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1.
Molecules ; 29(9)2024 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-38731470

RESUMEN

This investigation is motivated by an interest in multiferroic BaFe12O19 (BFO), which combines advanced ferrimagnetic and ferroelectric properties at room temperature and exhibits interesting magnetoelectric phenomena. The ferroelectric charge storage properties of BFO are limited due to high coercivity, low dielectric constant, and high dielectric losses. We report the pseudocapacitive behavior of BFO, which allows superior charge storage compared to the ferroelectric charge storage mechanism. The BFO electrodes show a remarkably high capacitance of 1.34 F cm-2 in a neutral Na2SO4 electrolyte. The charging mechanism is discussed. The capacitive behavior is linked to the beneficial effect of high-energy ball milling (HEBM) and the use of an efficient dispersant, which facilitates charge transfer. Another approach is based on the use of conductive polypyrrole (PPy) for the fabrication of PPy-BFO composites. The choice of new polyaromatic dopants with a high charge-to-mass ratio plays a crucial role in achieving a high capacitance of 4.66 F cm-2 for pure PPy electrodes. The composite PPy-BFO (50/50) electrodes show a capacitance of 3.39 F cm-2, low impedance, reduced charge transfer resistance, enhanced capacitance retention at fast charging rates, and good cyclic stability due to the beneficial effect of advanced dopants, HEBM, and synergy of the contribution of PPy and BFO.

2.
Molecules ; 28(4)2023 Feb 06.
Artículo en Inglés | MEDLINE | ID: mdl-36838550

RESUMEN

The full potential of Fe3O4 for supercapacitor applications can be achieved by addressing challenges in colloidal fabrication of high active mass electrodes. Exceptional adsorption properties of catecholate-type 3,4-dihydroxybenzoic acid (DHBA) molecules are explored for surface modification of Fe3O4 nanoparticles to enhance their colloidal dispersion as verified by sedimentation test results and Fourier-transform infrared spectroscopy measurements. Electrodes prepared in the presence of DHBA show nearly double capacitance at slow charging rates as compared to the control samples without the dispersant or with benzoic acid as a non-catecholate dispersant. Such electrodes with active mass of 40 mg cm-2 show a capacitance of 4.59 F cm-2 from cyclic voltammetry data at a scan rate of 2 mV s-1 and 4.72 F cm-2 from galvanostatic charge-discharge data at a current density of 3 mA cm-2. Experimental results are corroborated by density functional theory (DFT) analysis of adsorption behaviour of DHBA and benzoic acid at the (001) surface of Fe3O4. The strongest adsorption energy (ca. -1.8 eV per molecule) is due to the catechol group of DHBA. DFT analysis provides understanding of the basic mechanism of DHBA adsorption on the surface of nanoparticles and opens the way for fabrication of electrodes with high capacitance.


Asunto(s)
Nanopartículas de Magnetita , Adsorción , Capacidad Eléctrica , Electrodos
3.
Molecules ; 27(5)2022 Mar 03.
Artículo en Inglés | MEDLINE | ID: mdl-35268760

RESUMEN

The high theoretical capacitance of MnO2 renders it a promising material for the cathodes of asymmetric supercapacitors. The good dispersion of MnO2 and conductive additives in a nanocomposite electrode is a key factor for efficient electrode performance. This article describes, for the first time, the application of rhamnolipids (RL) as efficient natural biosurfactants for the fabrication of nanocomposite MnO2-carbon nanotube electrodes for supercapacitors. RL act as co-dispersants for MnO2 and carbon nanotubes and facilitate their efficient mixing, which allows for advanced capacitive properties at an active mass of 40 mg cm-2 in Na2SO4 electrolytes. The highest capacitance obtained from the cyclic voltammetry data at a scan rate of 2 mV s-1 is 8.10 F cm-2 (202.6 F g-1). The highest capacitance obtained from the galvanostatic charge-discharge data at a current density of 3 mA cm-2 is 8.65 F cm-2 (216.16 F g-1). The obtained capacitances are higher than the capacitances of MnO2-based electrodes of the same active mass reported in the literature. The approach developed in this investigation is simple compared to other techniques used for the fabrication of electrodes with high active mass. It offers advantages of using a biocompatible RL biosurfactant.


Asunto(s)
Nanotubos de Carbono , Electrodos , Glucolípidos , Compuestos de Manganeso , Óxidos
4.
Molecules ; 27(16)2022 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-36014550

RESUMEN

This investigation is motivated by increasing interest in the development of magnetically ordered pseudocapacitors (MOPC), which exhibit interesting magnetocapacitive effects. Here, advanced pseudocapacitive properties of magnetic CuFe2O4 nanoparticles in negative potential range are reported, suggesting that CuFe2O4 is a promising MOPC and advanced negative electrode material for supercapacitors. A high capacitance of 2.76 F cm-2 is achieved at a low electrode resistance in a relatively large potential window of 0.8 V. The cyclic voltammograms and galvanostatic charge-discharge data show nearly ideal pseudocapacitive behavior. Good electrochemical performance is achieved at a high active mass loading due to the use of chelating molecules of ammonium salt of purpuric acid (ASPA) as a co-dispersant for CuFe2O4 nanoparticles and conductive multiwalled carbon nanotube (MCNT) additives. The adsorption of ASPA on different materials is linked to structural features of ASPA, which allows for different interaction and adsorption mechanisms. The combination of advanced magnetic and pseudocapacitive properties in a negative potential range in a single MOPC material provides a platform for various effects related to the influence of pseudocapacitive/magnetic properties on magnetic/pseudocapacitive behavior.

5.
Molecules ; 26(2)2021 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-33435538

RESUMEN

The ability to achieve high areal capacitance for oxide-based supercapacitor electrodes with high active mass loadings is critical for practical applications. This paper reports the feasibility of the fabrication of Mn3O4-multiwalled carbon nanotube (MWCNT) composites by the new salting-out method, which allows direct particle transfer from an aqueous synthesis medium to a 2-propanol suspension for the fabrication of advanced Mn3O4-MWCNT electrodes for supercapacitors. The electrodes show enhanced capacitive performance at high active mass loading due to reduced particle agglomeration and enhanced mixing of the Mn3O4 particles and conductive MWCNT additives. The strategy is based on the multifunctional properties of octanohydroxamic acid, which is used as a capping and dispersing agent for Mn3O4 synthesis and an extractor for particle transfer to the electrode processing medium. Electrochemical studies show that high areal capacitance is achieved at low electrode resistance. The electrodes with an active mass of 40.1 mg cm-2 show a capacitance of 4.3 F cm-2 at a scan rate of 2 mV s-1. Electron microscopy studies reveal changes in electrode microstructure during charge-discharge cycling, which can explain the increase in capacitance. The salting-out method is promising for the development of advanced nanocomposites for energy storage in supercapacitors.


Asunto(s)
Conductividad Eléctrica , Electrodos , Electrónica/instrumentación , Ácidos Hidroxámicos/química , Extracción Líquido-Líquido/métodos , Compuestos de Manganeso/química , Nanocompuestos/química , Óxidos/química , Electroquímica , Nanotubos de Carbono
6.
Molecules ; 26(6)2021 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-33808543

RESUMEN

Cathodes for supercapacitors with enhanced capacitive performance are prepared using MnO2 as a charge storage material and carbon nanotubes (CNT) as conductive additives. The enhanced capacitive properties are linked to the beneficial effects of catecholate molecules, such as chlorogenic acid and 3,4,5-trihydroxybenzamide, which are used as co-dispersants for MnO2 and CNT. The dispersant interactions with MnO2 and CNT are discussed in relation to the chemical structures of the dispersant molecules and their biomimetic adsorption mechanisms. The dispersant adsorption is a key factor for efficient co-dispersion in ethanol, which facilitated enhanced mixing of the nanostructured components and allowed for improved utilization of charge storage properties of the electrode materials with high active mass of 40 mg cm-2. Structural peculiarities of the dispersant molecules are discussed, which facilitate dispersion and charging. Capacitive properties are analyzed using cyclic voltammetry, chronopotentiometry and impedance spectroscopy. A capacitance of 6.5 F cm-2 is achieved at a low electrical resistance. The advanced capacitive properties of the electrodes are linked to the microstructures of the electrodes prepared in the presence of the dispersants.

7.
Molecules ; 26(7)2021 Mar 31.
Artículo en Inglés | MEDLINE | ID: mdl-33807421

RESUMEN

A dip-coating technique is designed for deposition of poly(methyl methacrylate) (PMMA) from water/2-propanol mixture, avoiding the use of traditional toxic solvents. Solutions of PMMA macromolecules with high molecular weight (MW) are obtained for a water/2-propanol ratio of 0.15-0.33 and the solubilization mechanism is discussed. The ability to use concentrated PMMA solutions and high MW of the polymer are the key factors for the successful dip coating deposition. The coating mass for 10 g L-1 polymer solutions shows a maximum at a water/2-propanol ratio of 0.25. The deposition yield increases with the polymer concentration increase and with an increasing number of the deposited layers. PMMA deposits protect stainless steel from aqueous corrosion. The coating technique allows for the fabrication of composite coatings, containing flame-retardant materials (FRMs), such as commercial halloysite, huntite, hydrotalcite, and synthesized Al(OH)3, in the PMMA matrix. The FRM content in the coatings is modified by variation of the FRM content in colloidal suspensions. A fundamentally new method is developed, which is based on the salting out aided dispersive extraction of Al(OH)3 from the aqueous synthesis medium to 2-propanol. It is based on the use of hexadecylphosphonic acid molecules as extractors. The method offers advantages of reduced agglomeration.

8.
Nanotechnology ; 28(7): 075603, 2017 Feb 17.
Artículo en Inglés | MEDLINE | ID: mdl-27976630

RESUMEN

A novel approach for the fabrication of nickel oxide nanotubes based on multiwalled carbon nanotubes as a sacrificial template is described. Electroless deposition is employed to deposit nickel onto carbon nanotubes. The subsequent annealing of the product in the presence of air oxidizes nickel to nickel oxide, and carbon is released as gaseous carbon dioxide, leaving behind nickel oxide nanotubes. Electron microscopy and elemental mapping confirm the formation of nickel oxide nanotubes. New chelating polyelectrolytes are used as dispersing agents to achieve high colloidal stability for both the nickel-coated carbon nanotubes and the nickel oxide nanotubes. A gravimetric specific capacitance of 245.3 F g-1 and  an areal capacitance of 3.28 F cm-2 at a scan rate of 2 mV s-1 is achieved, with an electrode fabricated using nickel oxide nanotubes as the active element with a mass loading of 24.1 mg cm-2.

9.
Nanomaterials (Basel) ; 13(10)2023 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-37242108

RESUMEN

This investigation is motivated by interest in nanostructured FeOOH anodes for aqueous asymmetric supercapacitors operating in Na2SO4 electrolyte. The research goal is the fabrication of anodes with high active mass loading of 40 mg cm-2, high capacitance and low resistance. The influence of high-energy ball milling (HEBM), capping agents and alkalizer on the nanostructure and capacitive properties is investigated. HEBM promotes the crystallization of FeOOH, which results in capacitance reduction. Capping agents from the catechol family, such as tetrahydroxy-1,4-benzoquinone (THB) and gallocyanine (GC), facilitate the fabrication of FeOOH nanoparticles, eliminate the formation of micron size particles and allow the fabrication of anodes with enhanced capacitance. The analysis of testing results provided insight into the influence of the chemical structure of the capping agents on nanoparticle synthesis and dispersion. The feasibility of a conceptually new strategy for the synthesis of FeOOH nanoparticles is demonstrated, which is based on the use of polyethylenimine as an organic alkalizer-dispersant. The capacitances of materials prepared using different nanotechnology strategies are compared. The highest capacitance of 6.54 F cm-2 is obtained using GC as a capping agent. The obtained electrodes are promising for applications as anodes for asymmetric supercapacitors.

10.
RSC Adv ; 13(38): 26995-27005, 2023 Sep 04.
Artículo en Inglés | MEDLINE | ID: mdl-37692350

RESUMEN

Iron oxides with advanced functional properties show great potential for applications in the fields of water splitting, drug delivery, sensors, batteries and supercapacitors. However, it is challenging to develop a simple and efficient strategy for fabricating patterned iron oxide based electrodes for supercapacitor applications. Herein, a facile, simple, scalable, binder-free, surfactant-free and conductive additive-free electric discharge rusting (EDR) technique is proposed to directly synthesize Fe1-xO oxide layer on a pure iron substrate. This new EDR strategy is successfully adopted to fabricate Fe-Fe1-xO integrative patterned electrodes and coplanar microsupercapacitors (CMSC) in one step. The CMSC devices with different geometries could be directly patterned by EDR, which is automatically controlled by a computer numerical control system. The fabricated Fe-Fe1-xO based 3D 2F-CMSC exhibits a maximum areal specific capacitance of 112.4 mF cm-2. Another important finding is the fabrication of 3D 2F-CMSC devices, which show good capacitive behavior at an ultra high scanning rate of 20 000 mV s-1. The results prove that EDR is a low-cost and versatile strategy for the scalable fabrication of high-performance patterned supercapacitor integrative electrodes and devices. Furthermore, it is a versatile technique which shows a great potential for development of next generation microelectronic devices, such as microbatteries and microsensors.

11.
Adv Sci (Weinh) ; 10(19): e2207223, 2023 07.
Artículo en Inglés | MEDLINE | ID: mdl-37088731

RESUMEN

There is a need for point-of-care bacterial sensing and identification technologies that are rapid and simple to operate. Technologies that do not rely on growth cultures, nucleic acid amplification, step-wise reagent addition, and complex sample processing are the key for meeting this need. Herein, multiple materials technologies are integrated for overcoming the obstacles in creating rapid and one-pot bacterial sensing platforms. Liquid-infused nanoelectrodes are developed for reducing nonspecific binding on the transducer surface; bacterium-specific RNA-cleaving DNAzymes are used for bacterial identification; and redox DNA barcodes embedded into DNAzymes are used for binding-induced electrochemical signal transduction. The resultant single-step and one-pot assay demonstrates a limit-of-detection of 102 CFU mL-1 , with high specificity in identifying Escherichia coli amongst other Gram positive and negative bacteria including Klebsiella pneumoniae, Staphylococcus aureus, and Bacillus subtilis. Additionally, this assay is evaluated for analyzing 31 clinically obtained urine samples, demonstrating a clinical sensitivity of 100% and specify of 100%. When challenging this assay with nine clinical blood cultures, E. coli-positive and E. coli-negative samples can be distinguished with a probability of p < 0.001.


Asunto(s)
ADN Catalítico , Escherichia coli , Escherichia coli/genética , Sensibilidad y Especificidad , Bacterias , ADN
12.
Nanomaterials (Basel) ; 12(5)2022 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-35269290

RESUMEN

This investigation addresses the challenges in the development of efficient nanostructured Mn3O4 cathodes for supercapacitors. A high areal capacitance and the ability to avoid a time-consuming activation procedure for electrodes with high active mass loading of 40 mg cm-2 are reported. This facilitates practical applications of Mn3O4 based electrodes. The highest capacitance of 6.11 F cm-2 (153 F g-1) is obtained from cyclic voltammetry at a scan rate of 2 mV s-1 and 6.07 F cm-2 (151.9 F g-1) from the chronopotentiometry at a current density of 3 mA cm-2 in a potential window of 0.9 V in a neutral Na2SO4 electrolyte. The new approach is based on the application of rhamnolipids (RL) as a capping agent for the synthesis of Mn3O4 particles and a co-dispersant for Mn3O4 and carbon nanotubes, which are used as conductive additives. The size and shape of the Mn3O4 particles are influenced by RL. The enhanced performance of the electrodes is linked to the chemical structure and properties of RL molecules, which exert influence on Mn3O4 particle size and shape during synthesis, reduce agglomeration, facilitate RL adsorption on Mn3O4 and carbon nanotubes, and influence their co-dispersion and mixing at the nanometric scale.

13.
Materials (Basel) ; 14(11)2021 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-34072315

RESUMEN

MXenes, such as Ti3C2Tx, are promising materials for electrodes of supercapacitors (SCs). Colloidal techniques have potential for the fabrication of advanced Ti3C2Tx composites with high areal capacitance (CS). This paper reports the fabrication of Ti3C2TX-Fe3O4-multiwalled carbon nanotube (CNT) electrodes, which show CS of 5.52 F cm-2 in the negative potential range in 0.5 M Na2SO4 electrolyte. Good capacitive performance is achieved at a mass loading of 35 mg cm-2 due to the use of Celestine blue (CB) as a co-dispersant for individual materials. The mechanisms of CB adsorption on Ti3C2TX, Fe3O4, and CNTs and their electrostatic co-dispersion are discussed. The comparison of the capacitive behavior of Ti3C2TX-Fe3O4-CNT electrodes with Ti3C2TX-CNT and Fe3O4-CNT electrodes for the same active mass, electrode thickness and CNT content reveals a synergistic effect of the individual capacitive materials, which is observed due to the use of CB. The high CS of Ti3C2TX-Fe3O4-CNT composites makes them promising materials for application in negative electrodes of asymmetric SC devices.

14.
ACS Appl Mater Interfaces ; 13(43): 50851-50861, 2021 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-34664926

RESUMEN

There is an increasing interest in using photoelectrochemistry for enhancing the signal-to-noise ratio and sensitivity of electrochemical biosensors. Nevertheless, it remains challenging to create photoelectrochemical biosensors founded on stable material systems that are also easily biofunctionalized for sensing applications. Herein, a photoelectrochemical immunosensor is reported, in which the concentration of the target protein directly correlates to a change in the measured photocurrent. The material system for the photoelectrode signal transducer involves using catecholate ligands to modify the properties of TiO2 nanostructures in a three-pronged approach of morphology tuning, photoabsorption enhancement, and facilitating bioconjugation. The catecholate-modified TiO2 photoelectrode is combined with a signal-off direct immunoassay to detect interleukin-6 (IL-6), a key biomarker for diagnosing and monitoring various diseases. Catecholate ligands are added during hydrothermal synthesis of TiO2 to enable the growth of three-dimensional nanostructures to form highly porous photoelectrodes that provide a three-dimensional scaffold for immobilizing capture antibodies. Surface modification by catecholate ligands greatly enhances photocurrent generation of the TiO2 photoelectrodes by improving photoabsorption in the visible range. Additionally, catecholate molecules facilitate bioconjugation and probe immobilization by forming a Schiff-base between their -COH group and the -NH2 group of the capture antibodies. The highest photocurrent achieved herein is 8.89 µA cm-2, which represents an enhancement by a factor of 87 from unmodified TiO2. The fabricated immunosensor shows a limit-of-detection of 3.6 pg mL-1 and a log-linear dynamic range of 2-2000 pg mL-1 for IL-6 in human blood plasma.


Asunto(s)
Técnicas Biosensibles , Catecoles/química , Técnicas Electroquímicas , Inmunoensayo , Interleucina-6/sangre , Titanio/química , Humanos , Estructura Molecular , Procesos Fotoquímicos
15.
Materials (Basel) ; 14(24)2021 Dec 20.
Artículo en Inglés | MEDLINE | ID: mdl-34947495

RESUMEN

Polyvinylidene fluoride (PVDF) is an advanced functional polymer which exhibits excellent chemical and thermal stability, and good mechanical, piezoelectric and ferroelectic properties. This work opens a new strategy for the fabrication of nanocomposites, combining the functional properties of PVDF and advanced inorganic nanomaterials. Electrophoretic deposition (EPD) has been developed for the fabrication of films containing PVDF and nanoparticles of TiO2, MnO2 and NiFe2O4. An important finding was the feasibility of EPD of electrically neutral PVDF and inorganic nanoparticles using caffeic acid (CA) and catechol violet (CV) as co-dispersants. The experiments revealed strong adsorption of CA and CV on PVDF and inorganic nanoparticles, which involved different mechanisms and facilitated particle dispersion, charging and deposition. The analysis of the deposition yield data, chemical structure of the dispersants and the microstructure and composition of the films provided an insight into the adsorption and dispersion mechanisms and the influence of deposition conditions on the deposition rate, film microstructure and composition. PVDF films provided the corrosion protection of stainless steel. Overcoming the limitations of other techniques, this investigation demonstrates a conceptually new approach for the fabrication of PVDF-NiFe2O4 films, which showed superparamagnetic properties. The approach developed in this investigation offers versatile strategies for the EPD of advanced organic-inorganic nanocomposites.

16.
Polymers (Basel) ; 13(18)2021 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-34577971

RESUMEN

Natural bone is a composite organic-inorganic material, containing hydroxyapatite (HAP) as an inorganic phase. In this review, applications of natural alginic acid (ALGH) polymer for the fabrication of composites containing HAP are described. ALGH is used as a biocompatible structure directing, capping and dispersing agent for the synthesis of HAP. Many advanced techniques for the fabrication of ALGH-HAP composites are attributed to the ability of ALGH to promote biomineralization. Gel-forming and film-forming properties of ALGH are key factors for the development of colloidal manufacturing techniques. Electrochemical fabrication techniques are based on strong ALGH adsorption on HAP, pH-dependent charge and solubility of ALGH. Functional properties of advanced composite ALGH-HAP films and coatings, scaffolds, biocements, gels and beads are described. The composites are loaded with other functional materials, such as antimicrobial agents, drugs, proteins and enzymes. Moreover, the composites provided a platform for their loading with cells for the fabrication of composites with enhanced properties for various biomedical applications. This review summarizes manufacturing strategies, mechanisms and outlines future trends in the development of functional biocomposites.

17.
Materials (Basel) ; 14(17)2021 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-34501070

RESUMEN

Applications of natural hyaluronic acid (HYH) for the fabrication of organic-inorganic composites for biomedical applications are described. Such composites combine unique functional properties of HYH with functional properties of hydroxyapatite, various bioceramics, bioglass, biocements, metal nanoparticles, and quantum dots. Functional properties of advanced composite gels, scaffold materials, cements, particles, films, and coatings are described. Benefiting from the synergy of properties of HYH and inorganic components, advanced composites provide a platform for the development of new drug delivery materials. Many advanced properties of composites are attributed to the ability of HYH to promote biomineralization. Properties of HYH are a key factor for the development of colloidal and electrochemical methods for the fabrication of films and protective coatings for surface modification of biomedical implants and the development of advanced biosensors. Overcoming limitations of traditional materials, HYH is used as a biocompatible capping, dispersing, and structure-directing agent for the synthesis of functional inorganic materials and composites. Gel-forming properties of HYH enable a facile and straightforward approach to the fabrication of antimicrobial materials in different forms. Of particular interest are applications of HYH for the fabrication of biosensors. This review summarizes manufacturing strategies and mechanisms and outlines future trends in the development of functional biocomposites.

18.
Adv Colloid Interface Sci ; 284: 102272, 2020 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-32987293

RESUMEN

This review is focused on new electrophoretic deposition (EPD) mechanisms for deposition biomacromolecules, such as biopolymers, proteins and enzymes. Among the rich literature sources of EPD of biopolymers, proteins and enzymes for biomedical applications we selected papers describing new fundamental deposition mechanisms. Such deposition mechanisms are of critical importance for further development of EPD method and its emerging biomedical applications. Our goal is to emphasize innovative ideas which have enriched colloid and interface science of EPD during recent years. We describe various mechanisms of cathodic and anodic EPD of charged biopolymers. Special attention is focused on in-situ chemical modification of biopolymers and crosslinking techniques. Recent innovations in the development of natural and biocompatible charged surfactants and film forming agents are outlined. Among the important advances in this area are the applications of bile acids and salts for EPD of neutral polymers. Such innovations allowed for the successful EPD of various electrically neutral functional polymers for biomedical applications. Particularly important are biosurfactant-polymer interactions, which facilitate dissolution, dispersion, charging, electrophoretic transport and deposit formation. Recent advances in EPD mechanisms addressed the problem of EPD of proteins and enzymes related to their charge reversal at the electrode surface. Conceptually new methods are described, which are based on the use of biopolymer complexes with metal ions, proteins, enzymes and other biomolecules. This review describes new developments in co-deposition of biomacromolecules and future trends in the development of new EPD mechanisms and strategies for biomedical applications.


Asunto(s)
Materiales Biocompatibles/química , Electroforesis/métodos , Polímeros/química , Proteínas/química , Animales , Humanos
19.
ACS Appl Mater Interfaces ; 12(33): 36895-36905, 2020 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-32814377

RESUMEN

As dynamic biorecognition agents such as functional nucleic acids become widely used in biosensing, there is a need for ultrasensitive signal transduction strategies, beyond fluorescence, that are robust and stable for operation in heterogeneous biological samples. Photoelectrochemical readout offers a pathway toward this goal as it offers the simplicity and scalability of electrochemical readout, in addition to compatibility with a broad range of nanomaterials used as labels for signal transduction. Here, a differential photoelectrochemical biosensing approach is reported, in which DNA nanospacers are used to program the response of two sensing channels. The differences in the motional dynamics of DNA probes immobilized on different channels are used to control the interaction between Au and TiO2 nanoparticles positioned at the two ends of the DNA nanospacer to achieve differential signal generation. Depending on the composition of the DNA constructs (fraction of the DNA sequence i.e., double-stranded), the channels can be programmed to produce a signal-on or a signal-off response. Incident photon-to-current conversion efficiency, UV-vis spectroscopy, and flat-band potential measurement indicate that direct transfer of electrons between metallic and semiconductive nanoparticles is responsible for the signal-on response, and incident light absorption and steric hindrance are responsible for the signal-off response. The differential photoelectrochemical signal readout developed here increases the device sensitivity by up to three times compared to a single channel design and demonstrates a limit of detection of 800 aM.


Asunto(s)
Compuestos de Boro/química , ADN/análisis , Oro/química , Nanopartículas/química , Semiconductores , Titanio/química , Secuencia de Bases , Técnicas Biosensibles , Técnicas Electroquímicas , Electrodos , Transporte de Electrón , Límite de Detección , Procesos Fotoquímicos , Relación Señal-Ruido , Propiedades de Superficie
20.
Talanta ; 199: 472-477, 2019 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-30952286

RESUMEN

Columns packed with ultrafine particles (e.g. sub-2 µm porous particles) are suitable for high-resolution, high-speed analytical separation of proteins. However, they require very expensive chromatography systems to provide the ultra-high pressure required for carrying out separations using such columns. Also, frictional heating at high pressure could result in peak broadening and on-column protein degradation. In this paper, we discuss the use of nanoparticles, packed in a box-shaped or cuboid packed-bed device having 50 mm length, 5 mm width, and 3 mm bed-height for fast, high-resolution separation of proteins at low pressure. The low bed height allows the separation to be carried out at low pressure while the cuboid device reduces dispersion effects and thereby keeps the resolution high. Two different types of hydroxyapatite nanoparticles, i.e., needle-shaped (about 20 nm × 150 nm) and spherical (<200 nm) ones, were examined. The experimental results showed that while the needle-shaped nanoparticles were suitable for the separation of small proteins such as lysozyme, the spherical nanoparticles were better suited for separation of larger proteins such as bovine serum albumin and monoclonal antibody. The separation of the two proteins could be carried out in less than 2 min at a pressure lower than 0.8 MPa, using inexpensive chromatography devices a7nd systems, and without high pressure related problems such as frictional heating and on-column protein denaturation.


Asunto(s)
Anticuerpos Monoclonales/aislamiento & purificación , Durapatita/química , Muramidasa/aislamiento & purificación , Nanopartículas/química , Albúmina Sérica Bovina/aislamiento & purificación , Animales , Anticuerpos Monoclonales/química , Bovinos , Muramidasa/química , Muramidasa/metabolismo , Tamaño de la Partícula , Presión , Albúmina Sérica Bovina/química , Propiedades de Superficie , Factores de Tiempo
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