RESUMEN
The development of sensitive, selective, and rapid methods to detect bacteria in complex media is essential to ensuring human health. Virulence factors, particularly pore-forming toxins (PFTs) secreted by pathogenic bacteria, play a crucial role in bacterial diseases and serve as indicators of disease severity. In this study, a nanochannel-based label-free electrochemical sensing platform was developed for the detection of specific pathogenic bacteria based on their secreted PFTs. In this design, wood substrate channels were functionalized with a Fe-based metal-organic framework (FeMOF) and then protected with a layer of phosphatidylcholine (PC)-based phospholipid membrane (PM) that serves as a peroxidase mimetic and a channel gatekeeper, respectively. Using Staphylococcus aureus (S. aureus) as the model bacteria, the PC-specific PFTs secreted by S. aureus perforate the PM layer. Now exposed to the FeMOF, uncharged 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) molecules in the electrolyte undergo oxidation to cationic products (ABTSâ¢+). The measured transmembrane ionic current indicates the presence of S. aureus and methicillin-resistant S. aureus (MRSA) with a low detection limit of 3 cfu mL-1. Besides excellent specificity, this sensing approach exhibits satisfactory performance for the detection of target bacteria in the complex media of food.
Asunto(s)
Toxinas Bacterianas , Técnicas Biosensibles , Técnicas Electroquímicas , Toxinas Bacterianas/metabolismo , Toxinas Bacterianas/análisis , Estructuras Metalorgánicas/química , Staphylococcus aureus Resistente a Meticilina/aislamiento & purificación , Peroxidasa/metabolismo , Peroxidasa/química , Staphylococcus aureus/aislamiento & purificación , Staphylococcus aureus/metabolismoRESUMEN
Enantioselective identification of chiral molecules is of paramount importance in medical science, biochemistry, and pharmaceutics owing to the configuration-dependent activities of enantiomers. However, the identical physicochemical properties of enantiomers remain challenging in chiral sensing. In this study, inspired by the peroxidase-mimicking activity of Fe(III)-based nanomaterials, an enantioselective artificial architecture is constructed on TiO2 nanochannels. Homochiral Ti-based metal-organic frameworks (MOFs) use a 2,2'-bipyridine-5,5'-dicarboxylic acid ligand as the artificial enzyme skeleton, Fe(III) as peroxidase-mimicking centers, and l-tartaric acid (TA) as a chiral recognition selector. Using l-/d-cystine as model enantiomers, the chiral moieties of l-TA on Ti-MOFs allow stereoselective recognition of guest molecules through hydrogen bonds formed between chiral cystine and the host. In a tris(2-carboxyethyl)phosphine hydrochloride-containing environment, the disulfide bonds in cystine molecules are further cleaved, and the HS-tails react with Fe(III) active sites, causing the loss of peroxidase-like performance of nanochannels. Benefitting from the nanochannel architecture's current-potential (I-V) properties, the selective recognition of cystine enantiomers is directly monitored through the peroxidase-like activity change-induced ionic current signatures. This study provides a new and universal strategy for distinguishing disulfide- and thiol-containing chiral molecules.
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Estructuras Metalorgánicas , Nanoestructuras , Cistina , Estereoisomerismo , Depresión , Compuestos FérricosRESUMEN
Enantioselective identification of chiral molecules is regarded as one of the key issues in biological and medical sciences because of their configuration-dependent effects on biological systems. In this study, we developed an electrochemical platform based on a tandem recognition-reaction zone design in TiO2 nanochannels for the specific recognition of reducing enantiomers. In this system, MIL-125(Ti) Ti-metal-organic frameworks, in situ grown in TiO2 nanochannels, provided a homochiral recognition environment via postmodification with l-tartaric acid (l-TA); MnO2 nanosheets possessing both glucose oxidase (GOD)- and peroxidase (POD)-mimicking activities served as the target-reactive zone at the end of the nanochannels. The use of penicillamine (Pen) enantiomers as model-reducing targets facilitated the passage of d-Pen through the homochiral recognition zone, owing to its lower affinity with l-TA. The passed Pen molecules reached the responsive zone and induced a target concentration-dependent MnO2 disassembly. Such target recognition event impaired the cascade GOD- and POD-like activities of MnO2. Combining the enantioselectivity of the recognition nanochannels with the cascade enzyme-like activity of MnO2 toward glucose and 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonate), the quantitative identification of l- and d-Pen was achieved through the changes in transmembrane ionic current induced by the generated charged products. This recognition-reaction zone design paves an effective way for developing a promising electrochemical platform for the identification of reducing enantiomers with improved selectivity and sensitivity.
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Compuestos de Manganeso , Óxidos , Estereoisomerismo , Glucosa Oxidasa , PenicilaminaRESUMEN
Glutathione (GSH) plays a vital role in many physiological processes, and its abnormal levels have been found to be associated with several diseases. In contrast to traditional methods using electron donor-containing electrolytes for photoelectrochemical (PEC) sensing, in this study, a target-driven electron donor generation in a PEC electrode was developed to detect GSH. Using well-aligned TiO2 nanotube arrays (TNTs) as the PEC substrate, mesoporous MIL-125(Ti) was grown in the TNTs through an in situ solvothermal method and subsequent two-step annealing treatment. The accommodation capacity of mesoporous MIL-125(Ti) allows a well loading of cystine and Pt nanoclusters (NCs). Taking advantage of the specific cleavage ability of disulfide bonds by GSH, cystine was converted to cysteine, which served as the electron donor for the PEC process. Benefiting from the confinement effect of mesoporous MIL-125(Ti), cysteine was effectively oxidized to cysteine sulfinic acid by the photogenerated holes. Importantly, the highly active Pt NCs decorated in the mesopores not only improved the charge transfer but also accelerated the above oxidation reaction. The synergistic effect of these factors enabled the efficient separation of the photogenerated electron-hole pairs, which induced a significant photocurrent increase and in turn led to the high-sensitivity detection of GSH. Consequently, the proposed PEC biosensor exhibited excellent performance in the detection of GSH in serum specimens. The target-driven electron donor generation designed in this study might open a new route for developing sensitive and selective PEC biosensors with application in complex biological environments.
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Cisteína , Cistina , Electrones , Electrodos , GlutatiónRESUMEN
Enzyme-mimicking nanoparticles play a key role in important catalytic processes, from biosensing to energy conversion. Therefore, understanding and tuning their performance is crucial for making further progress in biological applications. We developed an efficient and sensitive electrochemical method for the real-time monitoring of the glucose oxidase (GOD)-like activity of single nanoparticle through collision events. Using brush-like sulfonate (-SO3-)-doped polyaniline (PANI) decorated on TiO2 nanotube arrays (TiNTs-SPANI) as the electrode, we fabricated a proton reservoir with excellent response and high proton-storage capacity for evaluating the oxidase-like activity of individual Au nanoparticles (AuNPs) via instantaneous collision processes. Using glucose electrocatalysis as a model reaction system, the GOD-like activity of individual AuNPs could be directly monitored via electrochemical tests through the nanoparticle collision-induced proton generation. Furthermore, based on the perturbation of the electrical double layer of SPANI induced by proton injection, we investigated the relationship between the measured GOD-like activities of the plasmonic nanoparticles (NPs) and the localized surface plasmon resonance (LSPR) as well as the environment temperature. This work introduces an efficient platform for understanding and characterizing the catalytic activities of nanozymes at the single-nanoparticle level.
Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Oxidorreductasas , Oro/química , Técnicas Biosensibles/métodos , Protones , Nanopartículas del Metal/química , Glucosa Oxidasa/químicaRESUMEN
Accurate detection of trace biomarkers in biological samples is a key task in diagnostic testing, but it remains challenging due to the high concentration of other physiologically relevant interferences. This work presents a new electrochemiluminescence (ECL) sensing device based on a bio-inspired nanochannel membrane (NM) guarded with two differential gates. The recognition event at the aptamer gate is followed by the permitting of stimulator transport toward the metal-organic framework (MOF) gate. Proof of concept application is evaluated using cytochrome C (Cytc) as the analyte, and glucose, a commonly existing nutriment as the stimulator. The oxidase-mimic plasmonic nanoparticles induce an effective release of ECL luminophore from the MOF gate. This cascade-gates guarded NM can effectively separate biological matrices from the detection cell. Consequently, the proposed system can achieve direct sensing of 1.0 nm Cytc in undiluted serum within the threshold concentrations of leukemia and lymphoma, making it attractive for point-of-care applications.
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Técnicas Biosensibles , Nanopartículas del Metal , Estructuras Metalorgánicas , Nanopartículas , Mediciones Luminiscentes , Biomarcadores , Técnicas Electroquímicas , Límite de DetecciónRESUMEN
It is important to detect cancer biomarkers at an early stage of tumor development for the effective diagnosis and treatment of cancer. As a well-known probe for detecting superoxide (·O2-) radicals, nitro blue tetrazolium (NBT) can rapidly react with ·O2- to form a hydrophobic formazan precipitate. In this study, by deliberately utilizing this reaction, Pt asymmetrically decorated on a TiO2 nanochannel membrane (Pt/TiNM) is explored to fabricate an electrochemical immunosensing platform with outstanding selectivity and ultrahigh sensitivity. Using NBT as the substrate, hydrophobic formazan precipitation induces a substantial block of ionic diffusion flux in nanochannels. Using alpha fetoprotein (AFP) as the target analyte, the established immunorecognition event was used to induce MoS2-Ab2 conjugates. Thanks to the excellent light-shielding ability of MoS2 nanosheets, the production of ·O2- radicals from the photocatalysis of Pt/TiNM is effectively depressed because of the attenuated arrival of light. The reduced formazan precipitation results in ionic transport changes in nanochannels, which in turn enables the selective recognition of AFP down to 2 ng mL-1. This target-modulated sensing strategy is also capable of sensing other immune targets, thus paving a new way for designing nanochannel-based sensing platforms.
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Técnicas Biosensibles , alfa-Fetoproteínas , Biomarcadores de Tumor , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Formazáns , Molibdeno , Nitroazul de TetrazolioRESUMEN
A novel colorimetric and ratiometric fluorescence sensor has been established based on boron carbon oxynitride quantum dots (BCNO QDs) and Ca2+ for the detection of doxycycline (DOX). BCNO QDs were synthesized by microwave-assisted method with boric acid and ethylenediamine. The fluorescence of BCNO QDs at 425 nm was quenched due to the electrostatic interaction and inner filter effect with doxycycline. Meanwhile, doxycycline was combined with Ca2+ to form a fluorescence complex, which generated a new fluorescence peak at 520 nm. The fluorescence intensity ratio (F520/F425) has a good linear relationship with doxycycline concentration, and the detection limit is 25 nM. Moreover, the fluorescence of the reaction solution showed a concentration-dependent visual color change from blue to green. In order to facilitate further application, a portable fluorescent test paper which is easy to store was prepared. The RGB values of the reaction solution and corresponding test paper were identified by smartphone, and the visual detection of doxycycline was performed by digital image colorimetric analysis. The application of smartphone and fluorescent test paper can effectively shorten the detection time and simplified the operation, providing an effective scheme for quantitative detection of doxycycline in actual samples. Overall, this work provides a method for the detection of doxycycline and shows that the BCNO QDs have great potential application in food safety.
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Puntos Cuánticos , Boro , Calcio , Carbono , Doxiciclina , Colorantes Fluorescentes , Teléfono Inteligente , Espectrometría de Fluorescencia/métodosRESUMEN
Enantioselective sensing of chiral molecules is an important issue for both biomedical research and the pharmaceutical industry. Here, an enantioselective photoelectrochemical (PEC) sensor was constructed by integrating TiO2 nanotubes (NTs) with metal-organic frameworks (MOFs) for the identification of enantiomers. TiO2 NTs prepared by electrochemical anodization can not only be used as the PEC platform but also as the metal-ion precursor to react with terephthalic acid (BDC) to form MIL-125(Ti) in situ. A postsynthetic exchange (PSE) method was used for exchanging the ligand of MIL-125 by 2-aminoterephthalic acid (BDC-NH2) for further functionalization. Homochirality was then successfully introduced into achiral MIL-125-NH2 by postsynthetic modification (PSM) with l-histidine (l-His). The resulting homochiral metal-organic frameworks (MOF)-in-NT architecture exhibits excellent discrimination ability for the chiral recognition of 3,4-dihydroxyphenylalanine (l/d-DOPA) enantiomers. Moreover, by adjusting the charge-carrier separation-induced photocurrent variation mechanism, the as-proposed homochiral PEC electrode exhibits a broad application potential for the discrimination of enantiomers. Because of the construction of binder-free monochiral MOF-in-NT structure directly on a Ti-metal substrate, the valuable feature is that the PEC sensing platform can be used directly, thereby providing a stable, simplified, and low-cost sensing device for the recognition of chiral enantiomers.
Asunto(s)
Estructuras Metalorgánicas , Nanotubos , Electrodos , Estereoisomerismo , TitanioRESUMEN
Pathogenic bacteria can cause the outbreaks of disease and threaten human health, which stimulates the development of advanced detection techniques. Herein, a specific and sensitive electrochemical biosensor for Gram-negative bacteria was established based on the conductive polymer with artificial muscle properties. The effective recognition was achieved through the specific carbohydrate-carbohydrate interaction between gluconamide and lipopolysaccharide. The application of impulse voltage enhances the efficiency of recognition and shortens the detection time through the temporary deformation of the electrode surface, with a limit of detection (LOD) of 1 × 100 CFU/mL and a linear range of 1 × 100 - 1 × 106 CFU/mL for Escherichia coli (E. coli). In addition to the merits of low cost, high efficiency, and rapidity, the developed label-free electrochemical biosensor can also be applicable for other Gram-negative bacteria, owning promising potential in the application of portable devices and paving a potential way for the construction of electrochemical biosensors.
Asunto(s)
Técnicas Biosensibles/métodos , Escherichia coli/aislamiento & purificación , Gluconatos/química , Lipopolisacáridos/química , Pseudomonas putida/aislamiento & purificación , Animales , Técnicas Biosensibles/instrumentación , Agua Potable/microbiología , Técnicas Electroquímicas/instrumentación , Técnicas Electroquímicas/métodos , Electrodos , Escherichia coli/química , Contaminación de Alimentos/análisis , Jugos de Frutas y Vegetales/microbiología , Límite de Detección , Leche/microbiología , Nanoestructuras/química , Polímeros/química , Pseudomonas putida/química , Pirroles/química , Ríos/microbiología , Contaminantes del Agua/análisisRESUMEN
Electroporation induced by the "point discharge" effect is an effective technique for bacteria inactivation. Rapidly monitoring the electroporation-induced inactivation process is important for screening nanomaterials with high antimicrobial performance. In this study, we develop a facile strategy to in situ monitor the electroporation induced antimicrobial mechanism based on the surface-enhanced Raman scattering (SERS) effect of the Au-nanotip arrays. Owning to the high local-electric field (â¼107 V m-1) generated on the Au nanotips, the bacteria are rapidly electroporated and effectively inactivated with ≥99.9% reduction in bacteria colony counts by only applying an external voltage of +0.8 V for 10 s. The related inactivation mechanism is directly verified by the formation of the Prussian blue (PB) nanocrystals by leaking of the uptaken [Fe(CN)6]3- ions from the cleavage area on the cell membrane. These [Fe(CN)6]3- ions react with Fe2+ to form PB nanocrystals onsite as soon as they leak out. The characteristic peak of PB in the cellular Raman-silent region provides a collective monitoring approach for the destruction of microorganisms. The present strategy not only develops a facial method for future use in evaluating electroporation materials, but also paves a rapid way for offering accurate information on some antibacterial and antitumor processes.
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Antibacterianos/farmacología , Escherichia coli/efectos de los fármacos , Ferrocianuros/farmacología , Nanopartículas/química , Staphylococcus aureus/efectos de los fármacos , Antibacterianos/química , Ferrocianuros/química , Pruebas de Sensibilidad Microbiana , Tamaño de la Partícula , Espectrometría Raman , Propiedades de SuperficieRESUMEN
This research was to study the regulation of intravenous administration of human umbilical cord blood mesenchymal stem cells (HUCBMSCs) on secretion of neural specific protein in rats after traumatic brain injury (TBI), and to explore its mechanisms promoting the recovery of neurological function. The TBI models of rats were established. We then injected HUCBMSCs, labelled by Brdu (5-bromo-2-deoxyuridine), into the TBI rats via the tail vein using modified Feeney free-falling method. The levels of neural biochemical indicators (serum S100ß protein, NSE, LDH, CK) of rats were detected in shamed group, injury group and HUCBMSCs-transplanted group. And the morphological changes of brain tissue of rats in the three groups were observed by using HE staining under light microscope. During the whole experiment no immunosuppressant was used for the four groups. From the research, transplant-related death of the rats was not found in transplantation group. In the injury group, rises were found in contents of serum S100ß protein, NSE, LDH, CK in the early stage after the rats were injured, which were much higher than those in shamed group at correspondent time point (P < 0.01). In HUCBMSCs-transplanted group, although these biochemistry indexes were found rising for a short period in the early stage, along with the time, these indexes were obviously lower than in those injury group (P < 0.05). Under light microscopy pathological changes of rats in HUCBMSCs-transplanted group were much slighter than those in injury group. It was well concluded that in the situation of no immuno-suppressants, the intravenous-injected HUCBMSCs could reduce the secretion of serum S100ß protein, NSE, LDH, CK, promote the repair of tissue injury effectively, and promote the functional recovery of neurons.
Asunto(s)
Lesiones Encefálicas/terapia , Trasplante de Células Madre de Sangre del Cordón Umbilical , Trasplante de Células Madre Mesenquimatosas , Neuronas/química , Animales , Biomarcadores/química , Encéfalo/patología , Humanos , RatasRESUMEN
Alternative energy sources are required due to the decline in fossil fuel resources. Therefore, devices that utilize hydrovoltaic technology and light energy have drawn widespread attention because they are emission-free and solar energy is inexhaustible. However, previous investigations mainly focused on accelerating the water evaporation rate at the electrode interface. Here, a cooperative photoelectrochemical effect on a hydrovoltaic chip is achieved using NH2-MIL-125-modified TiO2 nanotube arrays (NTs). This device demonstrated significantly improved evaporation-triggered electricity generation. Under LED illumination, the open-circuit voltage (VOC) of the NH2-MIL-125/TiO2NTs active layer of the hydrovoltaic chip was enhanced by 90.3% (up to 400.2 mV). Furthermore, the prepared hydrovoltaic chip showed good high-salinity tolerance, maintaining 74.6% of its performance even in 5 M NaCl. By introducing a Schiff-based reaction between the active layer and formaldehyde, a fully integrated flexible sensor was successfully fabricated for formaldehyde monitoring, and a low limit of detection of 5.2 × 10-9 M was achieved. This novel strategy for improving the performance of hydrovoltaic devices offers a completely new general approach to construct self-powered devices for point-of-care sensing.
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Técnicas Electroquímicas , Formaldehído , Titanio , Formaldehído/análisis , Formaldehído/química , Titanio/química , Técnicas Electroquímicas/métodos , Técnicas Electroquímicas/instrumentación , Nanotubos/química , Salinidad , Procesos Fotoquímicos , Electrodos , Límite de DetecciónRESUMEN
In all their applications, gas sensors should satisfy several requirements, including low cost, reduced energy consumption, fast response/recovery, high sensitivity, and reliability in a broad humidity range. Unfortunately, the fast response/recovery and sensing reliability under high humidity conditions are often still missing, especially those working at room temperature. In this study, a humidity-resistant gas sensor with an ultrafast response/recovery rate was designed by integrating a defect-rich semiconducting sensing interface and a self-assembled monolayer (SAM) with controllable wettability. As a proof-of-concept application, ammonia (NH3), one of the atmospheric and indoor pollutants, was selected as the target gas. The decoration of interconnected defective CeO2 nanowires on spaced TiO2 nanotube arrays (NTAs) provided superior NH3 sensing performances. Moreover, we showed that manipulating the functional end group of SAMs is an efficient and simple method to adjust the wettability, by which 86% sensitivity retention with an ultrafast response (within 5 s) and a low limit of detection (45 ppb) were achieved even at 75% relative humidity and room temperature. This work provides a new route toward the comprehensive design and application of metal oxide semiconductors for trace gas monitoring under harsh conditions, such as those of agricultural, environmental, and industrial fields.
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Amoníaco , Nanotubos , Humedad , Reproducibilidad de los Resultados , HumectabilidadRESUMEN
As pure antipodes may differ in biological interactions, pharmacology, and toxicity, discrimination of enantiomers is important in the pharmaceutical and agrochemical industries. Two major challenges in enantiomer determination are transducing and amplifying the distinct chiral-recognition signals. In this study, a light-sensitive organic photoelectrochemical transistor (OPECT) with homochiral character is developed for enantiomer discrimination. Demonstrated with the discrimination of glucose enantiomers, the photoelectrochemically active gate electrode is prepared by integrating Au nanoparticles (AuNPs) and a chiral Cu(II)-metal-organic framework (c-CuMOF) onto TiO2 nanotube arrays (TNT). The captured glucose enantiomers are oxidized to hydrogen peroxide (H2O2) by the oxidase-mimicking AuNPs-loaded c-CuMOF. Based on the confinement effect of the mesopocket structure of the c-CuMOF and the remarkable charge transfer ability of the 1D nanotubular architecture, variations in H2O2 yield are translated into significant changes in OPECT drain currents (ID) by inducing a catalytic precipitation reaction. Variations in ID confer a sensitive discrimination of glucose enantiomers with a limit of detection (LOD) of 0.07 µM for L-Glu and 0.05 µM for D-Glu. This enantiomer-driven gate electrode response strategy not only provides a new route for enantiomer identification, but also helps to understand the origin of the high stereoselectivity in living systems.
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Técnicas Biosensibles , Técnicas Electroquímicas , Glucosa , Oro , Peróxido de Hidrógeno , Límite de Detección , Nanopartículas del Metal , Estructuras Metalorgánicas , Estructuras Metalorgánicas/química , Técnicas Biosensibles/instrumentación , Oro/química , Técnicas Electroquímicas/instrumentación , Estereoisomerismo , Nanopartículas del Metal/química , Glucosa/análisis , Glucosa/química , Glucosa/aislamiento & purificación , Peróxido de Hidrógeno/química , Peróxido de Hidrógeno/análisis , Titanio/química , Transistores Electrónicos , Cobre/química , Luz , Monosacáridos/análisis , Monosacáridos/química , Nanotubos/químicaRESUMEN
Herein, a dual-defective graphite carbon nitride (DDCN) was prepared by polymerization under N2 atmosphere combined with oxidation treatment. The luminous intensity of dual-defect graphite phase carbon nitride based on defect state luminescence is significantly improved compared to CN-air. On this basis, a biosensor for CEA detection was constructed based on specific immunobinding of antigen-antibody. It is noted that the biosensor exhibits a wide linear range of 1 × 10-5 â¼ 1 × 102 ngâ¢mL-1, a low detection limit of 3.3 × 10-4 pgâ¢mL-1, a recovery of 94 %â¼105 % and RSD less than 4.41 %. In addition, there was no significant difference to the clinical results, indicating that this work has good clinical application prospects.
RESUMEN
Adenosine triphosphate (ATP) universally exists in all living organisms and holds a paramount role as a fundamental energy molecule in daily life. The abnormal concentration of ATP is closely related to many diseases, making the highly efficient detection of ATP very urgent. In this study, a dual-mode sensing system was developed to detect ATP sensitively and selectively via both DPV and fluorescence (FL) techniques, based on the strong interaction of ATP and Zn (II) nodes of zeolitic imidazolate framework-90 (ZIF-90). The disassembly of ZIF-90 further induced the subsequent release of pre-loaded rhodamine B (RhB). Benefitting from the robust host-guest recognition of ß-cyclodextrin (ß-CD) towards RhB, an enzyme-free and highly specific DPV detection strategy was established with the linear detecting range of 10.0-1.0 × 108 pM and the limit of detection (LOD) as low as 0.13 pM. Meanwhile, the FL sensing mode based on RhB exhibits comparable sensing performance with the linearity range of 10.0-1.0 × 107 pM and the LOD of 0.29 pM. Furthermore, the enzyme-free ATP sensing system exhibit outstanding long-term storage stability. The two-mode sensing platform was successfully applied to detect the ATP in human serum samples with the yielded result highly agree with the results of commercial ELISA kits. This dual-mode sensing platform is inspiring and paves the road for developing high-performance biosensor, demonstrating enormous potential for vitro diagnosis and practice clinic.
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Estructuras Metalorgánicas , Nanopartículas , Zeolitas , Humanos , Adenosina Trifosfato , Ensayo de Inmunoadsorción Enzimática , Límite de DetecciónRESUMEN
Among the various hazardous substances, formaldehyde (HCHO), produced worldwide from wood furniture, dyeing auxiliaries, or as a preservative in consumer products, is harmful to human health. In this study, a sensitive room-temperature HCHO sensor, MTiNCs/Pd, has been developed by integrating Pd nanoclusters (PdNCs) into mesoporous MIL-125(Ti)-decorated TiO2 nanochannel arrays (TiNCs). Thanks to the enrichment effect of the mesoporous structure of MIL-125 and the large surface area offered by TiNCs, the resulting gas sensor accesses significantly enhanced HCHO adsorption capacity. The sufficient energetic active defects formed on PdNCs further allow an electron-extracting effect, thus effectively separating the photogenerated electrons and holes at the interface. The resulting HCHO sensor exhibits a short response/recovery time (37 s/12 s) and excellent sensitivity with a low limit of detection (4.51 ppb) under ultraviolet (UV) irradiation. More importantly, the cyclic redox reactions of Pdδ+ in PdNCs facilitated the regeneration of O2-(ads), thus ensuring a stable and excellent gas sensing performance even under a high-humidity environment. As a proof-of-principle of this design, a wearable gas sensing band is developed for the real-time and on-site detection of HCHO in cigarette smoke, with the potential as an independent device for environmental monitoring and other smart sensing systems.
RESUMEN
Monosaccharides play significant roles in daily metabolism in living organisms. Although various devices have been constructed for monosaccharide identification, most rely on the specificity of the natural enzyme. Herein, inspired by natural ionic channels, an asymmetrical MOF-in-nanochannel architecture is developed to discriminate monosaccharide enantiomers based on cascade reactions by combining oxidase-mimicking and Fenton-like catalysis in homochiral mesoporous CuMOF pockets. The identification performance is remarkably enhanced by the increased oxidase-mimicking activity of Au nanoparticles under a local surface plasmon resonance (LSPR) excitation. The apparent steady-state kinetic parameters and nano-fluidic simulation indicate that the different affinities induced by Au-LSPR excitation and the confinement effect from MOF pockets precipitate the high chiral sensitivity. This study offers a promising strategy for designing an enantiomer discrimination device and helps to gain insight into the origin of stereoselectivity in a natural enzyme.
RESUMEN
Formaldehyde is ubiquitously found in the environment, meaning that real-time monitoring of formaldehyde, particularly indoors, can have a significant impact on human health. However, the performance of commercially available interdigital electrode-based sensors is a compromise between active material loading and steric hindrance. In this work, a spaced TiO2 nanotube array (NTA) was exploited as a scaffold and electron collector in a formaldehyde sensor for the first time. A Sn-based metal-organic framework was successfully decorated on the inside and outside of TiO2 nanotube walls by a facile solvothermal decoration strategy. This was followed by regulated calcination, which successfully integrated the preconcentration effect of a porous Sn-based metal-organic framework (SnMOF) structure and highly active SnO2 nanocrystals into the spaced TiO2 NTA to form a Schottky heterojunction-type gas sensor. This SnMOF/SnO2@TiO2 NTA sensor achieved a high room-temperature formaldehyde response (1.7 at 6 ppm) with a fast response (4.0 s) and recovery (2.5 s) times. This work provides a new platform for preparing alternatives to interdigital electrode-based sensors and offers an effective strategy for achieving target preconcentrations for gas sensing processes. The as-prepared SnMOF/SnO2@TiO2 NTA sensor demonstrated excellent sensitivity, stability, reproducibility, flexibility, and convenience, showing excellent potential as a miniaturized device for medical diagnosis, environmental monitoring, and other intelligent sensing systems.