins, which was 74% more than our previous method based on aldehyde resin. Moreover, 279 protein neo-C-termini were identified.

  • Hedong Qi, Yuwei Xu, Pin Hu, Chi Yao, Dayong Yang
    Chinese Chemical Letters. 2022, 33(3): 1131-1140.

    As a biologically active macromolecule, deoxyribonucleic acid (DNA) has the advantages of sequence programmability and structure controllability and can accurately transmit sequence information to specific biological functions. Facing the complex internal microenvironment and heterogeneity in tumor treatment, the construction and applications of DNA-based nanomaterials have become a focus point of research. In particular, the hybridization of DNA molecules with other materials endows DNA-based nanomaterials with multiple functions such as targeting, stimulus responsiveness and regulations of biological activities, making DNA nanostructures great potential in the treatment of major human diseases. In this review, the construction and characteristics of DNA-based nanomaterials are introduced. Then, the functions and applications of DNA-based nanomaterials in the delivery of chemotherapy drugs and gene drugs, stimulus-responsive release and regulation of cell homeostasis are reviewed. Finally, the future development and challenges of DNA-based nanomaterials are prospected. We envision that DNA-based nanomaterials can enrich the nanomaterial system by rational design and synthesis and address the growing demands on biological and biomedical applications in the real world.

  • Fang Jing, Yanmeng Guo, Bo Li, Yi-Fan Chen, Chunman Jia, Jianwei Li
    Chinese Chemical Letters. 2022, 33(3): 1303-1307.

    Titanium dioxide (TiO2) has been limited in photocatalysis due to its wide band gap (3.2 eV) and limited absorption in the ultraviolet range. Therefore, organic components have been introduced to hybrid with TiO2 for enhanced photocatalytic efficiency under visible light. Here, we report that benzo[1, 2-b: 4, 5-b']dithiophene polymer was an ideal organic material for the preparation of a hybrid material with TiO2. The energy band gap of the resulting hybrid material decreased to 2.9 eV and the photocatalytic hydrogen production performance reached 745.0 µmol g−1 h−1 under visible light irradiation. Meanwhile, the material still maintained the stability of hydrogen production performance after 40 h of photocatalytic cycles. The analysis of the transient current response and electrochemical impedance revealed that the main reasons for the enhanced water splitting of the hybrid materials were the faster separation of electron hole pairs and the lower recombination of photocarrier ions. Our findings suggest that polythiophene is a promising organic material for exploring hybrid materials with enhanced photocatalytic hydrogen production.

  • Wei Xiang, Mingjie Huang, Xiaohui Wu, Fugang Zhang, Dan Li, Tao Zhou
    Chinese Chemical Letters. 2022, 33(3): 1275-1278.

    This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H2O2 Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H2O2/HA/MF system, e.g., pH and the dosages of ZVI, HA and H2O2, were investigated. Unlike the acid-favorable ZVI/H2O2 and ZVI/H2O2/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H2O2/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(Ⅱ) and local corrosion of iron. Large amounts of aqueous and bounded Fe(Ⅱ) catalyzed H2O2 to efficiently produce OH, while HA maintained the surface and bulk cycles of Fe(Ⅱ)/Fe(Ⅲ). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.

  • Yongbing Xie, Ya Liu, Yujie Yao, Yanchun Shi, Binran Zhao, Yuxian Wang
    Chinese Chemical Letters. 2022, 33(3): 1298-1302.

    Metal-free heteroatom doped nanocarbons are promising alternatives to the metal-based materials in catalytic ozonation for destruction of aqueous organic contaminants. In this study, N, S co-doped hollow carbon microspheres (NSCs) were synthesized from the polymerization products during persulfate wet air oxidation of benzothiazole. The contents of doped N and S as well as the structural stability were maneuvered by adjusting the subsequent N2-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N2-annealed NSCs demonstrated a higher catalytic ozonation activity for benzimidazole degradation. According to the quantitative structure-activity relationship (QSAR) analysis, the synergistic effect between the graphitic N and the thiophene-S which redistributed the charge distribution of the carbon basal plane contributed to the activity enhancement of the N2-annealed NSCs. Additionally, the hollow structure within the microspheres served as the microreactor to boost the mass transfer and reaction kinetics via the nanoconfinement effects. Quenching and electron paramagnetic resonance (EPR) tests revealed that benzimidazole degradation was dominated by the produced singlet oxygen (1O2) species, while hydroxyl radicals (·OH) were also generated and participated. This study puts forward a novel strategy for synthesis of heteroatom-doped nanocarbons and sheds a light on the relationship between the active sites on the doped nanocarbons and the catalytic performance.

  • Xiuying Li, Shuangqiu Huang, Huaihao Xu, Yuepeng Deng, Zhu Wang, Zhao-Qing Liu
    Chinese Chemical Letters. 2022, 33(3): 1321-1324.

    The leaching and non-recoverability of mental ions have always limited the practical application of Fenton-like processes. For the first time, we synthesized molybdenum phosphide (MoP) with dual active sites for the degradation of diclofenac (DCF) in the Fenton-like process. The DCF degradation rate constant (k) of MoP + H2O2 process was calculated to be 0.13 min-1 within 40 min, indicating a highly efficient catalytic ability of MoP. In addition, this catalyst exhibits a stable structure and good activity, which could apply in a broad pH range, different ions solution and real wastewater condition. Accordingly, this efficient catalytic capability may be attributed to the presence of the metal sites Moδ+ and the electron-rich sites Pδ in MoP, which could induce the generation of hydroxyl radical (·OH) and superoxide radical (·O2) through electron transfer, resulting in the effective removal of DCF. This study provides an idea for the optimization of Fenton-like technologies and environmental remediation.

  • Yu Liu, Xiaowei Zhang, Lisha Lu, Jun Ye, Jianlin Wang, Xiaomin Li, Xuedong Bai, Wenlong Wang
    Chinese Chemical Letters. 2022, 33(3): 1271-1274.

    The ability of plasmonic nanostructures to efficiently harvest light energy and generate energetic hot carriers makes them promising materials for utilization in photocatalytic water spitting. Apart from the traditional Au and Ag based plasmonic photocatalysts, more recently the noble–metal–free alternative plasmonic materials have attracted ever–increasing interest. Here we report the first use of plasmonic zirconium nitride (ZrN) nanoparticles as a promising photocatalyst for water splitting. Highly crystalline ZrN nanoparticles with sizes dominating at 30–50 nm were synthesized that exhibit intense visible and near–infrared absorption due to localized surface plasmon resonance (LSPR). Without utilizing any noble metal cocatalysts such as Pt, the plasmonic ZrN nanoparticles alone showed stable photocatalytic activity for H2 evolution in aqueous solution with methanol as sacrificial electron donor. The addition of a cobalt oxide (CoOx) cocatalyst can facilitate the separation of photogenerated charge carriers and further improve the photocatalytic activity. The optimized CoOx modified ZrN photocatalyst was observed not only to activate the O2 evolution reaction with presence of electron acceptor, but also to drive overall water splitting for the simultaneous H2 and O2 evolution in the absence of any sacrificial agents.

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