Latest ArticlesAn enantioselective catalytic method for the direct [4 + 1] annulation of yne–allylic acetates with pyrazolones has been realized by a copper-catalyzed remote strategy. A variety of enantioenriched spiropyrazolones are rapidly accessed in high yields with moderate to good enantiocontrol. The facile follow-up transformations highlight its potential utility in the synthesis of diverse spiropyrazolones building blocks.
MicroRNA-133a (miRNA-133a) and cardiac troponin I (cTnI) are different-type crucial biomarkers of acute myocardial infarction (AMI), whose levels are great significance for AMI diagnosis and treatment. Herein, a novel photoelectrochemical-electrochemical (PEC-EC) dual-mode biosensing platform for dual-target assays of miRNA-133a and cTnI was developed. In which, a PEC-EC dual-mode sensing platform for miRNA-133a was constructed based on the changes of the photocurrent inhibition effect and the electrochemical signal of Fc on the Fc-hairpin DNA probe (Fc-HP)/ZnCdS-quantum dots (QDs)/ITO electrode. Furthermore, under magnetic separation and the specific interaction between cTnI and its aptamer, the N-doped porous carbon-ZnO polyhedra (NPC-ZnO)-hemin-capture DNA probe hybrid (NH-CP) was obtained and introduced to the Fc-HP/ZnCdS-QDs/ITO electrode via hybridization between NH-CP and Fc-HP. The hemin molecules encapsulated in NH-CP could effectively induce the photocurrent-polarity-switching of the Fc-HP/ZnCdS-QDs/ITO electrode and generate a new electrochemical signal originating from hemin. Thus, cTnI was assayed sensitively and selectively by the PEC-EC dual-mode biosensing platform. Here, Fc and hemin not only serve as the electrochemical indicators, but also respectively inhibit the photocurrent and switch the photocurrent polarity of ZnCdS-QDs. Furthermore, the proposed biosensing platform could be easily expanded to the detection of other multiplex-type biomarkers via the change of the sequences of the related DNA probes, implying its significant potential in clinical diagnosis and biological analysis.
Utilizing small molecules as markers for specific cells or organs within biosystems is a crucial approach for studying and regulating physiological processes. However, current tagging strategies, due to the presence of exposed highly reactive groups, suffer from drawbacks such as low tagging efficiency or insufficient spatial specificity, thereby diminishing their expected effectiveness. Consequently, there is a pressing need to develop a strategy capable of in situ labeling of active groups in response to cellular or in vivo stimuli, ensuring both high tagging efficiency and spatial specificity. In this work, we devised a strategy for releasing aldehyde groups activated by hypochlorous acid (HOCl). Compounds synthesized through this strategy can release the fluorophore methylene blue (MB) and aldehyde-based compounds upon HOCl activation. Given high reactivity of the released aldehyde group, it can effectively interact with macromolecules in biological systems, facilitating tagging and enabling prolonged imaging. To validate this concept, we further incorporated a naphthalimide structure with stable light emission to create SW-110. SW-110 can specifically respond to in vitro and endogenous HOCl, when release MB, it also releases naphthalimide fluorophore with highly reactive aldehyde group for tagging within cells. This strategy provides a simple but efficient strategy for proximity tagging in situ.
A thickness-controllable method for preparing metal-organic framework hollow nanoflowers on magnetic cores (Fe3O4@MOFs HFs) was demonstrated for the first time. The petal of magnetic core with hollow nanoflower structure served as medium for assembling UiO-66-NH2 shell with different thickness. To further improve its performance, Zr4+ was immobilized on the surface of Fe3O4@UiO-66-NH2. Compared with conventional Fe3O4@UiO-66-NH2-Zr4+ nanospheres, the Fe3O4@UiO-66-NH2-Zr4+ HFs showed increased enrichment performance for phosphopeptides. The Fe3O4@UiO-66-NH2-Zr4+ HFs served as an attractive restricted-access adsorption material exhibited good selectivity (mβ-casein:mBSA=1:1000), high sensitivity (1.0 fmol) and excellent size-exclusion effect (mβ-casein digests:mBSA=1:200). Furthermore, the Fe3O4@UiO-66-NH2-Zr4+ HFs was successfully applied to the specific capture of ultratrace phosphopeptide from complex biological samples, revealing the great potential for the identification and analysis of trace phosphopeptides in clinical analysis. This work can be easily extended to the fabrication of diverse mag-MOF HFs with multifunctional and easy to post-modify properties, and open up a new avenue for the design and construction of new MOFs material.
Polyetheretherketone (PEEK) is a desirable candidate to replace conventional metal implants owing to its excellent mechanical properties. However, the intrinsic bioinertness of PEEK results in inferior or delayed osseointegration, which limits its further clinical application. To address these challenges, one leading strategy is to construct a biofunctionalized surface on PEEK that provides a coordinated osteoblast-osteoclast interactions microenvironment. Herein, alendronate (ALN), a common bone absorption inhibitor, was loaded in biomedical inorganic/organic microspheres, consisting of bioactive inorganic nano-hydroxyapatite core, and chitosan (CS) shell. Polydopamine (PDA) modification was employed to ensure the adherence of the microspheres to the PEEK surface. The delivery of ALN and Ca2+ from these microspheres simultaneously suppressed osteoclastogenesis and promoted osteogenesis, resulting in a coordinated cascade of osteoblast-osteoclast interactions crucial for the per-implant osseointegration. In vitro experiments demonstrated that the PEEK surface exhibited satisfactory biocompatibility and enhanced the proliferation and osteogenic differentiation of rat bone mesenchymal stem cells while inhibiting the osteoclast differentiation. Moreover, the in vivo rat femoral drilling model demonstrated superior osseointegration three months after implantation. By considering the bone remodeling processes, this study proposes a novel biofunctionalized PEEK surface that regulates the activities of both osteoblasts and osteoclasts to promote osseointegration.
Rapid diagnosis of Salmonella is crucial for the effective control of food safety incidents, especially in regions with poor hygiene conditions. Polymerase chain reaction (PCR), as a promising tool for Salmonella detection, is facing a lack of simple and fast sensing methods that are compatible with field applications in resource-limited areas. In this work, we developed a sensing approach to identify PCR-amplified Salmonella genomic DNA with the naked eye in a snapshot. Based on the ratiometric fluorescence signals from SYBR Green Ⅰ and Hydroxyl naphthol blue, positive samples stood out from negative ones with a distinct color pattern under UV exposure. The proposed sensing scheme enabled highly specific identification of Salmonella with a detection limit at the single-copy level. Also, as a supplement to the intuitive naked-eye visualization results, numerical analysis of the colored images was available with a smartphone app to extract RGB values from colored images. This work provides a simple, rapid, and user-friendly solution for PCR identification, which promises great potential in molecular diagnosis of Salmonella and other pathogens in field.
Plant bacterial diseases have inflicted substantial economic losses in global crop, fruit, and vegetable production. The conventional methods for managing these diseases typically rely on the application of antibiotics. However, these antibiotics often target the growth factors of the pathogenic bacteria, leading to the accumulation and emergence of drug-resistant strains, which exacerbates antibiotic resistance. Innovative methods are urgently needed to treat and prevent the toxicity caused by these pathogenic bacteria. Targeting virulence mechanisms in pathogens is a globally recognized and effective strategy for mitigating bacterial resistance. Type III secretion system (T3SS) serves as a crucial virulence determinant in Gram-negative pathogens, and its non-essentials for pathogen growth renders it an ideal target. Targeting the T3SS holds significant potential to alleviate selective pressure for resistance mutations in pathogens. Therefore, targeting T3SS in pathogenic bacteria, while preserving their growth, has emerged as a novel avenue for the development of antimicrobial drugs. In recent years, a multitude of small molecular inhibitors targeting T3SS have been identified. This article offers a comprehensive review of T3SS inhibitors in plant pathogens, while also presenting the latest research advancements in this research direction.
The micro-dispersion structure of silica fillers exerts significant influences on the performance characteristics of rubber-based products. How to monitor this parameter is an important issue in the rubber industry, but there is currently no suitable technical solution for numerical monitoring that can be applied in automatic production line. The labeling of silica in rubber is a challenge that bottlenecks the development of numerical quality monitoring technology. In this work, we employed the organometallic europium to modify silica endowing the fluorescence properties for characterization. It provides more feasible solutions for visually studying the relationship between the submicroscopic structure and macroscopic properties of inorganic-filled polymers, and is the key foundation for achieving numerical monitoring of rubber filler qualities in industry.
A novel Fe-doping three-dimensional flower-like Bi7O9I3 microspheres with plasmonic Bi and rich surface oxygen vacancies (Fe-Bi/Bi7O9I3/OVs) was prepared as catalysts, and further coupled with natural air diffusion electrode (NADE) to construct the heterogeneous visible-light-driven photoelectro-Fenton (HE-VL-PEF) process to enhance the degradation and mineralization of tetracycline (TC). Interfacial ≡Fe sites, OVs and Bi metal were simultaneously constructed via Fe doping, which effectively improved visible light absorption and the separation efficiency of photogenerated carriers to further accelerate the transformation of Fe(Ⅲ) to Fe(Ⅱ), achieving Fenton reaction recycling. HE-VL-PEF process could achieve enhanced treatment of pollutants, thanks to the synergistic effect of electro-Fenton (EF) and photo-Fenton (PF). NADE exhibited excellent H2O2 electrosynthesis without external oxygen-pumping equipment. Under the irradiation of visible light, Fe-Bi/Bi7O9I3/OVs could achieve more photoelectrons to accelerate the transformation of Fe(Ⅲ) to Fe(Ⅱ) or directly activate H2O2. DFT calculations also clearly demonstrated that except for the fast charge separation and transfer, Fe-Bi/Bi7O9I3/OVs could achieve a faster electron transport between Fe-O, facilitating Fe site acquire more electron. Consequently, the Fe-Bi/Bi7O9I3/OVs in HE-VL-PEF process presented performance superiorities including excellent pollutant removal (91.91%), low electric energy consumption of 66.34 kWh/kg total organic carbon (TOC), excellent reusability and wide pH adaptability (3–9).
With the rapid development of electric vehicles, hybrid electric vehicles and smart grids, people's demand for large-scale energy storage devices is increasingly intense. As a new type of secondary battery, potassium ion battery is promising to replace the lithium-ion battery in the field of large-scale energy storage by virtue of its low price and environmental friendliness. At present, the research on the anode materials of potassium ion batteries mainly focuses on carbon materials and the design of various nanostructured metal-based materials. Problems such as poor rate performance and inferior cycle life caused by electrode structure comminution during charge and discharge have not been solved. Quantum dots/nanodots materials are a new type of nanomaterials that can effectively improve the utilization of electrode materials and reduce production costs. In addition, quantum dots/nanodots materials can enhance the electrode reaction kinetics, reduce the stress generated in cycling, and effectively alleviate the agglomeration and crushing of electrode materials. In this review, we will systematically introduce the synthesis methods, K+ storage properties and K+ storage mechanisms of carbon quantum dots and carbon-based transition metal compound quantum dots composites. This review will have significant references for potassium ion battery researchers.
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