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1.
Anal Chem ; 96(9): 3914-3924, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38387027

RESUMEN

Wearable, noninvasive sensors enable the continuous monitoring of metabolites in sweat and provide clinical information related to an individual's health and disease states. Uric acid (UA) is a key indicator highly associated with gout, hyperuricaemia, hypertension, kidney disease, and Lesch-Nyhan syndrome. However, the detection of UA levels typically relies on invasive blood tests. Therefore, developing a wearable device for noninvasive monitoring of UA concentrations in sweat could facilitate real-time personalized disease prevention. Here, we introduce 1,3,6,8-pyrene tetrasulfonic acid sodium salt (PyTS) as a bifunctional molecule functionalized with Ti3C2Tx via π-π conjugation to design nonenzymatic wearable sensors for sensitive and selective detection of UA concentration in human sweat. PyTS@Ti3C2Tx provides many oxidation-reduction active groups to enhance the electrocatalytic ability of the UA oxidation reaction. The PyTS@Ti3C2Tx-based electrochemical sensor demonstrates highly sensitive detection of UA in the concentration range of 5 µM-100 µM, exhibiting a lower detection limit of 0.48 µM compared to the uricase-based sensor (0.84 µM). In volunteers, the PyTS@Ti3C2Tx-based wearable sensor is integrated with flexible microfluidic sweat sampling and wireless electronics to enable real-time monitoring of UA levels during aerobic exercise. Simultaneously, it allows for comparison of blood UA levels via a commercial UA analyzer. Herein, this study provides a promising electrocatalyst strategy for nonenzymatic electrochemical UA sensor, enabling noninvasive real-time monitoring of UA levels in human sweat and personalized disease prevention.


Asunto(s)
Técnicas Biosensibles , Nitritos , Elementos de Transición , Dispositivos Electrónicos Vestibles , Humanos , Ácido Úrico/análisis , Titanio/análisis , Sudor/química
2.
Anal Chem ; 96(22): 9278-9284, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38768425

RESUMEN

Antibody pharmaceuticals have become the most popular immunotherapeutic drugs and are often administered with low serum drug dosages. Hence, the development of a highly sensitive method for the quantitative assay of antibody levels is of great importance to individualized therapy. On the basis of the dual signal amplification by the glycan-initiated site-directed electrochemical grafting of polymer chains (glyGPC), we report herein a novel strategy for the amplified electrochemical detection of antibody pharmaceuticals. The target of interest was affinity captured by a DNA aptamer ligand, and then the glycans of antibody pharmaceuticals were decorated with the alkyl halide initiators (AHIs) via boronate cross-linking, followed by the electrochemical grafting of the ferrocenyl polymer chains from the glycans of antibody pharmaceuticals through the electrochemically controlled atom transfer radical polymerization (eATRP). As the glycans can be decorated with multiple AHIs and the grafted polymer chains are composed of tens to hundreds of electroactive tags, the glyGPC-based strategy permits the dually amplified electrochemical detection of antibody pharmaceuticals. In the presence of trastuzumab (Herceptin) as the target, the glyGPC-based strategy achieved a detection limit of 71.5 pg/mL. Moreover, the developed method is highly selective, and the results of the quantitative assay of trastuzumab levels in human serum are satisfactory. Owing to its uncomplicated operation and cost-effectiveness, the glyGPC-based strategy shows great promise in the amplified electrochemical detection of antibody pharmaceuticals.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Electroquímicas , Trastuzumab , Técnicas Electroquímicas/métodos , Humanos , Trastuzumab/química , Trastuzumab/sangre , Aptámeros de Nucleótidos/química , Límite de Detección , Polisacáridos/química , Técnicas Biosensibles/métodos , Polímeros/química
3.
Anal Chem ; 96(14): 5437-5445, 2024 Apr 09.
Artículo en Inglés | MEDLINE | ID: mdl-38529794

RESUMEN

The research on fluorescent rotors for viscosity has attracted extensive interest to better comprehend the close relationships of microviscosity variations with related diseases. Although scientists have made great efforts, fluorescent probes for cellular viscosity with both aggregation-induced emissions (AIEs) and large Stokes shifts to improve sensing properties have rarely been reported. Herein, we first report four new meso-C═N-substituted BODIPY-based rotors with large Stokes shifts, investigate their viscosity/AIE characteristics, and perform cellular imaging of the viscosity in subcellular organelles. Interestingly, the meso-C═N-phenyl group-substituted probe 6 showed an obvious 594 nm fluorescence enhancement in glycerol and a moderate 650 nm red AIE emission in water. Further, on attaching CF3 to the phenyl group, a similar phenomenon was observed for 7 with red-shifted emissions, attributed to the introduction of a phenyl group, which plays a key role in the red AIE emissions and large Stokes shifts. Comparatively, for phenyl-group-free probes, both the meso-C═N-trifluoroethyl group and thiazole-substituted probes (8 and 9) exhibited good viscosity-responsive properties, while no AIE was observed due to the absence of phenyl groups. For cellular experiments, 6 and 9 showed good lysosomal and mitochondrial targeting properties, respectively, and were further successfully used for imaging viscosity through the preincubation of monensin and lipopolysaccharide (LPS), indicating that C═N polar groups potentially work as rotatable moieties and organelle-targeting groups, and the targeting difference might be ascribed to increased charges of thiazole. Therefore, in this study, we investigated the structural relationships of four meso-C═N BODIPY-based rotors with respect to their viscosity/AIE characteristics, subcellular-targeting ability, and cellular imaging for viscosity, potentially serving as AIE fluorescent probes with large Stokes shifts for subcellular viscosity imaging.


Asunto(s)
Compuestos de Boro , Colorantes Fluorescentes , Orgánulos , Colorantes Fluorescentes/química , Viscosidad , Tiazoles
4.
Anal Chem ; 95(9): 4570-4575, 2023 03 07.
Artículo en Inglés | MEDLINE | ID: mdl-36825747

RESUMEN

The assay of thrombin levels is integral to the assessment of coagulation function and clinical screening of coagulation disorder-related diseases. In this work, we illustrate the ingenious use of the target-synergized biologically mediated reversible addition-fragmentation chain transfer (RAFT) polymerization (tsBMRP) as a novel amplification strategy for the electrochemical aptamer-based biosensing of thrombin at the femtomolar levels. Briefly, the tsBMRP-based strategy relies on the boronate affinity-mediated decoration of the glycan chain(s) of the target itself with RAFT agents and the subsequent recruitment of signal labels via BMRP, mediated by the direct reduction of RAFT agents by NADH into initiating/propagating radicals. Obviously, the tsBMRP-based strategy is biologically friendly, low-cost, and simple in operation. As thrombin is a glycoconjugate, its electrochemical aptasensing involves the use of the thrombin-binding aptamer (TBA) as the recognition receptor, the site-specific decoration of RAFT agents to the glycan chain of thrombin via boronate affinity, and further the recruitment of ferrocene signal labels via the BMRP of ferrocenylmethyl methacrylate (FcMMA). As boronate affinity results in the decoration of each glycan chain with tens of RAFT agents while BMRP recruits hundreds of signal labels to each RAFT agent-decorated site, the tsBMRP-based strategy allows us to detect thrombin at a concentration of 35.3 fM. This electrochemical aptasensor is highly selective, and its applicability to thrombin detection in serum samples has been further demonstrated. The merits of high sensitivity and selectivity, low cost, good anti-interference capability, and simple operation make the tsBMRP-based electrochemical thrombin aptasensor great promise in biomedical and clinical applications.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Trombina , Polimerizacion , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Límite de Detección
5.
Anal Chem ; 95(37): 14094-14100, 2023 09 19.
Artículo en Inglés | MEDLINE | ID: mdl-37672684

RESUMEN

The rapid quantification of therapeutic monoclonal antibodies (mAbs) is of great significance to their pharmacokinetics/pharmacodynamics (PK/PD) research and the personalized medication for disease treatment. Taking advantage of the direct decoration of tens of redox tags to the target of interest, we illustrate herein an amplification-free ratiometric electrochemical aptasensor for the point-of-care (POC) detection of trace amounts of therapeutic mAbs. The POC detection of therapeutic mAbs involved the use of the methylene blue (MB)-conjugated aptamer as the affinity element and the decoration of therapeutic mAbs with ferrocene (Fc) tags via the boronate crosslinking, in which the MB-derived peak current was used as the reference signal, and the peak current of the Fc tag was used as the output signal. As each therapeutic mAb carries tens of diol sites for the site-specific decoration of the Fc output tags, the boronate crosslinking enabled the amplification-free detection, which is cost-effective and quite simple in operation. In the presence of bevacizumab (BevMab) as the target, the resulting ratiometric signal (i.e., the IFc/IMB value) exhibited a good linear response over the range of 0.025-2.5 µg/mL, and the limit of detection (LOD) of the electrochemical aptasensor was 6.5 ng/mL. Results indicated that the aptamer-based affinity recognition endowed the detection of therapeutic mAbs with high selectivity, while the ratiometric readout exhibited satisfactory reproducibility and robustness. Moreover, the ratiometric electrochemical aptasensor is applicable to the detection of therapeutic mAbs in serum samples. Taking together, the amplification-free ratiometric electrochemical aptasensor holds great promise in the POC detection of therapeutic mAbs.


Asunto(s)
Anticuerpos Monoclonales , Tetranitrato de Pentaeritritol , Sistemas de Atención de Punto , Reproducibilidad de los Resultados , Bevacizumab , Azul de Metileno , Oligonucleótidos
6.
Anal Chem ; 95(25): 9646-9653, 2023 06 27.
Artículo en Inglés | MEDLINE | ID: mdl-37311071

RESUMEN

Fluorescent rotors with aggregation-induced emission (AIE) and organelle-targeting properties have attracted great attention for sensing subcellular viscosity changes, which could help understand the relationships of abnormal fluctuations with many associated diseases. Despite the numerous efforts spent, it remains rare and urgent to explore the dual-organelle targeting probes and their structural relationships with viscosity-responsive and AIE properties. Therefore, in this work, we reported four meso-five-membered heterocycle-substituted BODIPY-based fluorescent probes, explored their viscosity-responsive and AIE properties, and further investigated their subcellular localization and viscosity-sensing applications in living cells. Interestingly, the meso-thiazole probe 1 showed both good viscosity-responsive and AIE (in pure water) properties and could successfully target both mitochondria and lysosomes, further imaging cellular viscosity changes by treating lipopolysaccharide and nystatin, attributing to the free rotation and potential dual-organelle targeting ability of the meso-thiazole group. The meso-benzothiophene probe 3 with a saturated sulfur only showed good viscosity-responsive properties in living cells with the aggregation-caused quenching effect and no subcellular localization. The meso-imidazole probe 2 showed the AIE phenomenon without an obvious viscosity-responsive property with a C═N bond, while the meso-benzopyrrole probe 4 displayed fluorescence quenching in polar solvents. Therefore, for the first time, we investigated the structure-property relationships of four meso-five-membered heterocycle-substituted BODIPY-based fluorescent rotors with viscosity-responsive and AIE properties, and among these, 1 with a C═N bond and a saturated sulfur on the meso-thiazole, potentially contributing to their corresponding AIE and viscosity-responsive properties, served as a sensitive AIE fluorescent rotor for imaging dual-organelle viscosity in both mitochondria and lysosomes.


Asunto(s)
Colorantes Fluorescentes , Orgánulos , Colorantes Fluorescentes/química , Viscosidad , Diagnóstico por Imagen
7.
Anal Chem ; 95(12): 5463-5469, 2023 03 28.
Artículo en Inglés | MEDLINE | ID: mdl-36921250

RESUMEN

As the entering of bacterial endotoxin into blood can cause various life-threatening pathological conditions, the screening and detection of low-abundance endotoxin are of great importance to human health. Taking advantage of signal amplification by target-assisted electrochemically mediated atom transfer radical polymerization (teATRP), we illustrate herein a simple and cost-effective electrochemical aptasensor capable of detecting endotoxin with high sensitivity and selectivity. Specifically, the aptamer receptor was employed for the selective capture of endotoxin, of which the glycan chain was then decorated with ATRP initiators via covalent coupling between the diol sites and phenylboronic acid (PBA) group, followed by the recruitment of ferrocene signal reporters via the grafting of polymer chains through potentiostatic eATRP under ambient temperature. As the glycan chain of endotoxin can be decorated with hundreds of ATRP initiators while the further grafting of polymer chains through eATRP can recruit hundreds to thousands of signal reporters to each initiator-decorated site, the teATRP-based strategy allows for the dual amplification of the detection signal. This dually amplified electrochemical aptasensor has the ability to sensitively and selectively detect endotoxin at a concentration as low as 1.2 fg/mL, and its practical applicability has been further demonstrated using human serum samples. Owing to the simplicity, high efficiency, biocompatibility, and inexpensiveness of the teATRP-based amplification strategy, this electrochemical aptasensor holds great application potential in the sensitive and selective detection of low-abundance endotoxin and many other glycan chain-containing bio-targets.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Humanos , Límite de Detección , Endotoxinas , Polímeros , Oligonucleótidos , Técnicas Electroquímicas
8.
Angew Chem Int Ed Engl ; 62(43): e202312076, 2023 Oct 23.
Artículo en Inglés | MEDLINE | ID: mdl-37667537

RESUMEN

The effective conversion of carbon dioxide (CO2 ) and nitrogen (N2 ) into urea by photocatalytic reaction under mild conditions is considered to be a more environmentally friendly and promising alternative strategies. However, the weak adsorption and activation ability of inert gas on photocatalysts has become the main challenge that hinder the advancement of this technique. Herein, we have successfully established mesoporous CeO2-x nanorods with adjustable oxygen vacancy concentration by heat treatment in Ar/H2 (90 % : 10 %) atmosphere, enhancing the targeted adsorption and activation of N2 and CO2 by introducing oxygen vacancies. Particularly, CeO2 -500 (CeO2 nanorods heated treatment at 500 °C) revealed high photocatalytic activity toward the C-N coupling reaction for urea synthesis with a remarkable urea yield rate of 15.5 µg/h. Besides, both aberration corrected transmission electron microscopy (AC-TEM) and Fourier transform infrared (FT-IR) spectroscopy were used to research the atomic surface structure of CeO2 -500 at high resolution and to monitor the key intermediate precursors generated. The reaction mechanism of photocatalytic C-N coupling was studied in detail by combining Density Functional Theory (DFT) with specific experiments. We hope this work provides important inspiration and guiding significance towards highly efficient photocatalytic synthesis of urea.

9.
Anal Chem ; 94(39): 13516-13521, 2022 10 04.
Artículo en Inglés | MEDLINE | ID: mdl-36130914

RESUMEN

Tumor biomarkers are of great value in the liquid biopsy of malignant tumors. In this work, a simple and cost-friendly electrochemical aptasensor was presented for the highly sensitive and selective detection of glycoprotein tumor biomarkers. The DNA aptamer-modified electrode was used as the sensing interface to specifically capture the target glycoprotein tumor biomarkers, to which the alkyl halide initiators for atom transfer radical polymerization (ATRP) were then attached via the esterification crosslinking between the boronic acid group and the cis-dihydroxyl sites of the conjugated oligosaccharide chains on glycoprotein tumor biomarkers followed by the growth of long-chain polymers through electrochemically controlled ATRP (eATRP) to efficiently recruit the ferrocene detection tags. As there are tens to hundreds of cis-dihydroxyl sites on a glycoprotein tumor biomarker for attaching ATRP initiators while each long-chain polymer can recruit hundreds to thousands of ferrocene detection tags, a significantly high current signal can be generated even in the presence of ultralow-abundance targets. Hence, the eATRP-based electrochemical aptasensor is capable of sensitively and selectively detecting glycoprotein tumor biomarkers. Using alpha-fetoprotein as the model target, the limit of detection was demonstrated to be 0.32 pg/mL. Moreover, the aptasensor has been successfully applied to detect glycoprotein tumor biomarkers in human serum samples. In view of its high sensitivity and selectivity, simple operation, and cost-friendliness, the eATRP-based electrochemical aptasensor shows great promise in the glycoprotein-based liquid biopsy of malignant tumors, even at the early stage of development.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Biomarcadores de Tumor , Ácidos Borónicos , ADN/genética , Técnicas Electroquímicas , Compuestos Ferrosos , Humanos , Límite de Detección , Metalocenos , Polimerizacion , Polímeros , alfa-Fetoproteínas
10.
Anal Chem ; 94(20): 7319-7328, 2022 05 24.
Artículo en Inglés | MEDLINE | ID: mdl-35536877

RESUMEN

Sweat pH is a critical indicator for evaluating human health. With the extensive attention on the wearable and flexible biosensing devices, the technology for the monitoring of human sweat can be realized. In this study, a sensitive, miniaturized, and flexible electrochemical sweat pH sensor was developed for the continuous and real-time monitoring of the hydrogen-ion concentration in human sweat. A flexible electrode was fabricated on the poly(ethylene terephthalate) (PET) substrate by a simple and low-cost screen-printing technology, which was based on the integration of fluoroalkyl silane-functionalized Ti3C2Tx (F-Ti3C2Tx) and the polyaniline (PANI) membrane technology instead of the traditional ion-sensitive membrane. The surface functionalization strategy for Ti3C2Tx with perfluorodecyltrichlorosilane can provide environmental stability. Functionalized Ti3C2Tx (F-Ti3C2Tx) was doped with PANI to obtain improved responsiveness, sensitivity, and reversibility. The constructed microsize, portable, and wearable F-Ti3C2Tx/PANI pH sensor aimed to real-time monitor the pH value of human sweat during exercise. On-body sweat pH monitoring for females and males, respectively, exhibited high accuracy and continuous stability compared with ex situ analyses. This study thus offers a facile and practical solution for developing a highly reliable MXene-based mini-type pH sensor to realize the online monitoring of human sweat pH.


Asunto(s)
Técnicas Biosensibles , Dispositivos Electrónicos Vestibles , Femenino , Humanos , Concentración de Iones de Hidrógeno , Interacciones Hidrofóbicas e Hidrofílicas , Sudor/química , Titanio/análisis
11.
Anal Chem ; 94(50): 17733-17738, 2022 12 20.
Artículo en Inglés | MEDLINE | ID: mdl-36475636

RESUMEN

As lipopolysaccharide (LPS) is closely associated with sepsis and other life-threatening conditions, the point-of-care (POC) detection of LPS is of significant importance to human health. In this work, we illustrate an electrochemical aptasensor for the POC detection of low-abundance LPS by utilizing boronate affinity (BA) as a simple, efficient, and cost-effective amplification strategy. Briefly, the BA-amplified electrochemical aptasensing of LPS involves the tethering of the aptamer receptors and the BA-mediated direct decoration of LPS with redox signal tags. As the polysaccharide chain of LPS contains hundreds of cis-diol sites, the covalent crosslinking between the phenylboronic acid group and cis-diol sites can be harnessed for the site-specific decoration of each LPS with hundreds of redox signal tags, thereby enabling amplified detection. As it involves only a single-step operation (∼15 min), the BA-mediated signal amplification holds the significant advantages of unrivaled simplicity, rapidness, and cost-effectiveness over the conventional nanomaterial- and enzyme-based strategies. The BA-amplified electrochemical aptasensor has been successfully applied to specifically detect LPS within 45 min, with a detection limit of 0.34 pg/mL. Moreover, the clinical utility has been validated based on LPS detection in complex serum samples. As a proof of concept, a portable device has been developed to showcase the potential applicability of the BA-amplified electrochemical LPS aptasensor in the POC testing. In view of its simplicity, rapidness, and cost-effectiveness, the BA-amplified electrochemical LPS aptasensor holds broad application prospects in the POC testing.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Nanoestructuras , Humanos , Lipopolisacáridos , Técnicas Electroquímicas , Límite de Detección , Oro
12.
Anal Chem ; 94(46): 16246-16253, 2022 11 22.
Artículo en Inglés | MEDLINE | ID: mdl-36368001

RESUMEN

A near-infrared (NIR) light-driven NaYF4:Yb/Er-TiO2-Ti3C2 (NYF-TiO2-Ti3C2) heterostructure-based photoelectrochemical (PEC) biosensing platform was constructed for highly sensitive d-serine (d-ser) detection. Accurate d-ser detection depends on the model biocatalyst, d-amino acid oxidase (DAAO), which converts d-ser into hydroxypyruvate and an equimolar concentration of hydrogen peroxide (H2O2) via an enzymatic reaction. The TiO2-Ti3C2 semiconductor and NaYF4:Yb/Er optical transducer formed a Schottky junction that provided an irreversible channel for electron transfer. Infrared light was converted into absorbable multiemission light, thereby effectively increasing light absorption. Simultaneously, the generated H2O2 rapidly scavenged photogenerated holes to separate electron-hole pairs, which amplified the photocurrent signal. Under optimal conditions, the NIR light-driven PEC biosensor exhibited an excellent PEC performance for d-ser detection, with a wide linear range of 2-1650 µmol L-1 and detection limit as low as 0.286 µmol L-1. Importantly, high detection reproducibility and accuracy were achieved using this strategy for analyzing human serum and rat cerebrospinal fluid (CSF) specimens. The admirable applicability of the NYF-TiO2-Ti3C2-based PEC biosensor for detecting d-ser may lead to further opportunities for detecting other disease-related biomarkers.


Asunto(s)
Técnicas Biosensibles , Técnicas Electroquímicas , Humanos , Ratas , Animales , Titanio/química , Peróxido de Hidrógeno , Serina , Reproducibilidad de los Resultados , Límite de Detección
13.
Small ; 18(7): e2105770, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-35174634

RESUMEN

The aqueous alkaline rechargeable batteries (AARBs) have an attractive potential for electrochemical energy storage devices. In view of the advantages of high theoretical capacity and desirable negative operating window, bismuth (Bi) has been deemed as a hopeful anode material for AARBs. Unfortunately, intensive reported works of Bi anode are still confronted with limited capacity and poor cycling stability. Herein, the designed electrodes of different size Bi nanoparticles embedded in porous carbon nanofibers with a contrasting nitrogen doping content are obtained by electrospinning and thermal treatment processes. The effect of the N dopant in carbon shell is demonstrated on the Bi core, which is in favor of enhancing the capacity of Bi anodes. More importantly, the core structure with highly dispersed ultrasmall Bi nanoparticles (<20 nm) in carbon matrix plays a crucial role in long-term durability. Accordingly, the optimized polydisperse ultrasmall Bi nanoparticles confined in N-rich porous carbon nanofibers electrode (Bi@NPCF) presents an admirable capacity of 196.1 mAh g-1 at 3 A g-1 and outstanding durable lifespan (retain 116.95% after 10 000 cycles). In addition, the fabricated Bi@NPCF//NiCo2 O4 battery exhibits an exceptional energy and power density with durable stability (95.9% after 5000 cycles).

14.
Langmuir ; 38(45): 13668-13673, 2022 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-36326721

RESUMEN

In recent years, it has been very interesting to dynamically adjust the emission of circularly polarized luminescence (CPL) materials through external stimulation due to their applications and the fundamental interest in them. In this work, luminescence-tunable and light-responsive supramolecular co-assembly CPL-active materials are fabricated by mixing an achiral functional spiropyran (SP-COOH) molecule with a chiral gelator. The spiropyran achieves a reversible change between a white closed ring state spiropyran and a purple zwitterionic merocyanine state in supramolecular co-assembly gels under alternate visible (vis) and ultraviolet (UV) light irradiation. The gel shows strong CPL signals due to the chirality transfer in co-assembly systems. These signals could change reversibly under alternate exposure to UV and vis light. Therefore, utilizing the multistimulus-responsive CPL signals in different states, a CPL switch of the supramolecular system signal according to the combinatorial control of UV-vis light irradiation is constructed.

15.
Crit Rev Food Sci Nutr ; 62(13): 3490-3498, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-33372540

RESUMEN

Glycated lipids are formed by a Maillard reaction between the aldehyde group of a reducing sugar with the free amino group of an amino-lipid. The formation and accumulation of glycated lipids are closely related to the prognosis of diabetes, vascular disease, and cancer. However, it is not clear whether food-derived glycated lipids pose a direct threat to the human body. In this review, potentially harmful effect, distribution, formation environment and mechanism, and determination and inhibitory methods of glycated lipids are presented. Future research directions for the study of food-derived glycated lipids include: (1) understanding their digestion, absorption, and metabolism in the human body; (2) expanding the available database for associated risk assessment; (3) relating their formation mechanism to food production processes; (4) revealing the formation mechanism of food-derived glycated lipids; (5) developing rapid, reliable, and inexpensive determination methods for the compounds in different foods; and (6) seeking effective inhibitors. This review will contribute to the final control of food-derived glycated lipids.


Asunto(s)
Alimentos , Reacción de Maillard , Alérgenos , Manipulación de Alimentos , Humanos , Lípidos
16.
Analyst ; 147(24): 5739-5746, 2022 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-36409228

RESUMEN

The hydrogen peroxide (H2O2) levels in living organisms and environment have strong effects on many biological processes inducing cell apoptosis/cell necrosis and wound disinfection. Therefore, it is important to have an accurate and in situ detection of H2O2. Herein, an AuPd@FexOy nanozyme-based electrochemical (EC) sensor (termed as AuPd@FexOy NPs/GCE) with good stability and anti-interference ability has been prepared for the detection of H2O2 by differential pulse voltammetry (DPV) and chronoamperometry dual-measurement modes. The AuPd@FexOy NPs/GCE exhibits good linear relationships in the ranges from 13.0 to 6.0 × 103 µM (DPV measurement) and 50 to 1.0 × 103 µM (chronoamperometry measurement), low detection limits (LODs) of 1.6 µM (DPV measurement) and 3.0 µM (chronoamperometry measurement) and high sensitivities of 83.8 nA µM-1 cm-2 (DPV measurement) and 120.7 nA µM-1 cm-2 (chronoamperometry measurement). The practicability of the as-prepared AuPd@FexOy NPs/GCE has been demonstrated by an in situ real-time detection of H2O2 released from adherent living MCF-7 cells triggered by varying amounts of N-formyl-L-methionyl-L-leucyl-L-phenylalanine (FMLP) from 0.5 to 3.0 µM and the quantitative determination of H2O2 in commercial disinfectants.


Asunto(s)
Desinfectantes , Peróxido de Hidrógeno , Humanos , N-Formilmetionina Leucil-Fenilalanina , Apoptosis , Células MCF-7 , Necrosis
17.
Analyst ; 147(12): 2703-2711, 2022 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-35612404

RESUMEN

The production of reactive oxygen species (ROS) leads to the generation of oxidative stress, which will result in the excessive production and accumulation of melanin in the body and even the occurrence of some skin diseases. The intervention of antioxidants can slow down the rate of melanin formation to some extent. In order to explore the relationship between ROS, melanin and antioxidants, this work investigated the effects of antioxidants on melanin formation by the scavenging of ROS in vitro, where zebrafish were used as the model organism in in vivo experiments. The results showed that the inhibition order of natural antioxidants on melanin formation was GSH > AA > GA and PG > BHT > BHA for synthetic antioxidants. Between natural antioxidants and synthetic antioxidants, the former mainly have a strong scavenging ability on ˙OH and 1O2, while the latter have a strong scavenging ability on O2˙-. At the same time, the results in vivo showed that GSH and PG within a certain concentration not only did not affect the hatchability, survival rate and teratogenic rate of zebrafish embryos, but also can significantly inhibit melanin formation in zebrafish embryos. The results of this study have an important guiding significance for the dosage of antioxidants used in the cosmetics and food industries.


Asunto(s)
Antioxidantes , Melaninas , Animales , Antioxidantes/farmacología , Estrés Oxidativo , Especies Reactivas de Oxígeno , Pez Cebra/metabolismo
18.
Analyst ; 147(14): 3291-3297, 2022 Jul 12.
Artículo en Inglés | MEDLINE | ID: mdl-35726908

RESUMEN

3,4-Methylenedioxyamphetamine (MDA) and 3,4-methylenedioxymethamphetamine (MDMA) are the main components of illicit stimulant drugs, also known as "ecstasy", which belong to psychoactive medicine and tend to be increasingly abused among drug addicts worldwide. Herein, an electrochemical sensor based on molecularly imprinted polydopamine (MIP@PDA) was developed to detect MDA and MDMA using differential pulse voltammetry (DPV). An MIP film on a Au electrode was synthesized via electrochemical polymerization with the safe chemical DA as the polymerization monomer and the uncontrolled pharmaceutical intermediate 3,4-methylenedioxyphenethylamine (MDPEA) as the template molecule, which can provide a great quantity of specific binding sites and expand the practical application of the sensor. Due to the superior affinity of MIP@PDA to the target, the proposed sensor displayed excellent analytical performance, with LODs of 37 nM and 54 nM for the determination of MDA and MDMA, respectively. Additionally, this sensor presented suitable selectivity, stability, reproducibility and detection ability in practical urine samples, which suggested that it is a promising candidate as a rapid diagnostic method in drug investigations.


Asunto(s)
Impresión Molecular , N-Metil-3,4-metilenodioxianfetamina , Técnicas Electroquímicas/métodos , Electrodos , Indoles , Límite de Detección , Impresión Molecular/métodos , Polímeros , Reproducibilidad de los Resultados
19.
Macromol Rapid Commun ; 43(7): e2100905, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35092115

RESUMEN

Creating nanosized pores in layered materials can increase the abundant active surface area and boost potential applications of energy storage devices. Herein, a unique synthetic strategy based on polyaniline (PANI) doped 2D cobalt-iron layered double hydroxide (CoFe-LDH/P) nanomaterials are designed, and the formation of pores at low temperature (80 °C) is developed. It is found that the optimized concentration of PANI creates the nanopores on the CoFe-LDH nanosheets among all other polymers. The well-ordered pores of CoFe-LDH/P allow the high accessibility of the redox-active sites and promote effective ion diffusion. The optimized CoFe-LDH/P2 cathode reveals a specific capacitance 1686 (1096 Cg-1 ) and 1200 Fg-1 (720 Cg-1 ) at 1 and 30 Ag-1 respectively, a high rate capability (71.2%), and a long cycle life (98% over 10 000 cycles) for supercapacitor applications. Charge storage analysis suggests that the CoFe-LDH/P2 electrode displays a capacitive-type storage mechanism (69% capacitive at 1 mV s-1 ). Moreover, an asymmetric aqueous supercapacitor (CoFe-LDH/P2//AC) is fabricated, delivering excellent energy density (75.9 Wh kg-1 at 1124 W kg-1 ) with outstanding stability (97.5%) over 10 000 cycles. This work opens a new avenue for designing porous 2D materials at low temperature for aqueous energy storage devices.


Asunto(s)
Cobalto , Hierro , Compuestos de Anilina/química , Cobalto/química , Hidróxidos
20.
J Environ Manage ; 302(Pt B): 114033, 2022 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-34763188

RESUMEN

Phosphorus was one of the nutrient limitations to vegetations in wetland ecosystem. In peatland, organic phosphorus is accumulated as vegetation residues in anaerobic conditions, affecting the contents of phosphorus pools for long time. It is unclear that different vegetations affect the contents of phosphorus and whether successions of vegetations could reflected by sedimentation of phosphorus forms. Phosphorus forms from six surface soils plots and four dominant vegetations in the north of the Great Khingan mountains were detected to investigate the differences of phosphorus forms of soil between different vegetations. Phosphorus forms and macrofossil were also detected in a 77-cm peat core (1-cm intervals) in TQ. A fingerprinting historical vegetations were reconstructed by phosphors forms to reflect successions of vegetations during 2200 cal yr BP in TQ area. The results showed that the main phosphorus forms in peatland were NaOH-Po and conc. HCl-Po. The percentages of inorganic phosphorus forms of trees were generally higher than other vegetations. Moss was more conducive for accumulation of organic phosphorus. NaHCO3-Pi, NaOH-Pi, conc. HCl-Po and Pi were selected into linear discrimination analysis. The vegetations reconstructed by phosphorus forms were strongly correlated with the pollen records of moss, herbs and shrubs, as well as with macrofossils in herbs. The fingerprinting of vegetations by phosphorus has potential geochemical reference to reflect the successions of vegetation in peatland.


Asunto(s)
Fósforo , Suelo , Ecosistema , Árboles , Humedales
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