Programming of a Portable Digital Monitoring System-Integrated DNA Aptamer Reversely Regulated Oxidase-Like Nanozyme for Real-Time Dynamic Analysis of Atmospheric Perfluorooctanoic Acid.

Timely and efficient analysis of the fluorinated per- and polyfluoroalkyl substances (PFAS) in an atmospheric environment is critical to environmental pollution traceability, early warnings, and governance. Here, a portable, reliable, and intelligent digital monitoring device for onsite real-time dynamic analysis of atmospheric perfluorooctanoic acid (PFOA) is proposed. The sensing mechanism is attributed to the oxidase-like activity of PtCoNPs@g-C3N4 that is reversely regulated by the surface modification of a PFOA-recognizable DNA aptamer, engineering a PFOA-activated oxidase-like activity of nanozyme (Apt-PtCoNPs@g-C3N4) to combine the nonfluorescence o-phenylenediamine (OPD) as the dual-modality response system. The present PFOA interacts with its DNA aptamer and dissociates from the surface of Apt-PtCoNPs@g-C3N4, restoring the oxidase-like activity of PtCoNPs@g-C3N4 to oxidize OPD into yellow fluorescence 2,3-diphenylaniline (DAP), thereby observing a PFOA-triggered colorimetric as well as fluorescence dual-modality change. Then, a hydrogel kit-programmed Apt-PtCoNPs@g-C3N4 + OPD system is used as the sensitive element to incorporate into this homemade portable device, automatically gathering and processing the PFOA-triggered hydrogel colorimetric and fluorescence image gray values by our self-weaving software, ultimately realizing the onsite real-time dynamic analysis of atmospheric PFOA surrounding a fluorochemical production plant. This work provides a direction and theoretical foundation for designing portable onsite screening devices that cater to other atmospheric contaminants detection requirements.

Effect of sodium metabisulfite-mediated self-assembly on the quality of silver carp myofibrillar protein-EGCG composite gels.

Myofibrillar protein (MP) gels are susceptible to oxidation, which can be prevented by complexing with hydrophilic polyphenols, but may cause gel deterioration. Sodium metabisulfite (Na2S2O5) has been used to induce self-assembly of MP and analyze the impact of self-assembly on the quality of composite gels containing high amounts of (-)-epigallocatechin gallate (EGCG). Hydrophobic forces were confirmed as the main driver of self-assembly. Self-assembly reduced the size of the MP-EGCG complex to approximately 670 nm and increased the gel's hydrophobic force by approximately 3.6-fold. The maximum hardness of the Na2S2O5-treated MP-EGCG composite gel was 52.43 g/kg, which was approximately 49% greater than pure MP gel. After oxidative treatment, the Na2S2O5-treated MP-EGCG composite gel had considerably lower carbonyl and dityrosine levels (2.47-µmol/g protein and 450 a.u.) than the control (8.37-µmol/g protein and 964 a.u.). Therefore, Na2S2O5 shows potential as a cost-effective additive for alleviating MP limitations in the food industry.

Intelligent onsite dual-modal assay based on oxidase-like fluorescence carbon dots-driven competitive effect for ethyl carbamate detection.

Intelligent onsite accurate monitoring ethyl carbamate (EC, a group 2 A carcinogen) in environment is of great significance to safeguard environmental health and public safety. Herein, we reported an intelligent dual-modal point-of-care (POC) assay based on the bimetallic Mn and Ce co-doped oxidase-like fluorescence carbon dots (Ce&MnCDs) nanozyme-driven competitive effect. In brief, the oxidase-like activity of Ce&MnCDs was inhibited by thiocholine (TCh, originating from the hydrolysis of acetylcholinesterase (AChE) to acetylthiocholine (ATCh)), preventing the oxidation of o-phenylenediamine (OPD) to 2,3-diaminophenothiazine (DAP). However, with the aid of Br2 + NaOH, EC inactivated AChE to prevent TCh generation for re-launching the oxidase-like activity of Ce&MnCDs to trigger the oxidation of OPD into DAP, thereby outputting an EC concentration-dependent ratiometric fluorescence and colorimetric readouts by employing Ce&MnCDs and OPD as the optical signal reporters. Interestingly, these dual-modal optical signals could be transduced into the gray values that was linearly proportional to the residual levels of EC on a smartphone-based portable platform, with a detection limit down to 1.66 µg/mL, qualifying the requirements of analysis of EC residues in real samples. This opened up a new avenue for onsite assessment of the risk of residues of EC, safeguarding environmental health and public safety.

AIE fluorescent nanozyme-based dual-mode biosensor for analysis of the bioactive component hypoxanthine in meat products.

The development of facile, low-cost reliable, and precise onsite assays for the bioactive component hypoxanthine (Hx) in meat products is significant for safeguarding food safety and public health. Herein, we proposed a smartphone-assissted aggregation-induced emission (AIE) fluorogen tetraphenylethene (TPE)-incorporated amorphous Fe-doped phosphotungstates (Fe-Phos@TPE) nanozyme-based ratiometric fluorescence-colorimetric dual-mode biosensor for achieving the onsite visual detection of Hx. When the Hx existed, xanthine oxidase (XOD) catalyzed Hx into H2O2 to be further catalyzed into •OH by the prominent peroxidase activity of Fe-Phos@TPE at pH = 6.5, resulting in the oxidization of nonfluorescent o-phenylenediamine (OPD, naked-eye colorless) to be yellow fluorescent emissive 2,3-diaminophenazine (DAP, naked-eye dark yellow) at 550 nm as well as the intrinsic blue fluorescence of Fe-Phos@TPE at 440 nm to be decreased via inner-filter effect (IFE) action, thereby realizing a multi-enzyme cascade catalytic reaction at near-neutral pH to overcome the traditional acidity dependence-induced time-consuming and low sensitivity troublesome.

Portable hydrogel kit driven by bimetallic carbon dots nanozyme for H2O2-self-supplying dual-modal monitoring of atmospheric CH3SH.

Due to the typical volatility of gaseous pollutant methyl mercaptan (CH3SH), the development of a facile, reliable, and accurate onsite environmental surveillance of highly toxic CH3SH faces many challenges, but it is critical to environmental atmosphere assessment and safeguarding public health. Here, we prepared a novel bimetallic carbon dots (Fe&Cu@CDs) nanozyme with high peroxidase-mimicking activity to design a portable hydrogel kit for onsite visual H2O2-self-supplying enzymatic cascade catalytic colorimetric and photothermal signal synergistic amplification dual-modal monitoring of CH3SH in atmospheric environment. Assisted by alcohol oxidase (AOX), CH3SH could be specifically converted into H2O2 for oxidizing chromogenic substrate 3,3',5,5'-tetramethylbenzidine (TMB) catalyzed by Fe&Cu@CDs to produce dark blue ox-TMB with absorption at 652 nm and photothermal characters. Consequently, a CH3SH concentration-dependent change both in naked-eye color and photothermal effect-triggered temperature were observed. By hybridizing AOX-assisted Fe&Cu@CDs + TMB with agarose, a H2O2-self-supplying colorimetric and photothermal signal synergistic amplification sensory hydrogel kit integrated with Color Picker APP-installed smartphone and 660 nm laser-equipped handheld thermal imager for CH3SH was proposed with acceptable results in atmospheric environment around wastepile (e.g., solid waste and food waste piles), which exhibited great potentials to further develop commercial onsite monitoring platforms in warning-early abnormal atmospheric CH3SH for safeguarding environmental health.

Synergetic surface enhancement of quantum dots-based electrochemiluminescence with photonic crystal light scattering and metal surface plasmon resonance for sensitive bioanalysis.

Noble metal nanostructures and photonic crystals (PhCs) have been widely investigated as substrates for constructing surface enhanced electrochemiluminescence (SE-ECL) biosensors. However, their applications are hindered by the limited enhancement intensity of surface plasmon resonance (SPR) and an incomplete mechanism for the photonic enhancement effect. Hence, developing a novel SE-ECL strategy with better signal enhanced capability and enriching our understanding of the intrinsic mechanisms for efficient bioanalysis is extremely urgent. Here, a synergistic SE-ECL strategy was developed for the sensitive determination of prostate specific antigen (PSA) protein. The randomly arranged polystyrene (r-PS) spheres and PS PhC arrays were applied to enhance the ECL emission of cadmium sulfide quantum dots (CdS QDs) and the results suggested that the PhC arrays displayed superior intensity (0.22) than the r-PS interface (0.10). Au nanoparticles (NPs) were introduced onto the two kinds of surfaces and further boosted the ECL intensity. According to the ECL measurements, Au NPs modified at the r-PS surface exhibited only a slight increase (0.13), while the PhC arrays showed approximately 5-fold enhancement (0.92), benefiting from the synergistic enhancement. The finite-difference time-domain (FDTD) simulation indicated that the ECL enhancement was ascribed to the coupled electromagnetic (EM) field at the surfaces of PS PhCs and Au NPs. The SE-ECL could achieve a detection range from 1 pg/mL to 1 µg/mL with a detection limit of 0.41 pg/mL (S/N = 3). This study provides the first combination of PhC arrays and metal surface plasmon nanostructure for the synergetic enhancement of SE-ECL systems. It opens a new avenue for the rational design of advanced ECL biosensors and shows great perspective for clinical diagnosis.

Prevalence and correlates of suicide risk among non-psychiatric inpatients in a general hospital in China.

OBJECTIVE: This study aims to investigate the suicide risk and mental health status of non-psychiatric inpatients in general hospital and explore the risk factors of suicide. METHODS: A prospective study was conducted at a tertiary general hospital in Guangzhou, Guangdong Province, China. On-line assessment of mental health status and suicide was completed at admission and discharge. We assessed depression, anxiety, insomnia and suicide of inpatients and binary logistics regression was used to examine the risk factors of suicide. RESULTS: From April 1, 2021 and January 31, 2022, 3685 inpatients were included. The detection rates of depression, anxiety and insomnia were 14.6 %, 9.0 % and 17.8 %, respectively. There were 2.7 % of inpatients at suicide risk. Binary logistics regression demonstrated that the inpatients with anxiety were at higher risk of suicide. LIMITATIONS: (1) Single-center study limits the generalization of conclusion, (2) low response rate at discharge. CONCLUSIONS: The comorbidity of physical illnesses and mental health problems, including depression, anxiety, insomnia, and suicide among non-psychiatric patients in general hospital was common. An assessment of anxiety may help identify individuals at high suicide risk. Medical staff in general hospitals should be trained to improve their ability to identify mental disorders and high-risk individuals for suicide, provide timely interventions and effectively reduce the suicide risk of patients.

AIE fluorogen-based oxidase-like fluorescence nanozyme-integrated smartphone for monitoring the freshness authenticity of soy products.

Food safety concerns about the authenticity of soy product freshness have increased due to high demand from public. Developing an accurate and convenient monitoring method for freshness authenticity is crucial for safeguarding food safety. From this motive, this study employed PtPd NPs to encapsulate tetraphenylethylene (TPE) for engineering an AIE-based fluorescent nanozyme (PtPd NPs@TPE) with oxidase-like activity, achieving the ratiometric fluorescence monitoring of putrescine (PUT) to judge the freshness authenticity of soy products. In this design, PUT acted as an antioxidant and inhibited the oxidation process of PtPd NPs@TPE to o-phenylenediamine (OPD), leading to the reduction of oxidative product 2,3-diaminophenothiazine (DAP) alone with the weaken of yellow fluorescence from DAP at 552 nm and bright of bule fluorescence from PtPd NPs@TPE at 442 nm. On this basis, a ratiometric fluorescence strategy integrated with smartphone-based sensor was developed for PUT with acceptable results to combat food freshness fraud of soy products.

Dual-Modal Bimetallic Nanozyme-Based Sensing Platform Combining Colorimetric and Photothermal Signal Cascade Catalytic Enhancement for Detection of Hypoxanthine to Judge Meat Freshness.

Considering the enormous demand for meat in people's daily lives, the development of efficient meat freshness assays is of great significance for safeguarding food safety. Here, a novel bimetallic nanozyme Fe@CeO2 with high peroxidase-like activity was first synthesized by embedding ferrocenecarboxylic acid (Fc) into hollow CeO2 nanospheres, which combined with xanthine oxidase (XOD) to develop a self-supplying H2O2-facilitated enzymatic cascade catalytic system of XOD + Fe@CeO2, yielding a meat freshness indicator hypoxanthine (Hx)-responsive colorimetric and photothermal dual-mode analytical platform for judging meat freshness upon the assistance of 3,3',5,5'-tetramethylbenzidine (TMB). Owing to the catalytic activity of XOD to convert Hx into H2O2, Fe@CeO2 rapidly dissociated it into •OH via a peroxidase activity-triggered Fenton-like reaction, emerging a typical enzymatic cascade catalytic reaction. As a result, the colorless TMB was oxidized to be the product of dark-blue oxTMB by •OH, with a chromogenic reaction-driven absorption enhancement at 652 nm, which endowed it with a significant photothermal effect under 660 nm laser irradiation. On this basis, an Hx concentration-dependent colorimetric and photothermal dual-mode signal cascade catalytic enhancement sensing platform was proposed by integrating with a Color Picker App-installed smartphone and a 660 nm laser-equipped handheld thermal imager, achieving the onsite quantitative, reliable, and visual detection of Hx in real meat samples for judging meat freshness with acceptable results. Notably, the colorimetric and photothermal dual-mode signal cascade catalytic enhancement improved not only the reliability but also the sensitivity of the assay, which provided new insights for efficient onsite visual monitoring of meat freshness to safeguard food safety.

Transition Metal High-Entropy Nanozyme: Multi-Site Orbital Coupling Modulated High-Efficiency Peroxidase Mimics.

Strong substrate affinity and high catalytic efficiency are persistently pursued to generate high-performance nanozymes. Herein, with unique surface atomic configurations and distinct d-orbital coupling features of different metal components, a class of highly efficient MnFeCoNiCu transition metal high-entropy nanozymes (HEzymes) is prepared for the first time. Density functional theory calculations demonstrate that improved d-orbital coupling between different metals increases the electron density near the Fermi energy level (EF ) and shifts the position of the overall d-band center with respect to EF , thereby boosting the efficiency of site-to-site electron transfer while also enhancing the adsorption of oxygen intermediates during catalysis. As such, the proposed HEzymes exhibit superior substrate affinities and catalytic efficiencies comparable to that of natural horseradish peroxidase (HRP). Finally, HEzymes with superb peroxidase (POD)-like activity are used in biosensing and antibacterial applications. These results suggest that HEzymes have great potential as new-generation nanozymes.

Dual-Mechanism Tuned Engineered Polyphenols with Cascade Photocatalytic Self-Fenton Reaction for Sustainable Biocidal Coatings.

Traditional disposable personal protective equipment (PPE) only blocks pathogenic bacteria by mechanical filtration, with the risk of recontamination and transmission remaining. Herein, inspired by phenolic-enabled nanotechnology (PEN), we proposed engineered polyphenol coatings by plant-derived aromatic aldehydes and metal involvement, denoted as FQM, to obtain the desired photocatalysis-self-Fenton antibacterial performance. Experiments and theoretical analysis proved the dual mechanism of Fe-induced enhancement: (1) tuning of molecular structure realized improved optical properties; (2) Fe(III)/Fe(II) triggered photocatalytic cascade self-Fenton reaction. Mechanism study reveals FQM killing bacteria by direct-contact ROS attack and gene regulation. Further, the FQM was developed as the ideal antibacterial coating on different fabrics (cloth cotton, polyester, and N95 mask), killing more than 93% of bacteria after 5 cycles of use. Such photocatalysis-self-Fenton coatings based on engineered polyphenols endowed with desirable safety, sustainability, and efficient antibacterial features are promising solutions to meet the challenges of the currently available PPE.

Integrated Design of a Dual-Mode Colorimetric Sensor Driven by Enzyme-like Activity Regulation Strategy for Ultratrace and Portable Detection of Hg2.

Colorimetric analysis for mercury detection has great application potential in the prevention of health damage caused by mercury in the environment. Sensitivity, selectivity, and portability are core competencies of sensors, and concentrating these properties in a single sensor for efficient mercury detection remains a great challenge. Herein, a hollow structure CuS@CuSe@PVP (CCP) was prepared in which the enzyme-like activities could be activated by Hg2+ due to the antagonism between Hg and Se, inspiring the establishment of a colorimetric method for Hg2+ detection. As for Hg2+ detection performance, the linear range (LR) and limit of detection (LOD) were 1-900 and 0.81 nM in the POD-like activity system, respectively. Also, 5-550 nM of LR and 2.34 nM of LOD were achieved in the OD-like activity system. Further, a smartphone-mediated portable RGB nanosensor was fabricated, with a LOD down to 6.65 nM in the POD-like system and 7.97 nM in the OD-like system. Moreover, the excellent self-calibration and satisfactory recovery of 94.77%-106.16% were shown in the application of real water samples analysis. This study represented advanced progress toward emerging applications of nanozymes with multiple enzyme-like activities in heavy metal detection and will accelerate the development of efficient and portable heavy metal sensors.

Probiotic Potential, Antibacterial, and Antioxidant Capacity of Aspergillus luchuensis YZ-1 Isolated From Liubao Tea.

Aspergillus fungi are widely used in the traditional fermentation of food products, so their safety risks and functions are worthy of investigation. In this study, one Aspergillus luchuensis YZ-1 isolated from Liubao tea was identified based on phylogenetic analyses of sequences of three genes coding for internal transcribed spacer 1 (ITS1), ß-tubulin (benA), and calmodulin (CaM). The results of hemolytic activity, DNase activity, cytotoxicity assay, and antibiotic resistance assay indicated that the strain is potentially safe. The excellent gastrointestinal fluid tolerance, acid tolerance, bile tolerance, auto-aggregation, co-aggregation, cell surface hydrophobicity, and adhesion to human colon adenocarcinoma (HT29) cell line were observed on analysis of the probiotic properties. Furthermore, the results of the antibacterial activity of A. luchuensis YZ-1 indicated that the strain had strong antagonistic effects against Gram-negative and Gram-positive bacteria as well as fungi. Simultaneously, the water extracts and 80% ethanolic extracts of A. luchuensis YZ-1 cells also showed strong ABTS, DPPH, and OH- scavenging ability. Taken together, our results suggest that A. luchuensis YZ-1 has desirable functional probiotic properties and can be proposed as a biocontrol agent in the food industry.

Silver metallization-triggered liposome-embedded AIE fluorophore for dual-mode detection of biogenic amines to fight food freshness fraud.

To combat food freshness fraud, it is urgent to develop a method which could realize the detection of biogenic amines (BAs) present in food. In our study, we developed a colorimetric and ratiometric fluorescence dual-mode sensor which integrated with silver metallization-based response system of AIE liposome + OPD + RSM + Ag+ toward BAs in foods for fighting freshness fraud. With the hydrolysis from the alkaline of BAs to resorcinol monoacetate (RSM), the production resorcinol (RS) could metallize silver ion (Ag+) to silver atoms (Ag0) which could lead to a BAs concentration-dependent decrease of the oxidation product 2,3-diaminophenothiazine (DAP) of Ag+ to o-phenylenediamine (OPD). As a result, the dual-mode sensor has a low detection limit and wide linear range in the spiked detection of soy products, pork and milk samples for BAs. Thus, providing a reliable method for food safety and forestalling food freshness fraud.

A multifunctional cascade nanoreactor based on Fe-driven carbon nanozymes for synergistic photothermal/chemodynamic antibacterial therapy.

Healing bacterial chronic wounds caused by hyperglycemia is of great significance to protect the physical and mental health of diabetic patients. In this context, emerging chemodynamic therapy (CDT) and photothermal therapy (PTT) with broad antibacterial spectra and high spatiotemporal controllability have flourished. However, CDT was challenged by the near-neutral pH and inadequate H2O2 surrounding the chronic wound site, while PTT showed overheating-triggered side effects (e.g., damaging the normal tissue) and poor effects on thermotolerant bacterial biofilms. Therefore, we engineered an all-in-one glucose-responsive photothermal nanozyme, GOX/MPDA/Fe@CDs, consisting of glucose oxidase (GOX), Fe-doped carbon dots (Fe@CDs), and mesoporous polydopamine (MPDA), to efficiently treat chronic diabetic wound bacterial infections and eradicate biofilms without impacting the surrounding normal tissues. Specifically, GOX/MPDA/Fe@CDs produced a local temperature (∼ 45.0°C) to enhance the permeability of the pathogenic bacterium and its biofilm upon near-infrared (NIR) 808 nm laser irradiation, which was seized to initiate endogenous high blood glucose to activate the catalytic activity of GOX on the GOX/MPDA/Fe@CD surface to achieve the simultaneous self-supplying of H2O2 and H+, cascade catalyzing •OH production via a subsequent peroxidase-mimetic activity-induced Fenton/Fenton-like reaction. As such, the in vivo diabetic wound infected with methicillin-resistant Staphylococcus aureus was effectively healed after 12.0 days of treatment. This work was expected to provide an innovative approach to the clinical treatment of bacterially infected diabetic chronic wounds. STATEMENT OF SIGNIFICANCE: An all-in-one glucose-responsive photothermal nanozyme GOX/MPDA/Fe@CDs was constructed. Cascade nanozyme GOX/MPDA/Fe@CDs self-supply H2O2 and H+ to break H2O2 and pH limits to fight bacterial infections. Synergistic chemotherapy and photothermal therapy with nanozyme GOX/MPDA/Fe@CDs accelerates healing of biofilm-infected diabetic wounds.

Robust PANI@MXene/GQDs-Based Fiber Fabric Electrodes via Microfluidic Wet-Fusing Spinning Chemistry.

Two-dimensional transition metal titanium carbide (Ti3 C2 Tx ) as a promising candidate material for batteries and supercapacitors has shown excellent electrochemical performance, but it is difficult to meet practical applications because of its poor morphology structure, low mechanical properties, and expensive process. Here, an applied and efficient method based on microfluidic wet-fusing spinning chemistry (MWSC) is proposed to construct hierarchical structure of MXene-based fiber fabrics (MFFs), allowing the availability of MFF electrodes with ultrastrong toughness, high conductivity, and easily machinable properties. First, a dot-sheet structure constructed by graphene quantum dots (GQDs) and MXene nanosheets with multianchor interaction in the microchannel of a microfluidic device enhances the mechanical strength of MXene fibers; next, the interfused fiber network structure of Ti3 C2 Tx /GQDs fabrics assembled by the MWSC process enhances the deformability of the whole fabrics; finally, the core-shell structure of PANI@Ti3 C2 Tx /GQDs architected by in-situ polymerization growth of polyaniline (PANI) nanofibers provides more ion-accessible pathways and sites for kinetic migration and ion accumulation. Through the morphology and microstructure design, this strategy has directive significance to the large-scale preparation of conductive fabric electrodes and provides a viable solution for simultaneously enhancing mechanical strength and electrochemical performance of conductive fabric electrodes.

Allosteric probe-triggered isothermal amplification to activate CRISPR/Cas12a for sensitive electrochemiluminescence detection of Salmonella.

We report an electrochemiluminescence (ECL) sensor for Salmonella detection based on allosteric probe as a bio-recognition element and CRISPR/Cas12a as a signal amplification strategy. In the presence of Salmonella, the structure switching occurs on allosteric probes, resulting in their hybridization with primers to trigger isothermal amplification. Salmonella is then released to initiate the next reaction cycle accompanying by generating a large amount of dsDNA, which are subsequently recognized by CRISPR-gRNA for activating the trans-cleavage activity of Cas12a. Furthermore, the activated Cas12a can indiscriminately cut the ssDNA which is bound to the electrode, enabling the release of the ECL emitter porphyrinic Zr metal - organic framework (MOF, PCN-224) and exhibiting a decreased ECL signal accordingly. The linear range is 50 CFU·mL-1-5 × 106 CFU·mL-1 and the detection limit is calculated to be 37 CFU·mL-1. This method sensitively detects Salmonella in different types of real samples, indicating it is a promising strategy for Salmonella detection.

Ultrathin C3N4 nanosheets-based oxidase-like 2D fluorescence nanozyme for dual-mode detection of organophosphorus pesticides.

Engineering efficient dual-mode portable sensor with built-in cross reference correction is of great significance for onsite reliable and precise detection of organophosphorus pesticides (OPs) and evading the false-positive outputs, especially in emergency case. Currently, most nanozyme-based sensors for OPs monitoring primarily replied on the peroxidase-like activity, which involved unstable and toxic H2O2. In this scenario, a hybrid oxidase-like 2D fluorescence nanozyme (PtPdNPs@g-C3N4) was yielded by in situ growing PtPdNPs in the ultrathin two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanosheet. When acetylcholinesterase (AChE) hydrolyzed acetylthiocholine (ATCh) to thiocholine (TCh), it ablated O2-• from the dissolved O2 catalyzed by PtPdNPs@g-C3N4's oxidase-like activity, hampering the oxidation of o-phenylenediamine (OPD) into 2,3-diaminophenothiazine (DAP). Consequently, with the increasing concentration of OPs which inhibited the blocking effect by inactivating AChE, the produced DAP caused an apparent color change and a dual-color ratiometric fluorescence change in the response system. Through integrating into a smartphone, a H2O2-free 2D nanozyme-based onsite colorimetric and fluorescence dual-mode visual imaging sensor for OPs was proposed with acceptable results in real samples, which holds vast promise for further development of commercial point-of-care testing platform in early warning and controlling of OPs pollution for safeguarding environmental health and food safety.

Schiff-Base Chemistry-Coupled Catechol Oxidase-Like Nanozyme Reaction as a Universal Sensing Mode for Ultrasensitive Biosensing.

Expanding sensing modes and improving catalytic performance of nanozyme-based analytical chemistry are beneficial to realizing the desired biosensing of analytes. Herein, Schiff-base chemistry coupled with a novel catechol oxidase-like nanozyme (CHzyme) is designed and constructed, exhibiting two main advantages, including (1) improving catalytic performance by nearly 2-fold compared with only the oxidase-like role of CHzyme; (2) increasing the designability of the output signal by signal transduction of cascade reaction. Thereafter, the substrate sensing modes based on a cascade reaction between the CHzyme-catalyzed reaction and Schiff-base chemistry are proposed and comprehensively studied, containing catalytic substrate sensing mode, competitive substrate sensing mode, and generated substrate sensing mode, expecting to be employed in environmental monitoring, food analyses, and clinical diagnoses, respectively. More meaningfully, the generated substrate sensing mode is successfully applied to construct a cascade reaction coupling ratiometric fluorescent immunoassay for the detection of clenbuterol, increasing 15-fold in detection sensitivity compared with the traditional enzyme-linked immunosorbent assay. It is expected that the expanded universal substrate sensing modes and the Schiff-base chemistry-enhanced nanozyme can enlighten the exploration of innovative biosensors.