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1.
Chem Sci ; 15(19): 7308-7315, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38756792

RESUMO

Surface-enhanced Raman scattering (SERS) spectroscopy is an effective technique that can reveal molecular structure and molecular interaction details. Semiconductor-based SERS platforms exhibit multifaceted tunability and unique selectivity to target molecules as well as high spectral reproducibility. However, the detection sensitivity of semiconductors is impeded by inferior SERS enhancement. Herein, a surface and interference co-enhanced Raman scattering (SICERS) platform based on corrugated TiO2 nanotube arrays (c-TiO2 NTs) was developed, and the coupling of structural regulation and photo-induced charge transfer (PICT) effectively optimized the SERS performance of the semiconductor substrate. Due to the regularly oscillating optical properties of the c-TiO2 NTs, well-defined interference patterns were generated and the local electric field was significantly increased, which greatly promoted both the electromagnetic mechanism and PICT processes. The c-TiO2 NTs were subsequently applied as a highly sensitive SICERS substrate to investigate the mechanism of temperature influence on enantioselective identification. This identification process is related to the existence of temperature-sensitive hydrogen bonds and π-π interaction. This work demonstrates a simply prepared, low-cost, and sensitive SERS substrate that enables better investigation into molecular identification.

2.
Biosens Bioelectron ; 258: 116336, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38692222

RESUMO

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.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Glucose , Ouro , Peróxido de Hidrogênio , Limite de Detecção , Nanopartículas Metálicas , Estruturas Metalorgânicas , Estruturas Metalorgânicas/química , Técnicas Biossensoriais/instrumentação , Ouro/química , Técnicas Eletroquímicas/instrumentação , Estereoisomerismo , Nanopartículas Metálicas/química , Glucose/análise , Glucose/química , Glucose/isolamento & purificação , Peróxido de Hidrogênio/química , Peróxido de Hidrogênio/análise , Titânio/química , Transistores Eletrônicos , Cobre/química , Luz , Monossacarídeos/análise , Monossacarídeos/química , Nanotubos/química
3.
ACS Sens ; 9(5): 2520-2528, 2024 05 24.
Artigo em Inglês | MEDLINE | ID: mdl-38723023

RESUMO

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.


Assuntos
Técnicas Eletroquímicas , Formaldeído , Titânio , Formaldeído/análise , Formaldeído/química , Titânio/química , Técnicas Eletroquímicas/métodos , Técnicas Eletroquímicas/instrumentação , Nanotubos/química , Salinidade , Processos Fotoquímicos , Eletrodos , Limite de Detecção
4.
Anal Chem ; 96(19): 7661-7668, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38687969

RESUMO

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 (ABTS•+). 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.


Assuntos
Técnicas Eletroquímicas , Staphylococcus aureus , Staphylococcus aureus/isolamento & purificação , Staphylococcus aureus/metabolismo , Estruturas Metalorgânicas/química , Staphylococcus aureus Resistente à Meticilina/isolamento & purificação , Peroxidase/metabolismo , Peroxidase/química , Toxinas Bacterianas/metabolismo , Toxinas Bacterianas/análise , Técnicas Biossensoriais
5.
ACS Sens ; 9(4): 1644-1655, 2024 04 26.
Artigo em Inglês | MEDLINE | ID: mdl-38503265

RESUMO

Chemiresistive gas sensors based on metal oxides have been widely applied in industrial monitoring, medical diagnosis, environmental pollutant detection, and food safety. To further enhance the gas sensing performance, researchers have worked to modify the structure and function of the material so that it can adapt to different gas types and environmental conditions. Among the numerous gas-sensitive materials, n-type TiO2 semiconductors are a focus of attention for their high stability, excellent biosafety, controllable carrier concentration, and low manufacturing cost. This Perspective first introduces the sensing mechanism of TiO2 nanostructures and composite TiO2-based nanomaterials and then analyzes the relationship between their gas-sensitive properties and their structure and composition, focusing also on technical issues such as doping, heterojunctions, and functional applications. The applications and challenges of TiO2-based nanostructured gas sensors in food safety, medical diagnosis, environmental detection, and other fields are also summarized in detail. Finally, in the context of their practical application challenges, future development technologies and new sensing concepts are explored, providing new ideas and directions for the development of multifunctional intelligent gas sensors in various application fields.


Assuntos
Gases , Nanoestruturas , Titânio , Titânio/química , Gases/análise , Gases/química , Nanoestruturas/química , Humanos , Semicondutores
6.
ACS Sens ; 9(2): 1014-1022, 2024 02 23.
Artigo em Inglês | MEDLINE | ID: mdl-38334494

RESUMO

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.


Assuntos
Amônia , Nanotubos , Umidade , Reprodutibilidade dos Testes , Molhabilidade
7.
Small ; 20(1): e2304792, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37649199

RESUMO

Large-capacity energy storage devices are attracting widespread research attention. However, the decreased capacity of these devices due to cold weather is a huge obstacle for their practical use. In this study, an electrochemical self-adaptive reconstructed Cux S/Cu(OH)2 -based symmetric energy storage device is proposed. This device provides a satisfactorily enhanced photothermal capacity under solar irradiation. After electrochemical reconstruction treatment, the morphological structure is rearranged and the Cux S component is partially converted to electrochemically active Cu(OH)2 with the introduction of a large number of active sites. The resulting Cux S/Cu(OH)2 electrode provides a significant capacitance of 115.2 F cm-2 at 5 mA cm-2 . More importantly, its wide working potential range and superior photo-to-thermal conversion ability endow Cux S/Cu(OH)2 with superb performance as full-purpose photothermally enhanced capacitance electrodes. Under solar irradiation, the surface temperature of Cux S/Cu(OH)2 is elevated by 76.6 °C in only 30 s, and the capacitance is boosted to 230.4% of the original capacitance at a low temperature. Furthermore, the assembled symmetric energy storage device also delivers a photothermal capacitance enhancement of 200.3% under 15 min solar irradiation.

8.
ACS Sens ; 8(11): 4179-4188, 2023 11 24.
Artigo em Inglês | MEDLINE | ID: mdl-37904486

RESUMO

In this study, we developed a gas sensing platform that can sensitively and specifically detect trace H2S in a high-humidity atmosphere at RT. Upon integrating a carbon nitride (C3N4) nanofilm and molybdenum dioxide (MoO2) nanosheets onto nanojungle-like TiO2 nanotube arrays (TiNTs), the fabricated chemiresistor showed rapid response (38 s)/recovery (58 s) abilities and remarkable detection sensitivity for H2S at concentrations down to 2 ppb, with an estimated detection limit of 1.13 ppb at RT and room-environmental light (REL). Importantly, the gas sensor exhibited satisfactory H2S sensing performance even in dark conditions with a response of 1.9 at 200 ppb. In this design, apart from the architectural advantages of the nanojungle-like TiNTs for accelerating the gas flow efficiency and the abundant sensing sites provided by the C3N4 film, the MoO2 nanosheets act as the essential electron pump not only for the H2S response but also for the subsequent recovery process in air. After employing the MoO2 pump onto C3N4/TiNTs, the response time and recovery time of the system are shortened to ∼35 and ∼11%, respectively. Moreover, we demonstrated the good performance of the flexible gas sensor in detecting trace H2S in human exhaled breath with good humidity resistance. These results highlight the possibility of designing chemiresistors operating in RT and REL conditions and to use these environmentally friendly TiO2-based sensors in real applications.


Assuntos
Líquidos Corporais , Humanos , Temperatura , Elétrons , Expiração
9.
ACS Sens ; 8(11): 4189-4197, 2023 11 24.
Artigo em Inglês | MEDLINE | ID: mdl-37870917

RESUMO

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.


Assuntos
Estruturas Metalorgânicas , Nanotubos , Humanos , Reprodutibilidade dos Testes , Temperatura , Formaldeído
10.
Anal Chim Acta ; 1279: 341759, 2023 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-37827662

RESUMO

Alzheimer's disease (AD) is an irreversible brain disorder, which has been found to be associated with neurotoxic amyloid-ß oligomers (AßO). The early diagnosis of AD is still a great challenge. Herein, inspired by the hierarchical channel structure of natural wood, we design and demonstrate a low-cost and sensitive wood channel-based fluidic membrane for electrochemical sensing of AßO1-42. In this design, Zn/Cu-2-methylimidazole (Zn/Cu-Hmim) with artificial peroxidase (POD)-like activity was asymmetrically fabricated at one side of the wood channels by biomimetic mineralization and a subsequent ion exchange reaction. The strong affinity between Cu(II) and AßO1-42 enables Cu(II) species in Zn/Cu-Hmim to be extracted by AßO1-42, thus suppressing the POD-like performance via Zn/Cu-Hmim disassembly. Using Zn/Cu-Hmim to catalyze the oxidation reaction of 2,2'-diazo-bis-3-ethylbenzothiazoline-6-sulfonic acid (ABTS) by H2O2, the current-voltage (I-V) properties of wood channels are influenced by the generated oxidation product (ABTS•+), thus providing information useful for the quantitative analysis of AßO1-42. Importantly, the three aggregation states of Aß1-42 (AßM1-42, AßO1-42, and AßF1-42) can also be identified, owing to the affinity difference and available reaction sites. The proposed wood membrane provides a novel, assessable, and scalable channel device to develop sensitive electrochemical sensors; moreover, the sustainable wood materials represent alternative candidates for developing channel-structured sensing platforms.


Assuntos
Doença de Alzheimer , Peptídeos beta-Amiloides , Peptídeos beta-Amiloides/química , Peróxido de Hidrogênio , Madeira/química , Doença de Alzheimer/diagnóstico , Antioxidantes , Cobre/química
11.
Anal Chem ; 95(38): 14465-14474, 2023 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-37699410

RESUMO

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.


Assuntos
Compostos de Manganês , Óxidos , Estereoisomerismo , Glucose Oxidase , Penicilamina
12.
Micromachines (Basel) ; 14(8)2023 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-37630083

RESUMO

The Bird-like Flapping-wing Air Vehicle (BFAV) is a robotic innovation that emulates the flight patterns of birds. In comparison to fixed-wing and rotary-wing air vehicles, the BFAV offers superior attributes such as stealth, enhanced maneuverability, strong adaptability, and low noise, which render the BFAV a promising prospect for numerous applications. Consequently, it represents a crucial direction of research in the field of air vehicles for the foreseeable future. However, the flapping-wing vehicle is a nonlinear and unsteady system, posing significant challenges for BFAV to achieve autonomous flying since it is difficult to analyze and characterize using traditional methods and aerodynamics. Hence, flight control as a major key for flapping-wing air vehicles to achieve autonomous flight garners considerable attention from scholars. This paper presents an exposition of the flight principles of BFAV, followed by a comprehensive analysis of various significant factors that impact bird flight. Subsequently, a review of the existing literature on flight control in BFAV is conducted, and the flight control of BFAV is categorized into three distinct components: position control, trajectory tracking control, and formation control. Additionally, the latest advancements in control algorithms for each component are deliberated and analyzed. Ultimately, a projection on forthcoming directions of research is presented.

13.
Anal Chem ; 95(35): 13242-13249, 2023 09 05.
Artigo em Inglês | MEDLINE | ID: mdl-37615488

RESUMO

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.


Assuntos
Cisteína , Cistina , Elétrons , Eletrodos , Glutationa
14.
ACS Sens ; 8(9): 3487-3497, 2023 09 22.
Artigo em Inglês | MEDLINE | ID: mdl-37643286

RESUMO

The accurate, sensitive, and selective on-site screening of volatile aldehyde biomarkers for lung cancer is of utmost significance for preclinical cancer diagnosis and treatment. Applying surface-enhanced Raman scattering (SERS) for gas sensing remains difficult due to the small Raman cross section of most gaseous molecules and interference from other components in exhaled breath. Using an Au asymmetrically coated TiO2 nanochannel membrane (Au/TiO2 NM) as the substrate, a ZIF-8-covered Au/TiO2 NM SERS sensing substrate is designed for the detection of exhaled volatile organic compounds (VOCs). Au/TiO2 NM provides uniformly amplified Raman signals for trace measurements in this design. Importantly, the interfacial nanocavities between Au nanoparticles (NPs) and metal-organic frameworks (MOFs) served as gaseous confinement cavities, which is the key to enhancing the capture and adsorption ability toward gaseous analytes. Both ends of the membrane are left open, allowing gas molecules to pass through. This facilitates the diffusion of gaseous molecules and efficient capture of the target analyte. Using benzaldehyde as a typical gas marker model of lung cancer, the Schiff base reaction with a Raman-active probe molecule 4-aminothiophene (4-ATP) pregrafted on Au NPs enabled trace and multicomponent detection. Moreover, the combination of machine learning (ML) and Raman spectroscopy eliminates subjective assessments of gaseous aldehyde species with the use of a single feature peak, allowing for more accurate identification. This membrane sensing device offers a promising design for the development of a desktop SERS analysis system for lung cancer point-of-care testing (POCT).


Assuntos
Neoplasias Pulmonares , Nanopartículas Metálicas , Humanos , Aldeídos , Ouro , Biomarcadores , Gases , Neoplasias Pulmonares/diagnóstico
15.
Anal Chem ; 95(31): 11807-11814, 2023 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-37497564

RESUMO

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.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Oxirredutases , Ouro/química , Técnicas Biossensoriais/métodos , Prótons , Nanopartículas Metálicas/química , Glucose Oxidase/química
16.
ACS Nano ; 17(14): 13296-13309, 2023 07 25.
Artigo em Inglês | MEDLINE | ID: mdl-37399243

RESUMO

Skin infections are major threats to human health, causing ∼500 incidences per 10 000 person-year. In patients with diabetes mellitus, particularly, skin infections are often accompanied by a slow healing process, amputation, and even death. Timely diagnosis of skin infection strains and on-site therapy are vital in human health and safety. Herein, a double-layered "test-to-treat" pad is developed for the visual monitoring and selective treatment of drug-sensitive (DS)/drug-resistant (DR) bacterial infections. The inner layer (using carrageenan hydrogel as a scaffold) is loaded with bacteria indicators and an acid-responsive drug (Fe-carbenicillin frameworks) for infection detection and DS bacteria inactivation. The outer layer is a mechanoluminescence material (ML, CaZnOS:Mn2+) and visible-light responsive photocatalyst (Pt@TiO2) incorporated elastic polydimethylsiloxane (PDMS). On the basis of the colorimetric sensing result (yellow for DS-bacterial infection and red for DR-bacterial infection), a suitable antibacterial strategy is guided and then performed. Two available bactericidal routes provided by double pad layers reflect the advantage. The controllable and effective killing of DR bacteria is realized by in situ generated reactive oxygen species (ROSs) from the combination of Pt@TiO2 and ML under mechanical force, avoiding physical light sources and alleviating off-target side effects of ROS in biomedical therapy. As a proof-of-concept, the "test-to-treat" pad is applied as a wearable wound dressing for sensing and selectively dealing with DS/DR bacterial infections in vitro and in vivo. This multifunctional design effectively reduces antibiotic abuse and accelerates wound healing, providing an innovative and promising Band-Aid strategy in point-of-care diagnosis and therapy.


Assuntos
Anti-Infecciosos , Infecções Bacterianas , Infecção dos Ferimentos , Humanos , Titânio , Antibacterianos/farmacologia , Bactérias , Hidrogéis
17.
J Chromatogr A ; 1704: 464134, 2023 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-37307635

RESUMO

Metal-organic frameworks (MOFs) demonstrate strong potential in biosample separation. However, the obtained MOFs powders are unsuitable for recovery techniques in an aqueous solution, especially the challenges of withdrawing MOFs particles and expanding their functions for specific applications. Herein, a general strategy is designed utilizing metal oxide-nanochannel arrays as precursors and templates for in-situ selective growth of MOFs structures. The exemplary MOFs (Ni-bipy) with tailored composition are selectively grown in NiO/TiO2 nanochannel membrane (NM) using NiO as the sacrificial precursor, which enables one to achieve a ∼262 times concentration of histidine-tagged proteins within 100 min. The significantly improved adsorption efficiency in a wide pH range and the effective enrichment from a complex matrix as a nanofilter illustrate the great potential of MOFs in nanochannels membranes for the high-efficiency recovery of essential proteins in complex biological samples. The porous self-aligned Ni-MOFs/TiO2 NM exhibits biocompatibility and flexible functionalities, which is desirable for the generation of multifunctional nanofilter devices and developing biomacromolecule delivery vehicles.


Assuntos
Estruturas Metalorgânicas , Adsorção , Cromatografia , Excipientes
18.
ACS Sens ; 8(7): 2824-2833, 2023 07 28.
Artigo em Inglês | MEDLINE | ID: mdl-37347220

RESUMO

As a biomarker of periodontitis, sensitive and timely monitoring of hydrogen sulfide (H2S) in exhaled breath at room temperature (RT) is important for the early intervention of oral diseases. However, the required high operation temperature to achieve high sensitivity is still a technical challenge for directly monitoring exhaled breath. In this study, by integrating metal-organic frameworks (MOFs) into self-aligned TiO2 nanotube arrays (NTs), a chemiresistor gas sensor with outstanding sensitivity and selectivity was constructed for the detection of H2S at RT. The precise regulation of a Co(III)-based MOF CoBDC-NH2 (BDC-NH2 = 2-aminoterephthalic acid) not only induced more active surface for the preconcentration of the target gas but also caused a buildup of Z-scheme heterojunctions in the H2S atmosphere that induced an ultrahigh sensitivity at RT via 365 nm light-emitting diode irradiation. The response and recovery times decreased to ∼50 and ∼28%, respectively, when this system was exposed to UV light. The sensing chips based on the as-prepared TiO2/CoBDC-NH2 NTs exhibited the highest-ranking H2S sensing performance, i.e., a limit of detection of 1.3 ppb and excellent selectivity even to 100 times high concentration of interference gases, owing to the synergistic chemical environment provided by NH2-functionalized Co-MOFs and abundant photogenerated electrons provided by Z-scheme heterojunctions. This sensing chip was also used in a practical application for the timely monitoring of halitosis from direct exhaled breath. This study provides a reliable and sensitive design for clinically aiding the timely detection of H2S in a complex oral environment.


Assuntos
Testes Respiratórios , Sulfeto de Hidrogênio , Temperatura , Gases
19.
Anal Chem ; 95(20): 8128-8136, 2023 05 23.
Artigo em Inglês | MEDLINE | ID: mdl-37163772

RESUMO

Chiral recognition is a crucial issue in the biomedical and pharmaceutical research communities. Due to the need for expensive equipment, reagents, and external energy, enantiomer identification is difficult to perform outside of a laboratory. Based on water evaporation-induced hydrovoltaic effect, a power-free sensing platform with sensitive chiral recognition capability is proposed for the discrimination of enantiomers. The chiral recognizer was bovine serum albumin (BSA), a naturally occurring protein. Using arginine (Arg) enantiomers as the sensing targets, the difference in enantioselectivity between l-Arg and d-Arg on a BSA-modified porous carbon substrate can be measured directly from the output voltage. By combining the cyclization reaction between NO and O-phenylenediamine (OPD), it has been discovered that the sensitivity and specificity of enantioselective identification can be significantly enhanced based on the surface charges. The limit of detection (LOD) could be as low as 76.0 nM. In addition, the proposed chips are extremely flexible and can function under deformation without sacrificing output performance. This self-powered chiral recognition chip paves a new path for the detection of chiral molecules at any time, any place, and it also has excellent potential for use in flexible wearable technology.


Assuntos
Arginina , Dispositivos Eletrônicos Vestíveis , Arginina/química , Estereoisomerismo , Água , Soroalbumina Bovina
20.
J Orthop Surg Res ; 18(1): 362, 2023 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-37194103

RESUMO

PURPOSE: To investigate the relationship between neutrophil to lymphocyte ratio (NLR)/platelet to lymphocyte ratio (PLR) with deep venous thrombosis (DVT) following ankle fracture and the diagnostic ability of combination model. METHOD: This retrospective study included patients with a diagnosis of ankle fracture who had undergone preoperative Duplex ultrasound (DUS) examination for detecting the possible deep venous thrombosis (DVT). The variables of interest, the calculated NLR and PLR and others (demographics, injury, lifestyles and comorbidities) were extracted from the medical records. Two independent multivariate logistics regression models were used to detect the relationship between NLR or PLR and DVT. If any, combination diagnostic model was constructed and its diagnostic ability was evaluated. RESULTS: There were 1103 patients included, and 92 (8.3%) were found to have preoperative DVT. The NLR and PLR, which had respective optimal cut-off point of 4 and 200, were significantly different between patients with and without DVT either in continuous or categorical variable. After adjustment for covariates, both NLR and PLR were identified as independent risk factors associated with DVT, with odd ratio of 2.16 and 2.84, respectively. The combination diagnostic model, including NLR, PLR and D-dimer, demonstrated to significantly improved the diagnostic performance than any one alone or combined (all P < 0.05), and the area under the curve was 0.729 (95% CI 0.701-0.755). CONCLUSION: We concluded the relatively low incidence rate of preoperative DVT after ankle fracture, and both NLR and PLR were independently associated with DVT. The combination diagnostic model can be considered as a useful auxiliary tool for identifying high-risk patients for DUS examination.


Assuntos
Fraturas do Tornozelo , Trombose Venosa , Humanos , Neutrófilos , Estudos Retrospectivos , Contagem de Linfócitos , Fraturas do Tornozelo/diagnóstico por imagem , Contagem de Plaquetas , Plaquetas , Linfócitos , Trombose Venosa/diagnóstico por imagem
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