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1.
J Colloid Interface Sci ; 665: 144-151, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38520931

RESUMEN

Electrochemiluminescence (ECL) biosensors provide a convenient and high sensitivity method for early disease diagnosis. However, creating luminophore arrays relying on powerful ECL signals remains a daunting task. Porphyrin-centered metal organic frameworks (MOFs) exhibit remarkable potential in ECL sensing applications. In this paper, based on a simple one-pot synthesis method, PCN-222@Ag NPs doped with CeO2 was synthesized to enhance the ECL performance. Due to the strong catalytic ability of CeO2, the ECL signal strength of the new material PCN-222@CeO2@Ag NPs is much higher than that of the PCN-222@Ag NPs and PCN-222. The luminous properties of PCN-222@CeO2@Ag NPs become more intense and stable due to the excellent electronic conductivity of Ag NPs. Based on the fact that CuS@PDA composite can quench the ECL signal of PCN-222@CeO2@Ag NPs, we constructed a novel sandwich ECL immune sensor for the detection of phosphorylated Tau 181 (p-Tau-181) protein. The ECL sensor has a great linear relationship with p-Tau-181 protein concentration, ranging from 1 pg/mL to 100 ng/mL. The detection limit is as low as 0.147 pg/mL. This work provides new ideas for developing sensitive ECL sensors for the p-Tau-181 protein, the marker of Alzheimer's disease.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Mediciones Luminiscentes/métodos , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Límite de Detección
2.
Chem Commun (Camb) ; 59(100): 14847-14850, 2023 Dec 14.
Artículo en Inglés | MEDLINE | ID: mdl-38015452

RESUMEN

An ultrasensitive photoelectrochemical (PEC) aptasensor was originally designed by using ZnIn2S4/ReS2 as a photoactive material and AgInS2 as a signal amplifier. The signal amplifier AgInS2 was incubated on the terminal of H-DNA (immobilized on the ZnIn2S4/ReS2/FTO surface), leading to an enhanced photocurrent response. Then, due to the introduction of DNA2, the formation of a double-stranded structure caused AgInS2 to keep away from the electrode surface, and the photocurrent was reduced. In the presence of kanamycin, DNA2 was released from the system due to the competition relationship, and a restored photocurrent response was obtained. The combination of ZnIn2S4/ReS2 and AgInS2 accelerated the electron transfer and enhanced the separation efficiency of photogenerated electron-hole pairs, resulting in an improved performance of the PEC aptasensor, which was capable of accurate and sensitive detection of kanamycin in actual samples.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Kanamicina , Técnicas Electroquímicas/métodos , Técnicas Biosensibles/métodos , Transporte de Electrón , Electrodos , Límite de Detección , Aptámeros de Nucleótidos/química
3.
Analyst ; 148(4): 772-779, 2023 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-36661384

RESUMEN

In this study, for the first time, a silver-based metal-organic framework (Ag-MOF) was synthesized and used as the electrochemiluminescence (ECL) emitter for building an ECL sensor. After modification with chitosan (CS) and gold nanoparticles (Au NPs), the ECL stability of Ag-MOF was improved. To detect mercury ions, a biosensor was constructed using the mercury ion aptamer and steric effect of streptavidin. First, the capture strand (cDNA) with terminal-modified sulfhydryl group was attached to the electrode surface by the Au-S bond. Then, the mercury-ion aptamer (Apt-Hg) modified with biotin was anchored to the electrode by complementary pairing with cDNA. Streptavidin (SA) could be fixed on the electrode by linking with biotin, thereby reducing the ECL signal. However, in the presence of mercury ions, the aptamer was removed and streptavidin could not be immobilized on the electrode. Hence, the ECL signal of the sensor increased with the concentration of mercury ions, which was linear in the range from 1 µM to 300 fM. The detection limit could reach 66 fM (S/N = 3). The sensor provided a new method for the detection of mercury ions.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Mercurio , Nanopartículas del Metal , Biotina/química , Estreptavidina/química , Plata , ADN Complementario , Oro/química , Técnicas Electroquímicas/métodos , Nanopartículas del Metal/química , Mediciones Luminiscentes/métodos , Aptámeros de Nucleótidos/química , Iones , Técnicas Biosensibles/métodos , Límite de Detección
4.
Talanta ; 253: 123601, 2023 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-36126520

RESUMEN

A novel photoelectrochemical (PEC) biosensor based on b-TiO2/CdS:Eu/Ti3C2 heterojunction was developed for ultrasensitive determination of miRNA-21. In this device, the b-TiO2/CdS:Eu/Ti3C2 heterojunction with excellent energy level arrangement effectively facilitated photoelectric conversion efficiency and accelerated the separation of the photogenerated electron hole pairs, which because that the structure of heterojunction overcomes the drawbacks of single material, such as narrow light absorption range, wide band gap, short carrier lifetime, etc., improves light utilization, extends the lifetime of photogenerated electron hole pairs, and promotes electron transfer. Herein, hairpin DNA1 (H1) decorated on the b-TiO2/CdS:Eu/Ti3C2 electrode surface by Cd-S bonds, after H2/miRNA-21 heterduplex was introduced, the strand-displacement reaction (SDR) was triggered between H1 and H2/miRNA-21, accordingly, miRNA-21 was discharged from the H2/miRNA-21 heterduplex, forming the H1/H2 duplex, and the reuse of miRNA-21 was realized. As a signal amplification factor, the signal amplification factor H3-CdSe was hybridized with H1/H2 duplex, which greatly enhanced the sensitivity of the PEC biosensor. Under optimal conditions, the designed PEC biosensor displayed outstanding sensitivity, selectivity and stability with a wide liner range from 1.0 µM to 10.0 fM and a low detection limit of 3.3 fM. The preparation of the optoelectronic material affords a new direction for the progress of heterojunction photovoltaic materials and the construction of the proposed biosensor also provides a new thought for the PEC detection of human miRNA-21 with superior performance. Simultaneously, the established biosensor exhibiting tremendous possibility for detecting other biomarkers and biomolecules in clinical diagnosis fields.


Asunto(s)
Técnicas Biosensibles , MicroARNs , Titanio , Humanos , Electrodos , Fotoquímica
5.
Mikrochim Acta ; 189(7): 264, 2022 07 01.
Artículo en Inglés | MEDLINE | ID: mdl-35776207

RESUMEN

The electrochemiluminescence and resonance energy transfer (ECL-RET) method was adopted to detect miRNAs, in which the two-dimensional Ti3C2 Mxenes with high surface area modified with CdS:W nanocrystals (CdS:W NCs) were used as ECL signal emitter. Mxenes with a specific surface area of 5.2755 m2/g carried more emitters and promote ECL intensity. As an energy acceptor, BiOCl nanosheets (BiOCl NSs) have a wide UV-Vis absorption peak in the range 250 nm-700 nm, including the emission band of CdS:W NCs with 520 nm emission wavelength. Hence, BiOCl NSs are covalently bound to hairpin DNA 2 by amide bond to quench the ECL signal of CdS:W NCs. In the presence of miRNA-141, the hairpin DNA 1 modified on the GCE was unfold and then paired with hairpin DNA 2 to release miRNA-141 and quench the signal of the ECL biosensor. Then, the concentration signal of miRNA-141 was amplified by catalytic hairpin assembly. The novel specific biosensor demonstrated a satisfactory linear relationship with miRNA-141 in the range 0.6 pM to 4000 pM; the detection limit was as low as 0.26 pM (3 s/m) under the potential of 0 ~ -1.3 V and showed outstanding RSD of 1.19%. The findings of the present work with high accuracy and sensitivity will be of positive significance for the clinical diagnosis of miRNA in the future work. The construction process of the biosensor and electrochemiluminescence mechanism.


Asunto(s)
Técnicas Electroquímicas , MicroARNs , ADN/química , ADN/genética , Técnicas Electroquímicas/métodos , Transferencia de Energía , Mediciones Luminiscentes/métodos , MicroARNs/genética
6.
Artículo en Inglés | MEDLINE | ID: mdl-35537183

RESUMEN

In this work, a two-dimensional (2D) MOF sheet with electrochemiluminescence (ECL) activity is prepared with Ti3C2Tx MXene as the metal precursor and the meso-tetra(4-carboxyl-phenyl) porphyrin (H2TCPP) as the organic ligand. The atomically thin 2D Ti3C2Tx MXene is utilized as the metal precursor and soft template to produce the MOF with a 2D nanosheet morphology (Ti3C2Tx-PMOF). Ti3C2Tx MXene is a kind of strong electron acceptor, which can deprotonate H2TCPP due to the high electronegativity and low work function of its terminal atoms. The deprotonated H2TCPP continues to bind with Ti atoms to form the 2D MOF sheet. The ECL activity is inherited from H2TCPP and stabilized by introducing Ag NPs. Then, we construct an ECL biosensor based on the Ag NPs/Ti3C2Tx-PMOF to detect the oral cancer overexpressed 1 (ORAOV 1). A bipedal three-dimensional DNA walker strategy is adopted to further improve the biosensor sensitivity. As expected, the biosensor exhibits sterling sensitivity and selectivity. The ECL biosensor responds linearly to ORAOV 1 concentrations in the range of 10 fM-1 nM, and the detection limit is as low as 3.3 fM (S/N = 3). It means that Ag NPs/Ti3C2Tx-PMOF is a potential material to design and construct the high-performance ECL biosensors.

7.
Anal Chem ; 94(9): 4095-4102, 2022 03 08.
Artículo en Inglés | MEDLINE | ID: mdl-35196001

RESUMEN

The recent surge of interest in metal-organic gels (MOGs) has emerged for their soft porous structure, large surface area, and abundant active metal sites, making them a promising candidate for building catalyst matrices. In this work, facilely synthesized Fe(III)-organic gel was directly used as a robust electrode matrix. Detailed studies illustrated that their Fe(III) centers can speed up the electro-oxidation/reduction of the H2O2 coreactant to produce reactive oxygen species for enhancing a potential-resolved dual electrochemiluminescence (ECL) emission. Among them, the anodic signal of luminol varied with the cell concentration based on the impedance ECL mechanism, while the cathodic signal of CdS quantum dots traced the VEGF165 subtype at cell surface by specific aptamer recognition. Based on this, a ratiometric strategy was proposed for accurate cytosensing by eliminating environmental interference. Moreover, by cooperating these two signals, a novel strategy was developed for direct evaluation of the VEGF165 subtype, further realizing rapid drug screening and subtype assessment on different cell lines. This work not only opens up the promising application of MOGs as an effective catalyst matrix but also develops reliable cell assays and protein subtype identification for clinical diagnosis and research.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Catálisis , Técnicas Electroquímicas , Geles , Peróxido de Hidrógeno , Hierro , Mediciones Luminiscentes , Luminol , Nanopartículas del Metal/química , Factor A de Crecimiento Endotelial Vascular
8.
Talanta ; 233: 122546, 2021 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-34215049

RESUMEN

In this paper, hydrothermal method was used for the synthesis of SnO2 quantum dots (QDs). The prepared SnO2 QDs have a uniform particle size distribution and good electrochemiluminescence (ECL) property. Then the prepared SnO2 QDs was combined with graphene-like carbon nitride (g-C3N4) through chitosan to form SnO2/chitosan/g-C3N4 nanocomposite and used for detecting the lincomycin. The characteristics of SnO2/chitosan/g-C3N4 nanocomposite were presented by transmission electron microscopy (TEM), X-ray diffraction (XRD) and energy dispersive spectroscopy (EDS), and the analytical results proving that the nanocomposite was prepared successfully. In this strategy, the SnO2/chitosan/g-C3N4 nanocomposite was acted as the substrate of aptasensor. Then, SH-DNA (aptamer DNA) was assembled on the surface of electrode, after 6-mercaptohexanol (MCH) blocked the unbound sites of the electrode surface, ferrocene-DNA (Fc-DNA) was incubated on the electrode surface through base complementation with aptamer DNA. In the absence of lincomycin, due to the low conductivity of Fc-DNA and the photo-excited energy electron transfer, the ECL signal was quenched. In the presence of lincomycin, the aptamer DNA was specific binding with lincomycin, and ferrocene-DNA (Fc-DNA) was detached from the surface of aptasensor electrode, generating an obviously enhancement of ECL signal. To ensure the accuracy of the data, each electrode runs continuously for 3600 s. Under optimal experimental conditions, the detection range of the aptasensor was 0.10 ng mL-1 - 0.10 mg mL-1, and the detection limit was 0.028 ng mL-1. In addition, the aptasensor has good stability and reproducibility, and also provided a hopeful device for all kinds of other protein target.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Quitosano , Nanocompuestos , Técnicas Electroquímicas , Lincomicina , Mediciones Luminiscentes , Reproducibilidad de los Resultados
9.
Analyst ; 146(1): 146-155, 2021 Jan 04.
Artículo en Inglés | MEDLINE | ID: mdl-33107868

RESUMEN

Herein, a label-free photoelectrochemical immunosensor based on a g-C3N4/CdSe nanocomposite was established and applied to detect carcinoembryonic antigen (CEA). The prepared nanocomposite materials were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), ultraviolet-visible absorption spectroscopy (UV-vis), X-ray photoelectron spectroscopy (XPS), fourier transform infrared spectrometer (FT-IR) and photoluminescence spectroscopy (PL). The results indicate that g-C3N4/CdSe nanocomposite materials were successfully synthesized. In a typical assembly process, the immunosensor was constructed by modifying a fluorine-doped tin oxide (FTO) electrode with poly dimethyl diallyl ammonium chloride (PDDA), the g-C3N4/CdSe nanocomposite, the anti-carcinoembryonic antigen antibody (Ab) and the blocking agent bovine serum albumin (BSA) successively. In the presence of CEA, the photocurrent signal of the prepared immunosensor decreased significantly. Accordingly, under the optimal conditions, a label-free photoelectrochemical immunosensor was established, and it exhibited excellent selectivity and repeatability for CEA detection. The detection limit was 0.21 ng mL-1, and the range was 10 ng mL-1-100 µg mL-1. Simultaneously, the immunosensor also provides a likely sensing device for detecting other protein targets, which is of great significance for early clinical diagnosis.


Asunto(s)
Técnicas Biosensibles , Compuestos de Cadmio , Nanocompuestos , Compuestos de Selenio , Antígeno Carcinoembrionario , Técnicas Electroquímicas , Inmunoensayo , Espectroscopía Infrarroja por Transformada de Fourier
10.
Biosens Bioelectron ; 165: 112416, 2020 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-32729534

RESUMEN

Herein, an ultra-sensitive photoelectrochemical biosensor based on Ti3C2:CdS nanocomposite was established for the selective detection of microRNA159c. Ti3C2:CdS nanocomposites were used as optoelectronic materials because Ti3C2:CdS interaction effectively separates photogenerated electrons and holes, and significantly improves the high photoelectric conversion efficiency. Firstly, Ti3C2:CdS nanocomposite was deposited on the surface of the fluorine-doped tin oxide (FTO) electrode. After the chitosan (CS) was dropped, the SH-miRNA were bonded on the electrode surface via the S-Cd bond. Then 6-mercaptohexanol (MCH) blocked the unbound site, the DNA strand was introduced to hybridize with the target SH-miRNA. At this time, the obtained photocurrent gradually decreases. Subsequently, the photosensitizer TMPyP as signal amplification was modified, the photocurrent increased significantly. The target SH-miRNA was detected based upon the photocurrent change originated from quantities change of TMPyP. Working under the best experimental conditions, the sensing platform had good stability, selectivity, and high sensitivity. The detection range for miRNA159c was 1.0 × 10-6-1.0 × 10-13 mol·L-l, and the detection limit was approximately 33 fmol·L-l. The detection of miRNA159c in human serum provided a huge opportunity to explore the relationship between the abundance of this miRNA and the incidence of breast cancer (BC), and to further achieve effective detection of BC.


Asunto(s)
Técnicas Biosensibles , Neoplasias de la Mama , Compuestos de Cadmio , Nanocompuestos , Neoplasias de la Mama/diagnóstico , Neoplasias de la Mama/genética , Técnicas Electroquímicas , Humanos , Límite de Detección , Titanio
11.
Mikrochim Acta ; 187(8): 455, 2020 07 18.
Artículo en Inglés | MEDLINE | ID: mdl-32683571

RESUMEN

An ultrasensitive electrochemiluminescence biosensor was established based on the Zn-MOF/GO nanocomposite. Ag(I)-embedded DNA complexes were used as a signal amplification reagent. In this work, 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (TCPP) and Zn2+ were integrated into a porphyrin paddlewheel framework (Zn-MOF) by a hydrothermal method. The synthesized Zn-MOF material has electrochemiluminescence property, and the luminescence intensity is improved after being composited with graphene oxide (GO). Based on the composite material, we constructed an ultrasensitive ECL biosensor for the p53 antibody detection. The composite material acted as an admirable substrate and then loaded plenty of p53 antigens to recognize the target (p53 antibody) accurately. Because of the bridging effect of streptavidin and biotin-conjugated goat anti-rabbit IgG (bio-ab2), the rich-C DNA with positive correlation with the target was modified on the electrode and then captured the co-reactant accelerator Ag+ to amplify the signal. Therefore, the ECL biosensor response increases with increasing p53 antibody concentration. In the range 0.1 fg/mL-0.01 ng/mL, the response signal of the biosensor has a good linear relationship with the p53 antibody concentration. The detection limit is 0.03 fg/mL (S/N = 3). Impressively, the biosensor not only featured high sensitivity, good stability, and excellent specificity for the detection of p53 antibody, but also provides a new way for early detection of cancer. Graphical abstract Schematic representation of the electrochemiluminescence sensor based on a Zn-MOF/GO nanocomposite, which can be applied to the determination of p53 antibody.


Asunto(s)
Anticuerpos/análisis , Técnicas Biosensibles/métodos , ADN/química , Estructuras Metalorgánicas/química , Nanocompuestos/química , Plata/química , Anticuerpos/inmunología , Técnicas Electroquímicas/métodos , Grafito/química , Proteínas Inmovilizadas/inmunología , Límite de Detección , Mediciones Luminiscentes/métodos , Metaloporfirinas/química , Proteína p53 Supresora de Tumor/inmunología , Zinc/química
12.
Anal Bioanal Chem ; 412(13): 3073-3081, 2020 May.
Artículo en Inglés | MEDLINE | ID: mdl-32162087

RESUMEN

In this work, an electrochemiluminescence (ECL) biosensor was fabricated for the selective detection of vascular endothelial growth factor (VEGF165). g-C3N4/PDDA/CdSe nanocomposites were used as the ECL substrate. Then, DNA labeled at the 5' end with amino groups (DNA1) was immobilized on the surface of g-C3N4/PDDA/CdSe nanocomposite-modified glassy carbon electrode (GCE) by amido linkage. AuNP-labeled target DNA (Au-DNA2) could hybridize with DNA1 to form a double strand. The ECL of the g-C3N4/PDDA/CdSe nanocomposite was efficiently quenched due to the resonance energy transfer between CdSe QDs and Au NPs. After VEGF165 was recognized and bound by Au-DNA2, the double helix was disrupted, and the energy transfer was broken. In this case, Au-DNA2 was released from the electrode surface, and the ECL intensity recovered to a higher level. Under optimal conditions, this ECL biosensor possesses excellent selectivity, accuracy, and stability for VEGF165 detection in a linear range of 2 pg mL-1 to 2 ng mL-1 with a detection limit of 0.68 pg mL-1. In addition, this assay has been successfully applied to the determination of VEGF165 in serum samples. Graphical abstract Schematic representation of the electrochemiluminescence sensor based on a g-C3N4/PDDA/CdSe nanocomposite, which can be determined in the concentration of vascular endothelial growth factor in serum.


Asunto(s)
Compuestos de Cadmio/química , Técnicas Electroquímicas/métodos , Luminiscencia , Nitrilos/química , Polietilenos/química , Compuestos de Amonio Cuaternario/química , Compuestos de Selenio/química , Factor A de Crecimiento Endotelial Vascular/análisis , Técnicas Biosensibles , Límite de Detección , Microscopía Electrónica de Transmisión , Espectrofotometría Ultravioleta
13.
J Mater Chem B ; 8(12): 2471-2475, 2020 03 25.
Artículo en Inglés | MEDLINE | ID: mdl-32108205

RESUMEN

A novel electrochemiluminescence (ECL) biosensor was developed in this study, which was based on the Ag-NP modified tetrahedral DNA nanostructure. First, a stable and rigid three-dimensional tetrahedral DNA nanostructure (TDN) was modified on a gold electrode, which was used as a capture element. The TDN improves the accuracy and sensitivity of this biosensor. In addition, silver nanoparticles (Ag NPs) with excellent electrical conductivity were introduced on the edges of TDNs to enhance the ECL intensity of the metal-organic framework (MOF) nanomaterial. Apart from imparting conductivity, the Ag NPs can also act as co-reactant accelerators to enhance the ECL intensity. A Eu3+ doped Zr-MOF material (Eu@MOF) was proposed and used as an ECL material for the first time. Terminal phosphate-modified MUC1 aptamer DNA bonded with the exposed Zr nodes on the surface of MOFs through Zr-O-P bonds to construct the DNA-Eu@MOF signal element. Based on the Ag NP-modified TDN capture element and the DNA-Eu@MOF signal element, a hypersensitive biosensor was established. Under the optimal conditions, this biosensor exhibited a wide detection range from 1.135 fg mL-1 to 0.1135 ng mL-1 and a low detection limit of 0.37 fg mL-1 (S/N = 3) toward the target MUC1. The biosensor also showed excellent stability and high selectivity for MUC1 detection.


Asunto(s)
Técnicas Biosensibles , Técnicas Electroquímicas , Mediciones Luminiscentes , Nanopartículas del Metal/química , Mucina-1/análisis , Plata/química , Humanos , Tamaño de la Partícula , Propiedades de Superficie
14.
Mikrochim Acta ; 187(3): 155, 2020 02 05.
Artículo en Inglés | MEDLINE | ID: mdl-32025820

RESUMEN

An electrochemiluminescence (ECL) biosensor was fabricated for the evaluation of prostate specific antigen (PSA). The sensor was developed by successively modifying glassy carbon electrode (GCE) electrodes with CdS/Chito/g-C3N4 nanocomposites and DNA1 was labeled at the 5' end with thiol. The aptamer DNA was labeled at the 3' end with a quencher ferrocene (Fc) was ligated to DNA1 by the principle of complementary base pairing. In the absence of PSA, the ECL intensity signal is effectively quenches through the energy transfer and photoexcitation electron transfer between CdS/Chito/g-C3N4 emitter and quencher Fc. After incubation with target PSA, the aptamer DNA interacts with PSA and then moved away from the electrode surface together, which will recover the ECL intensity. Under the optimal conditions, the ECL intensity increases linearly with the logarithm of PSA concentration in the range of 1 pg·mL-1 to 100 ng·mL-1, and the detection limit is 0.14 pg·mL-1 (S/N = 3). The biosensor has been successfully applied to the determination of PSA in serum sample. Graphical abstractSchematic representation of the electrochemiluminescence sensor based on a CdS/chitosan/g-C3N4 nanocomposite, which can be applied to the determination of prostate specific antigen in serum.


Asunto(s)
Quitosano/química , Electroquímica/métodos , Inmunoensayo/métodos , Mediciones Luminiscentes/métodos , Nanocompuestos/química , Antígeno Prostático Específico/sangre , Humanos
15.
Beilstein J Nanotechnol ; 10: 912-921, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31165018

RESUMEN

Photocatalytic hydrogen generation from water splitting has become a favorable route for the utilization of solar energy. An effective strategy, the combination of C-doping with nanocomposite semiconductors, is presented in this work. C-doped g-C3N4 (CCN) was prepared by supramolecular self-assembly and subsequently a number of CdIn2S4/CCN composite photocatalysts were designed and fabricated though in situ decoration of CdIn2S4 crystals on the surface of CCN nanosheets via a hydrothermal method. This unique architecture was able to efficiently promote the transfer and separation of photon-generated charges, enhance light absorption, and significantly increase photocatalytic H2 production. Detailed characterization was performed to analyze the crystal structure, morphology, elementary composition, optical properties and catalytic mechanism. The CdIn2S4/CCN nanocomposites with optimal CdIn2S4 content exhibited a maximum H2 production rate of 2985 µmol h-1 g-1, almost 15 times more than that obtained using pure g-C3N4 (205 µmol h-1 g-1). In addition, the hybrid photocatalysts display good recycling stability under visible-light irradiation. This research may provide promising information for the preparation of more efficient multifunctional hybrid photocatalysts with excellent stability in fine chemical engineering.

16.
Anal Chim Acta ; 1048: 42-49, 2019 Feb 07.
Artículo en Inglés | MEDLINE | ID: mdl-30598156

RESUMEN

A novel enhanced photoelectrochemical (PEC) DNA biosensor, based on a compact heterojunction g-C3N4/MoS2 and co-sensitization effect with CdSe quantum dots (QDs), was first proposed for simple and accurate analysis of a short ssDNA. In this work, the g-C3N4/MoS2 was successfully synthesized and used as the electrode matrix material to construct PEC biosensor. 2D/2D heterojunction was formed between g-C3N4 and MoS2, which could promote the separation of photogenerated electron-hole pairs resulting in an enhanced photocurrent. In the presence of target DNA, CdSe QDs labeled reporter DNA was complementary pairing with target DNA which was specific recognized by capture DNA loading on self-assembled CdS QDs film, leading to close contact between CdSe QDs and g-C3N4/MoS2 modified electrode surface, thereby resulting in the enhanced photocurrent intensity due to the co-sensitization effect. Under the optimal operating conditions, the photoelectrochemical biosensor demonstrated favorable accuracy and could respond to 0.32 pM (S/N = 3) with a linear concentration range from 1.0 pM to 2.0 µM. Moreover, the proposed PEC DNA biosensor exhibits high sensitivity, excellent specificity, acceptable reproducibility and accuracy, showing a promising potential in DNA bioanalysis and other relative fields.


Asunto(s)
Técnicas Biosensibles/métodos , ADN de Cadena Simple/análisis , Técnicas Electroquímicas/métodos , Fotoquímica/métodos , Puntos Cuánticos/química , Compuestos de Cadmio/química , Compuestos de Cadmio/efectos de la radiación , ADN de Cadena Simple/genética , Disulfuros/química , Electrodos , Luz , Límite de Detección , Molibdeno/química , Nitrilos/química , Hibridación de Ácido Nucleico , Puntos Cuánticos/efectos de la radiación , Compuestos de Selenio/química , Compuestos de Selenio/efectos de la radiación
17.
Talanta ; 194: 745-751, 2019 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-30609601

RESUMEN

A highly selective DNA-based electrochemiluminescence (ECL) based biosensor is described for the detection of human IgG. It is exploiting the effect of steric hindrance that affects the strength of the ECL signal in the presence of IgG. Digoxin-linked signaling DNA was specifically bound to IgG, and this causes steric hindrance which limits the ability of DNA to hybridize with capturing DNA attached to a gold electrode. Europium (II) doped CdSe quantum dots were covalently linked to the DNA in order to generate the ECL signal. Using this steric hindrance hybridization method, the ECL signal of the biosensor were proportional to the concentration of IgG with a wide linear range and a 14 pM detection limit. Conceivably, the method can be expanded to the detection of a wide range of proteins for which homologous recognition elements are available.


Asunto(s)
Técnicas Biosensibles/métodos , ADN/química , Inmunoglobulina G/análisis , Límite de Detección , Mediciones Luminiscentes , Compuestos de Cadmio/química , Electroquímica , Electrodos , Europio/química , Oro/química , Humanos , Inmunoglobulina G/química , Modelos Moleculares , Conformación de Ácido Nucleico , Hibridación de Ácido Nucleico , Puntos Cuánticos/química , Compuestos de Selenio/química
18.
Anal Chem ; 91(2): 1563-1570, 2019 01 15.
Artículo en Inglés | MEDLINE | ID: mdl-30562453

RESUMEN

Herein, an efficient photoelectrochemical (PEC) platform was constructed by a cosensitization strategy with a cascade energy level arrangement for the ultrasensitive evaluation of T4 polynucleotide kinase (T4 PNK). Based on CdSe quantum dots (QDs) with an extremely narrow bandgap, this cosensitization strategy offered a highly efficient sensitizer with a matching band-edge level of a ternary TiO2/g-C3N4/CdS nanocomposite. In this protocol, the ternary nanocomposite was first prepared to serve as the matrix to construct the PEC sensing platform. On the other hand, a well-designed hairpin DNA1 probe with 5'-hydroxyl termini was specifically phosphorylated by T4 PNK which would be selectively cleaved with lambda exonuclease (λ-Exo) outputting the 3'-thiol end ssDNA2. After tagged with CdSe QDs, ssDNA2 was captured by the complementary capture DNA3 on the electrode surface. As a result, CdSe QDs were in close contact with the ternary nanocomposite matrix, leading to an enhanced photocurrent response. Therefore, this proposed PEC platform displayed an analytical performance with a wide linear range from 0.0001 to 0.02 U mL-1 and a low detection limit down to 6.9 × 10-5 U mL-1. Moreover, this ternary nanocomposite-based platform exhibited excellent selectivity, good reproducibility, and remarkable storage stability, which shows great potential for T4 PNK detection and inhibitor screening.


Asunto(s)
Técnicas Biosensibles/métodos , Compuestos de Cadmio/química , Límite de Detección , Nanocompuestos/química , Nitrilos/química , Polinucleótido 5'-Hidroxil-Quinasa/metabolismo , Sulfuros/química , Titanio/química , Electroquímica , Inhibidores Enzimáticos/farmacología , Estudios de Factibilidad , Procesos Fotoquímicos , Polinucleótido 5'-Hidroxil-Quinasa/antagonistas & inhibidores
19.
Nanoscale ; 10(43): 20266-20271, 2018 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-30362484

RESUMEN

Tungsten diselenide (WSe2) is the material with the lowest thermal conductivity in the world. Most physical methods are used for the synthesis of tungsten diselenide. Here, a simple colloidal method is reported for the synthesis of WSe2 nanosheets. The composition, valence, size, morphology and properties of the samples were characterized and measured. Results showed that the obtained WSe2 nanosheets with a thickness of 0.7 nm had strong blue fluorescence. Significantly, the synthesized WSe2 nanosheets exhibited excellent catalytic activity for the aerobic coupling of amines to imines, with 100% yield under visible light irradiation and air atmosphere. As a photocatalyst, it exhibited excellent recyclability, and maintained a high yield after 5 cycles. It was found that this reaction could also happen in the presence of natural light by slightly extending the reaction time. Moreover, H2O was used as a solvent in the catalytic process, avoiding expensive and toxic organic solvents. This work provides an efficient, economical and sustainable process for the synthesis of imines and shows the great potential of WSe2 nanosheets as photocatalysts for organic synthesis.

20.
Biosens Bioelectron ; 116: 23-29, 2018 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-29852473

RESUMEN

A novel enhanced photoelectrochemical DNA sensor, based on a TiO2/Au hybrid electrode structure, was developed to detect target DNA. The sensor was developed by successively modifying fluorine-tin oxide (FTO) electrodes with TiO2 nanoparticles, gold (Au) nanoparticles, hairpin DNA (DNA1), and CdSe-COOH quantum dots (QDs), which acted as signal amplification factors. In the absence of target DNA, the incubated DNA1 hairpin and the CdSe-COOH QDs were in close contact with the TiO2/Au electrode surface, leading to an enhanced photocurrent intensity due to the sensitization effect. After incubation of the modified electrode with the target DNA, the hairpin DNA changed into a double helix structure, and the CdSe QDs moved away from the TiO2/Au electrode surface, leading to a decreased sensitization effect and photoelectrochemical signal intensity. This novel DNA sensor exhibited stable, sensitive and reproducible detection of DNA from 0.1 µM to 10 fM, with a lower detection limit of 3 fM. It provided good specificity, reproducibility, stability and is a promising strategy for the detection of a variety of other DNA targets, for early clinical diagnosis of various diseases.


Asunto(s)
Técnicas Biosensibles/métodos , ADN/análisis , Oro/química , Compuestos de Estaño/química , Compuestos de Cadmio/química , ADN/química , Electrodos , Flúor/química , Humanos , Secuencias Invertidas Repetidas , Límite de Detección , Procesos Fotoquímicos , Puntos Cuánticos/química , Reproducibilidad de los Resultados , Compuestos de Selenio/química , Titanio/química
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