Latest ArticlesCompared with natural enzymes, nanozymes have the advantages of high stability and low cost; however, selectivity and sensitivity are key issues that prevent their further development. In this study, we report a cascade nanozymatic system with significantly improved selectivity and sensitivity that combines more substrate-specific reactions and sensitive fluorescence detection. Taking detection of ascorbic acid (AA) as an example, a cascade catalytic reaction system consisting of oxidase-like N-doped carbon nanocages (NC) and peroxidase-like copper oxide (CuO) improved the reaction selectivity in transforming the substrate into the target product by more than 1200 times against the interference of uric acid. The cascade catalytic reaction system was also applicable for transfer from open reactors into a spatially confined microfluidic device, increasing the slope of the calibration curves by approximately 1000-fold with a linear detection range of 2.5 nmol/L to 100 nmol/L and a low limit of detection of 0.77 nmol/L. This work offers a new strategy that achieves significant improvements in selectivity and sensitivity.
For nano-collision, regulating the interaction between nanoparticles (NPs) and electrode interfaces is crucial for the precise analysis of individual NPs. However, existing ultramicroelectrodes (UMEs) suffer from narrow electrochemical window and poor electrode interface adhesion, severely hindering the application of precise single NP analysis. Here, we propose a simple and effective interface modification strategy. By electrochemically self-assembling poly(diallyldimethylammonium chloride) (PC) on the surface of carbon nanocone electrodes (CNCEs), we successfully prepared PC-modified CNCEs (PC‑CNCEs). These electrodes not only possess sufficiently wide electrochemical window but also exhibit strong adhesion to negatively charged Ag NPs on their surfaces. Surface physical analysis and electrochemical molecule detection validated the high-density loading of PC on the modified electrodes. Furthermore, the working principle of PC‑CNCEs for single Ag NP collision detection was further verified through the techniques of nano-collision and double-potential steps. Leveraging these significant advantages, PC‑CNCEs not only achieved precise measurements of single or mixed-sized Ag NPs but also detected Ag NP solutions at concentrations as low as fmol/L levels. This advancement offers a new strategy for the rapid and precise analysis of NP colloids.
Herein, a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid (TSA) inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks (Q[10]-SOFs) in water. Importantly, the 2D Q[10]-SOFs can further serve as light harvesting antenna, achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation, resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature. Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process, due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.
Researchers have shown significant interest in modulating the peroxidase-like activity of nanozymes. Among these, bimetallic nanozymes have shown superior peroxidase-like activity over monometallic counterparts, offering enhanced performance and cost-efficiency in nanozyme designs. Herein, bimetallic nanozymes comprising nickel (Ni) and osmium (Os) incorporated into hyaluronate (HA) have been developed, resulting in HA-Nin/Os nanoclusters. Subsequently, comprehensive characterizations have been conducted. Further investigation has revealed that HA-Nin/Os efficiently catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation with hydrogen peroxide (H2O2), confirming its peroxidase-like behavior and role as a nanozyme. Impressively, HA-Ni2/Os (Ni/Os = 2:1) displays heightened substrate affinity, accelerated reaction rates, enhanced hydroxyl radical production in acidic conditions, and exhibits activity unit of 1224 U/mg, representing more than two-fold increase compared to non-Ni-supported Os nanozyme. Theoretical calculations indicate that Ni support enhances the peroxidase-like process of Os nanozyme by improving H2O2 adsorption and TMB oxidation. Crucially, the support of Ni does not significantly alter the other enzyme-like activities of Os nanozymes, thereby enabling Ni to selectively enhance their peroxidase-like activity. In terms of application, the peroxidase-like ability of HA-Ni2/Os, facilitated by HA's carboxyl groups enabling crosslinking, proves effective in a squamous carcinoma antigen immunoassay. Moreover, HA-Ni2/Os exhibit reliable stability, promising as a peroxidase substitute. This work underscores the advantages of incorporating Ni into Os, specifically enhancing peroxidase-like activity, highlighting the potential of Os bimetallic nanozymes for peroxidase-based applications.
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.
Glioma is the most common malignant tumor of the brain. The postoperative recurrence rate was high, and the 2-year survival rate only increased by 20%–25%. The reason is the blood-brain barrier (BBB). BBB is a physical barrier that stabilizes the physiological environment of brain tissue and protects the central nervous system from the invasion of harmful substances. Drug delivery based on nanotechnology and nanocarriers has attracted much attention due to its biological safety, continuous drug release time, increasing solubility, biological drug activity, and enhanced BBB permeability. By modifying different substances on the surface of nanocarriers, the BBB is bypassed by receptor-mediated and cell endocytosis and exocytosis. In addition, the purpose of bypassing BBB-targeted drug delivery can also be achieved by intranasal administration and local administration. This paper reviews different target transport mechanisms, mainly in invasive and non-invasive strategies, the nanocarriers that have made progress and the nanocarrier strategy of bypassing BBB are listed.
Photoheranostics have emerged as a promising tool for cancer theranostics owing to their real-time feedback on treatment and their precise diagnosis. Among them, how to improve the photothermal conversion efficiency (PCE) of phototheranostic agents (PTAs) is the key factor for phototheranostic systems. Herein, we provided an efficient method to improve PCE and constructed a biocompatible nano-material ICR-Qu@NH2-Fe3O4@PEG (QNFP) by combing near-infrared second region (NIR-Ⅱ) molecular dye ICR-Qu and amino-modified magnetic nanoparticles and then encapsulated by DSPE-mPEG2000. QNFP exhibited excellent performance for photothermal therapy with a high PCE of 95.6%. Both in vitro and in vivo experiments indicated that QNFP could inhibit the growth of tumors under laser irradiation with low toxicity and realized real-time NIR-Ⅱ fluorescent imaging of tumors. In general, we realized a simple but efficient method to improve the PCE of NIR-Ⅱ molecular dye without reduce its quantum yield, which is an ideal choice for cancer diagnosis and treatment.
Degrading volatile organic compounds at low temperatures and active sites aggregation are still challenging. In this study, a novel mesoporous zeolite silicalite-1 (S-1-meso) enveloped Pt–Ni bimetallic catalysts (noted as Pt1Ni1@S-1-meso) were synthesized via a facile in situ mesoporous template-free method. The Pt–Ni bimetallic nanoparticles were uniformly distributed and displayed a large specific surface area and enriched mesopores to facilitate the deep oxidation of toluene. The presence of the Pt–NiO interface both increased the dispersion of the catalyst and improved its catalytic performance, thereby reducing the consumption of Pt. The Mars-van Krevelen mechanism and density function theory (DFT) calculations revealed that the Pt–NiO interface effect changed the electronic structure of Pt and Ni species, reduced the activation potential for oxygen, formed reactive oxygen species, and facilitated the adsorption and activation of reactants in the direction favorable to the toluene oxidation. This study provides a guideline for minimizing the proportion of precious metals used in practical applications and a promising method for toluene elimination at low temperatures.
The occurrence, development, and metastasis of tumors often entail abnormal expression of genetic substances. Monitoring and regulating changes in intracellular nucleic acid substances hold promise for achieving accurate tumor diagnosis and effective treatment. However, the effectiveness of integrated tumor diagnosis and treatment based on functional nucleic acids still needs to be improved. In this study, we engineered a multifunctional nucleic acid delivery system grounded in a cationic covalent organic framework carrier. This system not only showcases effective gene silencing but also boasts high sensitivity in detecting miR21 levels within tumor cells, enabling real-time monitoring of tumor gene therapy efficacy. The construction of this integrated functional nucleic acid delivery platform provides new ideas for precise tumor detection and effective tumor treatment.
The hydration state of amphiphilic block copolymers during the self-assembly transition is closely related to the structure and properties of copolymers. In this study, the temperature-induced self-assembly of copolymer poly(N,N-dimethylacrylamide)-poly(diacetone acrylamide) (PDMAA30-PDAAM60)2 in aqueous solution was monitored by near-infrared spectroscopy with water as a probe. The wavelet packet transform was employed to improve the spectral resolution. The spectral information of hydrated water surrounding the hydrophilic PDMAA and hydrophobic PDAAM blocks was then extracted, revealing the significant roles of water in morphological transition of the copolymer from spherical to worm-like micelles. Specifically, water molecules interacting with N atoms and C=O groups of the hydrophilic block gradually decrease during the morphological transition, while hydrogen-bond structures NH-CO of the hydrophobic block gradually break, bringing more water molecules into contact with the hydrophobic block. This work provides a foundation for exploring the role of water molecules during the self-assembly transition of complex block copolymers.
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