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1.
J Hazard Mater ; 480: 136015, 2024 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-39366039

RESUMO

The intelligently efficient, reliable, economical and portable onsite assay toward pyrethroid pesticides (PPs) residues is critical for food safety analysis and environmental pollution traceability. Here, a fluorescent nanozyme Cu-ATP@ [Ru(bpy)3]2+ with laccase-like activity was designed to develop a versatile machine learning-assisted colorimetric and fluorescence dual-modal assay for efficient onsite intelligent decision recognition and quantification of PPs residues. In the presence of alkaline phosphatase (ALP), the laccase-like activity of Cu-ATP@ [Ru(bpy)3]2+ was enhanced to oxidize colorless o-phenylenediamine (OPD) into dark-yellow 2,3-diaminophenazine (DAP) via electron transfer, appearing a new yellow fluorescence at 550 nm. Meanwhile, the red fluorescence of Cu-ATP@ [Ru(bpy)3]2+ at 600 nm was quenched due to the internal filter effect (IFE) of DAP towards Cu-ATP@ [Ru(bpy)3]2+. However, the selective inhibition of PPs toward ALP activity enabled to observe a dual-modal response of PPs concentration-dependent decrease in colorimetric signal and enhancement in the fluorescence intensity ratio of F600 nm/F550 nm. On this basis, both the colorimetric and fluorescence images were captured and processed with a home-made WeChat applet-installed smartphone to extract the corresponding image color information, thus achieving machine learning-assisted onsite real-time and dynamic intelligent decision recognition and quantification of PPs residues in real samples, which shows a promising potential in safeguarding food safety and environmental health.

2.
Anal Chem ; 2024 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-39252431

RESUMO

Efficient field enhancement effects through plasmonic chemistry for ultrasensitive biosensing still face a great challenge. Herein, nanoconfinement engineering accumulation and synergistic effects are used to develop a "plasmonic storms" strategy with a high field enhancement effect, and gold nanoparticles (AuNPs) are used as active sites for a proof of concept because of their distinctive localized surface plasmon resonance and neighborly coupled electromagnetic field. Briefly, a large number of AuNPs are selectively and accurately stacked in the confined nanocavity of the bowl-like nanostructure through an in situ-synthesized strategy, which provides a space for strong coupling of electromagnetic fields between these adjacent AuNPs, forming "plasmonic storms" with an enhanced field that is 3 orders of magnitude higher than that of free AuNPs. The proposed nanoconfinement-engineered "plasmonic storms" are demonstrated by surface-enhanced Raman scattering (SERS) and photothermal experiments and theoretically visualized by finite element simulation. Finally, the proposed "plasmonic storms" are used for enhanced colorimetric/SERS/photothermal immunochromatographic assay to detect Salmonella typhimurium with the help of a machine learning algorithm, achieving a low limit of detection of 142 CFU mL-1, highlighting the potential of nanoconfinement in biosensing.

3.
Anal Chem ; 96(33): 13512-13521, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39110961

RESUMO

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.


Assuntos
Aptâmeros de Nucleotídeos , Caprilatos , Fluorocarbonos , Aptâmeros de Nucleotídeos/química , Fluorocarbonos/química , Fluorocarbonos/análise , Caprilatos/análise , Caprilatos/química , Oxirredutases/metabolismo , Técnicas Biossensoriais/métodos , Poluentes Atmosféricos/análise , Monitoramento Ambiental/métodos , Limite de Detecção
4.
Anal Chem ; 96(36): 14706-14713, 2024 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-39207941

RESUMO

Concerns regarding the hazard of the carcinogenic ethyl carbamate (EC) have driven attempts to exploit efficient, timely, straightforward, and economic assays for warning early food safety. Here, we proposed a novel molecularly imprinted polymer Co@MOF-MIP, with a high peroxidase (POD)-like activity and a bright blue fluorescence emission, to develop a versatile visual assay for colorimetric, fluorescent, and photothermal trimodal detection and logic gate outputting of EC. Briefly, the POD-like activity of Co@MOF-MIP made it to decompose H2O2 into ·OH for oxidizing colorless 3,3',5,5'-tetramethylbenzidine (TMB) into a blue oxTMB, resulting in a 660 nm irradiated photothermal effect and bursting the blue fluorescence of Co@MOF-MIP via inner filter effect, observing a decreased fluorescence signal together with an increased colorimetric and 660 nm irradiated photothermal signals. However, EC could specifically fill the imprinted cavities of Co@MOF-MIP to block the catalytic substrates TMB and H2O2 out of Co@MOF-MIP for further reacting with the inside catalytic center of Co2+, resulting in the transformation suppressing of TMB into oxTMB, yielding an EC concentration-dependent trimodal responses in fluorescence signal enhancement, colorimetric, and 660 nm irradiated photothermal signal decreases. Assisted by the portable devices such as smartphones and hand-held thermal imagers, a visual onsite portable trimodal analytical platform was proposed for EC fast and accurate detection with the low detection limits of 1.64, 1.24, and 1.78 µg/L in colorimetric, fluorescent, and photothermal modes, respectively. Interestingly, these reactive events could be programmed by the classical Boolean logic gate analysis to offer a novel promising avenue for the big data Internet of Things monitoring and warning early residual EC in a more intelligent, dynamical, fast, and accurate manner, safeguarding food safety.


Assuntos
Colorimetria , Uretana , Uretana/química , Impressão Molecular , Estruturas Metalorgânicas/química , Cobalto/química , Peróxido de Hidrogênio/química , Peróxido de Hidrogênio/análise , Peróxido de Hidrogênio/metabolismo , Polímeros Molecularmente Impressos/química , Benzidinas/química
5.
Food Chem ; 457: 140050, 2024 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-38901348

RESUMO

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.


Assuntos
Carpas , Catequina , Géis , Proteínas Musculares , Sulfitos , Animais , Géis/química , Sulfitos/química , Catequina/química , Catequina/análogos & derivados , Proteínas Musculares/química , Proteínas de Peixes/química , Interações Hidrofóbicas e Hidrofílicas , Oxirredução , Miofibrilas/química
6.
J Hazard Mater ; 474: 134707, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38810578

RESUMO

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.


Assuntos
Carbono , Pontos Quânticos , Uretana , Carbono/química , Pontos Quânticos/química , Fluorescência , Uretana/análise , Oxirredutases/metabolismo , Cério/química , Monitoramento Ambiental/métodos , Limite de Detecção , Acetilcolinesterase/metabolismo , Carcinógenos/análise , Carcinógenos/toxicidade , Poluentes Químicos da Água/análise
7.
Food Chem ; 450: 139242, 2024 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-38631208

RESUMO

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.


Assuntos
Técnicas Biossensoriais , Hipoxantina , Produtos da Carne , Técnicas Biossensoriais/instrumentação , Hipoxantina/análise , Hipoxantina/química , Produtos da Carne/análise , Xantina Oxidase/química , Xantina Oxidase/metabolismo , Contaminação de Alimentos/análise , Animais , Corantes Fluorescentes/química , Fluorescência , Smartphone , Colorimetria/métodos
8.
J Hazard Mater ; 469: 133871, 2024 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-38428301

RESUMO

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.


Assuntos
Peróxido de Hidrogênio , Eliminação de Resíduos , Carbono , Hidrogéis , Alimentos , Colorimetria/métodos
9.
Talanta ; 272: 125773, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38359720

RESUMO

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.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Pontos Quânticos , Ressonância de Plasmônio de Superfície/métodos , Ouro/química , Pontos Quânticos/química , Medições Luminescentes/métodos , Nanopartículas Metálicas/química , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Limite de Detecção
10.
J Affect Disord ; 347: 509-514, 2024 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-38036048

RESUMO

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.


Assuntos
Transtornos Mentais , Distúrbios do Início e da Manutenção do Sono , Suicídio , Humanos , Hospitais Gerais , Distúrbios do Início e da Manutenção do Sono/epidemiologia , Pacientes Internados/psicologia , Prevalência , Estudos Prospectivos , Transtornos Mentais/epidemiologia , Transtornos Mentais/psicologia , Suicídio/psicologia , Fatores de Risco
11.
Food Chem ; 439: 138122, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38070231

RESUMO

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.


Assuntos
Oxirredutases , Smartphone , Fluorescência , Oxirredução , Espectrometria de Fluorescência/métodos , Corantes Fluorescentes
12.
J Agric Food Chem ; 71(43): 16381-16390, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37908144

RESUMO

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.


Assuntos
Colorimetria , Peróxido de Hidrogênio , Humanos , Reprodutibilidade dos Testes , Carne , Peroxidases , Hipoxantinas
13.
Nano Lett ; 23(20): 9563-9570, 2023 10 25.
Artigo em Inglês | MEDLINE | ID: mdl-37819937

RESUMO

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.


Assuntos
Compostos Férricos , Polifenóis , Polifenóis/farmacologia , Polifenóis/química , Têxteis , Antibacterianos/farmacologia , Antibacterianos/química
14.
Adv Sci (Weinh) ; 10(33): e2303078, 2023 11.
Artigo em Inglês | MEDLINE | ID: mdl-37870181

RESUMO

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.


Assuntos
Peroxidase , Elementos de Transição , Entropia , Peroxidases , Catálise , Corantes
15.
Environ Sci Technol ; 57(36): 13397-13407, 2023 09 12.
Artigo em Inglês | MEDLINE | ID: mdl-37643359

RESUMO

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.


Assuntos
Colorimetria , Mercúrio , Calibragem , Limite de Detecção
16.
Acta Biomater ; 168: 580-592, 2023 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-37451659

RESUMO

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.


Assuntos
Diabetes Mellitus , Hiperglicemia , Staphylococcus aureus Resistente à Meticilina , Humanos , Peróxido de Hidrogênio/farmacologia , Terapia Fototérmica , Antibacterianos/farmacologia , Carbono/farmacologia , Glucose , Glucose Oxidase/farmacologia , Nanotecnologia
17.
Food Chem ; 429: 136961, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37499507

RESUMO

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.


Assuntos
Lipossomos , Prata , Aminas Biogênicas/análise , Inocuidade dos Alimentos
18.
Artigo em Inglês | MEDLINE | ID: mdl-37458925

RESUMO

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.

19.
Adv Mater ; 35(38): e2302326, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37354134

RESUMO

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.

20.
Food Chem ; 425: 136382, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37276664

RESUMO

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.


Assuntos
Técnicas Biossensoriais , Estruturas Metalorgânicas , Sistemas CRISPR-Cas , Primers do DNA , DNA de Cadeia Simples , Eletrodos , Salmonella/genética
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