Dual-functionalization of fluorescent carbon dots via cyclodextrin and aminosilane for visual detection of ß-glucuronidase and bioimaging.

A sensitive method for the detection of ß-glucuronidase was established using functionalized carbon dots (ß-CD-SiCDs) as fluorescent probes. The ß-CD-SiCDs were found to be obtained through in situ autopolymerization by mixing the solutions of methyldopa, mono-6-ethylenediamine-ß-cyclodextrin and N-(ß-aminoethyl)-γ-aminopropyltrimethoxysilane at room temperature. The method has the characteristics of low energy consumption, simple and rapid. ß-CD-SiCDs exhibited green fluorescence at 515 nm emission with a quantum yield of 7.9 %. 4-nitrophenyl-ß-D-glucuronide was introduced as a substrate for ß-glucuronidase to generate p-nitrophenol. Subsequently, p-nitrophenol self-assembled with ß-CD-SiCDs through host-guest recognition to form a stable inclusion complex, resulting in the fluorescence quenching of ß-CD-SiCDs. The linear range of ß-CD-SiCDs for detecting ß-glucuronidase activity was 0.5-60 U L-1 with a detection limit of 0.14 U L-1. For on-site detection, gel reagents were prepared by a simple method and the images were visualized and quantified by taking advantage of smartphones, avoiding the use of large instrumentation. The constructed fluorescence sensing platform has the benefits of easy operation and time saving, and has been successfully used for the detection of ß-glucuronidase activity in serum and cell imaging.

Mo Single-Atom Nanozyme Anchored to the 2D N-Doped Carbon Film: Catalytic Mechanism, Visual Monitoring of Choline, and Evaluation of Intracellular ROS Generation.

Single-atom nanozymes (SANs) have attracted great attention in constructing devices for instant biosensing due to their excellent stability and atom utilization. Here, Mo atoms were immobilized in 2D nitrogen-doped carbon films by cascade-anchored one-pot pyrolysis to obtain Mo single-atom nanozyme (Mo-SAN) with high atomic loading (4.79 wt %) and peroxidase-like activity. The coordination environment and enzyme-like activity mechanism of Mo-SAN were studied by combining synchrotron radiation and density functional theory. The strong oxophilicity of single-atom Mo makes the catalytic center more capable of transferring electrons to free radicals to selectively generate •OH in the presence of H2O2. Choline oxidase and Mo-SAN were used as signal opening unit and signal amplification unit, respectively. Combining the portability and visualization functions of smartphone and test strips, a paper-based visual sensing platform was constructed, which can accurately identify choline at a concentration of 0.5-35 µM with a limit of detection as low as 0.12 µM. The recovery of human serum samples was 96.4-102.2%, with an error of less than 5%. Furthermore, the potential of Mo-SAN to efficiently generate toxic •OH in tumor cells was intuitively confirmed. This work provides a technical and theoretical basis for designing highly active SANs and detecting neurological markers.

An upconversion nanosensor with phenolic-like functionality for accurate identification of chlorpyrifos in grapes.

The inappropriate use of the organophosphorus pesticide chlorpyrifos (CPF) in agricultural production could be harmful to the environment and non-target organisms. Here, we prepared a nano-fluorescent probe with phenolic function based on covalently coupled rhodamine derivatives (RDP) of upconverted nano-particles (UCNPs) for trace detection of chlorpyrifos. Due to the fluorescence resonance energy transfer (FRET) effect in the system, the fluorescence of UCNPs is quenched by RDP. The phenolic-functional RDP is converted to the spironolactone form when it captures chlorpyrifos. This structural shift prevents the FRET effect in the system and allows the fluorescence of UCNPs to be restored. In addition, the 980 nm excitement conditions of UCNPs will also avoid interference from non-target fluorescent backgrounds. This work has obvious advantages in terms of selectivity and sensitivity, which can be widely applied to the rapid analysis of chlorpyrifos residues in food samples.

Biocompatible Fluorescent Biosensor Reveals the Level and Distribution of Indole-3-Acetic Acid Signals in Plants.

To fully understand the function of the phytohormone indole-3-acetic acid (IAA) in regulating plant growth and development, we need to monitor their levels and distribution with high spatial and temporal resolution. In this work, an anthracene-based fluorescent biosensor for IAA was prepared using bovine serum albumin (BSA) as a bio-template. The single linear oxygen (1O2) specifically produced by IAA catalyzed with horseradish peroxidase (HRP) turns on the fluorescence of the probe, enabling specific trace sensing of IAA in the presence of multiple structural analogues. The presence of the bio-template BSA extends the biocompatibility of the probe, enabling visual monitoring of the level and distribution signal of endogenous IAA of plants in the field of bioimaging. In addition, the strategy has shown potential for application in portable paper-based sensors and in vivo fluorescent flower culture. This work provides a technical and theoretical basis for exploring the growth regulatory mechanisms of IAA in plants at the molecular level.

Realgar Alleviated Neuroinflammation Induced by High Protein and High Calorie Diet in Rats via the Microbiota-Gut-Brain Axis.

PURPOSE: Gastrointestinal heat retention syndrome (GHRS) often occurs in adolescents, resulting into nervous system injury. Realgar, an arsenic mineral with neuroprotective effect, has been widely used to treat GHRS. However, its mechanism of action remains unknown. METHODS: A GHRS rat model was established using a high protein and high calorie diet. We performed macroscopic characterization by assessing bowel sounds, hot/cold preference, anal temperature, and fecal features. Atomic fluorescence spectroscopy was employed to evaluate brain arsenic level while hippocampal ultrastructural changes were analyzed using transmission electron microscopy. In addition, inflammatory cytokines and BBB breakdown were analyzed by western blotting, immunofluorescence assays, and immunohistochemistry staining. We also evaluated hippocampal metabolites by LC-MS while fecal microorganisms were assessed by 16S rDNA sequencing. RESULTS: Our data showed that the high protein and high calorie diet induced GHRS. The rat model depicted decreased bowel sounds, increased fecal characteristics score, preference for low temperature zone, and increased anal temperature. In addition, there was increase in inflammatory factors IL-6, Iba-1, and NF-κB p65 as well as reduced BBB structural protein Claudin-5 and Occludin. The data also showed appearance of hippocampus metabolites disorder and fecal microbial imbalance. Realgar treatment conferred a neuroprotective effect by inhibiting GHRS-specific characteristics, neuroinflammatory response, BBB impairment, metabolites disorder, and microbial imbalance in the GHRS rat model. CONCLUSION: Taken together, our analysis demonstrated that realgar confers a neuroprotective effect in GHRS rats through modulation of the microbiota-gut-brain axis.

Smartphone-integrated dual-emission fluorescence sensing platform based on carbon dots and aluminum ions-triggered aggregation-induced emission of copper nanoclusters for on-site visual detecting sulfur ions.

A ratiometric fluorescence strategy was proposed based on carbon dots (CDs) and self-assembled copper nanoclusters (CuNCs) driven by Al3+ ions for S2- detection. Si-CDs/CuNCs@Al3+ exhibits blue and red emission under single excitation. Interestingly, the red emission of the CuNCs was regularly quenched while the blue fluorescence emission of the CDs was preserved after continuous addition of S2-. The fluorescence spectrometer-based S2- linear range is from 0.5 to 40 µM, with a low detection limit (LOD) of 0.16 µM. The fluorescence response of Si-CDs/CuNCs@Al3+ to S2- exhibits a distinct color change process (red to pink to blue), implying feasibility of visual analysis. A portable fluorescence sensing platform was established using the color-to-value conversion function of a smartphone for accurate visualization and quantitative identification of S2- without spectrometer. The fluorescent test strips prepared with Si-CDs/CuNCs@Al3+ can conduct on-site visual analysis of S2- in the water environment more conveniently and quickly. The linear range of S2- detection based on the smartphone-integrated test strip sensing platform is 1-40 µM, and the LOD is 0.42 µM. This work provides a new horizon for target on-site analysis in environmental samples.

Biocompatible Abscisic Acid-Sensing Supramolecular Hybridization Probe for Spatiotemporal Fluorescence Imaging in Plant Tissues.

Achieving detection of the phytohormone abscisic acid (ABA) is of critical importance for understanding plant growth and development. We report a hybrid supramolecular fluorescent probe that uses bovine serum albumin (BSA) as a host. Aggregation-induced emission of fluorescent chromophores (AIEgens) enables luminescence in the presence of BSA. ABA and its aptamer act as a switch to trigger this fluorescent system, the strategy that exhibits high sensitivity to abscisic acid with a detection limit of 0.098 nM. The probe test strip also enables visualization of ABA content from plants by colorimetric observation with the naked eye. In particular, the high biocompatibility and small molecular size of the prepared fluorescent probe allow for effective monitoring of ABA in plant tissues by fluorescence imaging. This strategy provides a new perspective to achieve the detection of endogenous and exogenous ABA in plants and has important implications for plant biology research.

A programmable and skin temperature-activated electromechanical synergistic dressing for effective wound healing.

Mechanical regulation and electric stimulation hold great promise in skin tissue engineering for manipulating wound healing. However, the complexity of equipment operation and stimulation implementation remains an ongoing challenge in clinical applications. Here, we propose a programmable and skin temperature-activated electromechanical synergistic wound dressing composed of a shape memory alloy-based mechanical metamaterial for wound contraction and an antibacterial electret thin film for electric field generation. This strategy is successfully demonstrated on rats to achieve effective wound healing in as short as 4 and 8 days for linear and circular wounds, respectively, with a statistically significant over 50% improvement in wound closure rate versus the blank control group. The optimally designed electromechanical synergistic stimulation could regulate the wound microenvironment to accelerate healing metabolism, promote wound closure, and inhibit infection. This work provided an effective wound healing strategy in the context of a programmable temperature-responsive, battery-free electromechanical synergistic biomedical device.

Polypyrrole-based nanotheranostic agent for MRI guided photothermal-chemodynamic synergistic cancer therapy.

Polypyrrole (PPy) nanoparticles have been widely studied in tumor photothermal therapy (PTT) for their significant photostability, good biocompatibility, and excellent photothermal performance. Herein, we report bovine serum albumin (BSA) stabilized PPy that were mineralized by MnO2 nanozyme on the surface (PPy@BSA-MnO2) to achieve synergistic photothermal and chemodynamic therapy (CDT) for breast cancer. In this multifunctional nanoplatform, the surface-loaded MnO2 undergoes a redox reaction with glutathione (GSH) to generate glutathione disulfide (GSSG) and Mn2+. Then, Mn2+ can convert H2O2 into a highly cytotoxic ˙OH to achieve chemodynamic therapy (CDT) and possess good magnetic resonance (MR) T1-weighted imaging capabilities to realize contrast imaging of the 4T1 tumor-bearing mouse models. In addition, PPy nanoparticles can efficiently convert near-infrared light energy into heat and achieve PTT. Most importantly, PPy@BSA-MnO2 nanoprobes have excellent in vitro 4T1 cell-killing effect and in vivo tumor-suppressive properties. The acute toxicity assessment results indicate that PPy@BSA-MnO2 nanoprobes have good biological safety. Therefore, the as-prepared multifunctional PPy@BSA-MnO2 nanoprobes possess excellent performance to promote MRI-guided PTT/CDT synergistic therapy for breast cancer treatment and have extensive clinical transformation and application prospects.

Nitrogen-doped carbon quantum dots fabricated from cellulolytic enzyme lignin and its application to the determination of cytochrome c and trypsin.

A sensitive and effective strategy for the detection of cytochrome c (Cyt c) and trypsin was developed using biomass nitrogen-doped carbon quantum dots (N-CQDs) as the fluorescence probe. N-CQDs were synthesized through a one-pot hydrothermal method by utilizing cellulolytic enzyme lignin as the carbon source and ammonia as the solvent and nitrogen source. The obtained N-CQDs had good water solubility and stable optical properties. The introduction of nitrogen increased fluorescence quantum yield (QY) to 8.23%, which was almost four times as high as that before nitrogen doping. The N-CQDs were fabricated as a label-free biosensor to detect Cyt c and trypsin. The fluorescence of N-CQDs was quenched with positively charged Cyt c due to electrostatic induction aggregation and static quenching. However, Cyt c tended to be hydrolyzed into small peptides in the presence of trypsin, which caused fluorescence recovery of the N-CQDs/Cyt c complex. A wide linear response range was achieved for Cyt c within 1-50 µM and the developed N-CQDs/Cyt c complex displayed a linear response for trypsin within 0.09-5.4 U/mL. The detection limits were 0.29 µM for Cyt c and 0.013 U/mL for trypsin, respectively. Furthermore, this assay had been applied to Cyt c and trypsin detection in serum samples with the recoveries in the range of 94.6-98.5% and 95.5-102.0%, respectively. The established method was sensitive, selective, easy to operate, and low cost, which proved its potential application in clinical diagnosis. The synthesis and fluorescence mechanism of N-CQDs and the strategy for Cyt c and trypsin detection.

Microcavity-integrated graphene waveguide: a reconfigurable electro-optical attenuator and switch.

Graphene has been widely utilized in optoelectronic applications due to its high carrier mobility, and extremely fast optical response. Microcavity-integrated graphene waveguide structure is one basic module of integrated photonic devices which can greatly improve the light-matter interaction strength. The enhanced optical absorption in the undoped graphene layer results from the light trapping and the corresponding long light-graphene interaction length. Tuning the Fermi energy level of the graphene layer enables the electro-optical modulation. We report the realization of reconfigurable electro-optical attenuator and switch with unity-order modulation depth in light reflection and transmission at near-infrared frequency. The transformation from a lossy absorber to a quasi-perfect transparent condition of the monolayer graphene by tuning the Fermi level leads to the unity-order tunability of the electro-optical attenuator and switch. We investigate theoretically and numerically the absorption properties of the designed microcavity-integrated graphene with respect to different graphene Fermi levels. Electro-optical attenuator with attenuating coefficient from 10% to 98.29% is fulfilled. On-off electro-optical switching with a switching contrast larger than 21 dB is demonstrated. Our approach provides the possibilities of graphene photonics applied in communications, and sensing.