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1.
Langmuir ; 40(13): 7060-7066, 2024 Apr 02.
Artículo en Inglés | MEDLINE | ID: mdl-38513212

RESUMEN

Nanosheet arrays with stable signal output have become promising photoactive materials for photoelectrochemical (PEC) immunosensors. However, an essential concern is the facile recombination of carriers in one-component nanoarrays, which cannot be readily prevented, ultimately resulting in weak photocurrent signals. In this study, an immunosensor using gold nanoparticle-anchored BiOI/Bi2S3 nanosheet arrays (BiOI/Bi2S3/Au) as a signal converter was fabricated for sensitive detection of cardiac troponin I (cTnI). The ternary nanosheet arrays were prepared by a simple method in which Bi2S3 was well-coated on the BiOI surface by in situ growth, whereas the addition of Au further improved the photoelectric conversion efficiency and could link more antibodies. The three-dimensional (3D) ordered sheet-like network array structure and BiOI/Bi2S3/Au ternary nanosheet arrays showed stable and high photoelectric signal output and no significant difference in signals across different batches under visible light excitation. The fabricated immunosensor has a sensitive response to the target detection marker cTnI in a wide linear range of 500 fg/mL to 50 ng/mL, and the detection limit was 32 fg/mL, demonstrating good stability and selectivity. This work not only shows the great application potential of ternary heterojunction arrays in the field of PEC immunosensors but also provides a useful exploration for improving the stability of immunosensors.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Troponina I , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Oro/química , Inmunoensayo/métodos , Límite de Detección , Troponina I/química , Troponina I/inmunología , Bismuto/química
2.
Mikrochim Acta ; 191(5): 280, 2024 04 22.
Artículo en Inglés | MEDLINE | ID: mdl-38649540

RESUMEN

An interfacial galvanic replacement strategy to controllable synthesize palladium nanoparticles (Pd NPs)-modified NiFe MOF nanocomposite on nickel foam, which served as an efficient sensing platform for quantitative determination of dopamine (DA). Pd NPs grown in situ on the nanosheets of NiFe MOF via self-driven galvanic replacement reaction (GRR) and well uniform distribution was achieved. This method effectively reduced the aggregation of metallic nanoparticles and significantly promoted the electron transfer rate during the electrochemical process, leading to improved electrocatalytic activity for DA oxidation. Remarkably, the precisely constructed biosensor achieved a low detection limit (LOD) of 0.068 µM and recovery of 94.1% (RSD 6.7%, N = 3) for simulated real sample detection and also exhibited superior selectivity and stability. The results confirmed that the as-fabricated Pd-NiFe/NF composite electrode could realize the quantitative determination of DA and showed promising prospects in real sample biosensing.


Asunto(s)
Técnicas Biosensibles , Dopamina , Estructuras Metalorgánicas , Nanoestructuras , Dopamina/análisis , Nanoestructuras/química , Nanoestructuras/ultraestructura , Técnicas Electroquímicas/instrumentación , Técnicas Electroquímicas/métodos , Técnicas Electroquímicas/normas , Níquel/química , Electrodos/normas , Paladio/química , Técnicas Biosensibles/instrumentación , Técnicas Biosensibles/métodos , Microscopía Electrónica de Rastreo , Estructuras Metalorgánicas/síntesis química , Estructuras Metalorgánicas/ultraestructura , Sensibilidad y Especificidad , Conductividad Eléctrica , Microscopía Electrónica de Transmisión , Hierro/química , Reproducibilidad de los Resultados
3.
J Environ Manage ; 357: 120597, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38552510

RESUMEN

Graphitic carbon nitride (g-C3N4) is a promising metal-free photocatalyst; however, its high carrier recombination rate and insufficient redox capacity limit its degradation effect on antibiotics. In order to overcome these shortcomings, the photocatalytic activity is improved by regulating the spin polarization state, constructing the internal electric field, and applying the external piezoelectric field. In this paper, the chlorine-doped and nitrogen-deficient porous carbon nitride composite carbon quantum dots (Nv-Cl/UPCN@CQD) has been synthesized successfully. The doping position of chlorine and spin polarization properties are verified by DFT calculation. The key intermediates *O2- and *OOH for the synthesis of reactive oxygen species were detected by in-situ infrared testing, which promotes the production of •O2- and H2O2. The degradation rate constant of Nv-Cl/UPCN@CQD for removal of tetracycline is 8.45 times higher than that of g-C3N4. The active oxygen production and degradation efficiency of piezoelectric photocatalysis under the synergistic effect of intense stirring and vis-light irradiation are much higher than those of photocatalysis and piezoelectric catalysis, and the conversion of H2O2 to •OH is promoted by piezoelectric field. This paper provides a reliable way to improve the performance of piezoelectric photocatalysts by adjusting their energy band, electronic structure and piezoelectric force.


Asunto(s)
Cloro , Puntos Cuánticos , Peróxido de Hidrógeno , Antibacterianos , Nitrógeno , Puntos Cuánticos/química , Catálisis
4.
Zhongguo Dang Dai Er Ke Za Zhi ; 26(6): 639-645, 2024 Jun 15.
Artículo en Zh | MEDLINE | ID: mdl-38926382

RESUMEN

OBJECTIVES: To explore the effects of iris xanthin on airway inflammation, airway remodeling, and the high mobility group box 1 protein (HMGB1)/Toll-like receptor 4 (TLR4)/nuclear factor-κB (NF-κB) pathway in asthmatic young mice. METHODS: Sixty male BALB/c young mice were randomly assigned into six groups: a blank group, a model group, a dexamethasone group, and low, medium, and high dose groups of iris xanthin, with ten mice per group. Asthma models were induced through intraperitoneal injections of a sensitizing agent [ovalbumin (OVA) 20 µg + aluminum hydroxide gel 2 mg], followed by 4% OVA aerosol inhalation. Lung function was measured using a pulmonary function tester to determine lung volume (LV), resting ventilation per minute (VE), and airway reactivity (Penh value). Hematoxylin-eosin (HE) staining was employed to examine and analyze airway remodeling. The contents of interleukin (IL)-1ß, IL-6, and tumor necrosis factor alpha (TNF-α) in bronchoalveolar lavage fluid were quantified using ELISA. Real-time fluorescence quantitative polymerase chain reaction and Western blot analysis were used to assess the expression of HMGB1/TLR4/NF-κB pathway-related mRNA and proteins in lung tissues. RESULTS: Compared to the model group, the dexamethasone and iris xanthin-treated groups (low, medium, and high doses) exhibited significant increases in LV and VE (P<0.05), with incremental dose-dependent increases observed in the iris xanthin groups. Additionally, Penh values, IL-1ß, IL-6, TNF-α, and airway remodeling indicators, along with mRNA levels of HMGB1, TLR4, and NF-κB p65 and protein levels of HMGB1, TLR4, and p-NF-κB p65, were all reduced (P<0.05) in a dose-dependent manner. When compared to the dexamethasone group, the low and medium dose iris xanthin groups showed decreases in LV and VE (P<0.05), whereas Penh values, IL-1ß, IL-6, TNF-α, and airway remodeling indicators, along with mRNA levels of HMGB1, TLR4, NF-κB p65 and protein levels of HMGB1, TLR4, and p-NF-κB p65, were increased (P<0.05). No significant differences were noted in these indices between the high dose iris xanthin group and the dexamethasone group (P>0.05). CONCLUSIONS: Iris xanthin can effectively alleviates airway inflammation and inhibits airway remodeling in asthmatic young mice, possibly through the suppression of the HMGB1/TLR4/NF-κB pathway.


Asunto(s)
Remodelación de las Vías Aéreas (Respiratorias) , Asma , Proteína HMGB1 , Ratones Endogámicos BALB C , FN-kappa B , Transducción de Señal , Receptor Toll-Like 4 , Animales , Remodelación de las Vías Aéreas (Respiratorias)/efectos de los fármacos , Asma/tratamiento farmacológico , Asma/metabolismo , Masculino , Ratones , Receptor Toll-Like 4/genética , Receptor Toll-Like 4/metabolismo , Proteína HMGB1/genética , Proteína HMGB1/metabolismo , FN-kappa B/metabolismo , Transducción de Señal/efectos de los fármacos
5.
Anal Chem ; 95(36): 13596-13604, 2023 09 12.
Artículo en Inglés | MEDLINE | ID: mdl-37643000

RESUMEN

Metal oxide nanomaterials have garnered significant attention in the field of electrochemiluminescence (ECL) sensing due to their efficient, stable, and nontoxic properties. However, the current research on metal oxide nanomaterials has primarily focused on their cathodic luminescence properties, with limited reports on their anodic ECL properties. In this study, we utilized MOF-derived ZrO2 nanomaterials as luminophores to generate stable anodic ECL signals in the presence of the coreactant tripropylamine (TPrA). Additionally, a signal-enhancing immunosensor was developed to analyze D-dimer by incorporating the coreaction accelerator Cu-doped TiO2 (TiO2-Cu). The ZrO2 synthesized by calcining UiO-67 demonstrated nontoxicity and biocompatibility, exhibiting efficient and stable ECL emission in a TPrA solution. The inclusion of TiO2-Cu as a coreaction accelerator in the immunosensor resulted in the formation of a ternary system of ZrO2/TiO2-Cu/TPrA. The Cu doping effectively narrowed the bandgap of TiO2 and enhanced its conductivity. As a substrate, TiO2-Cu reacted with more TPrA, generating sufficient free radicals to effectively enhance the ECL signal of ZrO2. In this article, a short peptide ligand, NFC (NARKFYKGC), was designed to immobilize antibodies and maintain the activity of antigen-binding sites during the construction of the immunosensor. The developed immunosensor was used for the accurate detection of D-dimers, with a wide linear range of 0.05-600 ng/mL and a low detection limit of 21 pg/mL..


Asunto(s)
Técnicas Biosensibles , Nanoestructuras , Inmunoensayo , Óxidos
6.
Anal Chem ; 95(38): 14317-14323, 2023 09 26.
Artículo en Inglés | MEDLINE | ID: mdl-37695886

RESUMEN

Inspired by the signal accumulation of circular DNA strand displacement reactions (CD-SDRs) and the in situ generation of silver nanoclusters (AgNCs) from signature template sequences, a dual-signal integrated aptasensor was designed for microcystin-LR (MC-LR) detection. The aptamer was programmed to be included in an enzyme-free CD-SDR, which utilized MC-LR as the primer and outputted the H1/H2 dsDNA in a continuous manner according to the ideal state. Ingeniously, H1/H2 dsDNA was enriched with signature template sequences, allowing in situ generation of AgNCs signal probes. To enhance the signal amplification performance, co-reaction acceleration strategies and CRISPR-Cas12a nucleases were invoked. The H1/H2 dsDNA could trigger the incidental cleavage performance of CRISPR-Cas12a nucleases: cis-cleavage reduced signature template sequences for the synthetic AgNCs, while trans-cleavage enabled fluorescence (FL) analysis. Meanwhile, AuPtAg was selected as the substrate material to facilitate the S2O82- reduction reaction for enhancing the electrochemiluminescence (ECL) basal signals. ECL and FL detection do not interfere with each other and have improved accuracy and sensitivity, with limits of detection of 0.011 and 0.023 pmol/L, respectively. This widens the path for designing dual-mode sensing strategies for signal amplification.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Nanopartículas del Metal , ADN Circular , Plata , ADN/genética , Aptámeros de Nucleótidos/genética , Límite de Detección
7.
Anal Chem ; 95(24): 9139-9144, 2023 06 20.
Artículo en Inglés | MEDLINE | ID: mdl-37284794

RESUMEN

In this work, a sensitive signal-on electrochemiluminescence biosensor using liposome-encapsuled 1,1,2,2-tetra(4-carboxylphenyl)ethylene (TPE) as a promising aggregation-induced electrochemiluminescence (AIECL) emitter for detection of biomarkers was developed. Aggregation-induced enhancement occurs internally through the spatial confinement effect and intramolecular self-encapsulation of encapsulating TPE and triethylamine (TEA) molecules in liposome cavities. Peptide sequence WTGWCLNPEESTWGFCTGSF (WF-20) was used to replace the antibody for reducing the steric hindrance of the sensing surface while taking into account the affinity. The proposed sensing strategies showed satisfactory properties for detection of human epidermal growth factor receptor 2 (HER2) ranging from 0.01 to 500 ng/mL with a limit of detection of 6.65 pg/mL. The results confirmed that encapsulation of luminescent molecules in the vesicle structure for triggering the AIECL phenomenon is a promising method to prepare a signal label for a trace detection biomarker.


Asunto(s)
Técnicas Biosensibles , Estilbenos , Humanos , Liposomas , Receptor ErbB-2 , Estilbenos/química , Técnicas Biosensibles/métodos , Mediciones Luminiscentes/métodos , Técnicas Electroquímicas/métodos , Límite de Detección
8.
Anal Chem ; 95(45): 16761-16770, 2023 Nov 14.
Artículo en Inglés | MEDLINE | ID: mdl-37905934

RESUMEN

Copper nanoclusters (Cu NCs) are highly promising nanomaterials in the field of electrochemiluminescence (ECL). Nevertheless, their limited stability and efficiency have impeded their practical applications. Here, we introduced a novel supramolecular anchoring strategy resulting in the creation of exceptionally stable Cu NCs (CET-Cu NCs) with remarkable ECL properties. Specifically, CET-Cu NCs exhibited a relative ECL efficiency (ΦECL) of 62% based on the annihilation ECL efficiency of [Ru(bpy)3]2+ (100%), with tripropylamine employed as a coreactant. Moreover, CET-Cu NCs can generate ECL emission through multiple different paths, which enables them to serve as signal probes in a wider range of testing scenarios, thereby enhancing the reliability and robustness of sensing and analytical systems. To demonstrate the practical utility, CET-Cu NCs were selected as an ECL signal probe for a sensing platform that facilitated ultrasensitive detection of progesterone via oriented immobilization technology and antibody/aptamer sandwich assays. This study surmounted the barriers to the practical application of Cu NCs through the implementation of a supramolecular anchoring strategy, thereby providing enhanced utility of Cu NCs in ECL sensing and analysis.

9.
Anal Chem ; 95(22): 8720-8727, 2023 06 06.
Artículo en Inglés | MEDLINE | ID: mdl-37224306

RESUMEN

Currently, the construction of heterojunctions as a method to enhance photoelectrochemical (PEC) activity has shown prospective applications in the analytical field. Restricted by carrier separation at the interface, developing a heterojunction sensing platform with high sensitivity remains challenging. Here, a double-photoelectrode PEC sensing platform was fabricated based on an antenna-like strategy by integrating MIL-68(In)-NH2, a p-type metal-organic framework (MOF) photocatalyst, as a photocathode with the type-II heterojunction of CdSe/MgIn2S4 as a photoanode synchronously. According to the ligand-to-metal charge transition (LMCT), the photo-generated carriers of MIL-68(In)-NH2 transferred from the organic ligand to the metal cluster, which provides an efficient antenna-like transfer path for the charge at the heterojunction interface. In addition, the sufficient Fermi energy difference between the double photoelectrode provides the continuous internal driving force required for rapid carrier separation at the anode detection interface, significantly improving the photoelectric conversion efficiency. Hence, compared with the traditional heterojunction single electrode, the photocurrent response of the double-photoelectrode PEC sensing platform developed using the antenna-like strategy is 2.5 times stronger. Based on this strategy, we constructed a PEC biosensor for the detection of programed death-ligand 1 (PD-L1). The elaborated PD-L1 biosensor exhibited sensitive and precise detection capability with a detection range of 1 × 10-5 to 1 × 103 ng/mL and a lower detection limit of 3.26 × 10-6 ng/mL and demonstrated the feasibility of serum sample detection, providing a novel and viable approach for the unmet clinical need of PD-L1 quantification. More importantly, the charge separation mechanism at the heterojunction interface proposed in this study provides new creative inspiration for designing sensors with high-sensitivity PEC performance.


Asunto(s)
Técnicas Biosensibles , Estructuras Metalorgánicas , Antígeno B7-H1 , Ligandos , Oro , Técnicas Biosensibles/métodos , Técnicas Electroquímicas , Límite de Detección
10.
Anal Bioanal Chem ; 415(22): 5551-5562, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37401964

RESUMEN

An efficient photo-to-electrical signal is pivotal to photoelectrochemical (PEC) biosensors. In our work, a novel PEC biosensor was fabricated for the detection of neuron-specific enolase (NSE) based on a ZnIn2S4/Ag2CO3 Z-scheme heterostructure. Due to the overlapping band potentials of the ZnIn2S4 and Ag2CO3, the formed Z-scheme heterostructure can promote the charge separation and photoelectric conversion efficiency. And the concomitant Ag nanoparticles in Ag2CO3 provided multiple functions to enhance the PEC response of the Z-scheme heterostructure. It acts not only as a bridge for the transfer of carriers between ZnIn2S4 and Ag2CO3, promoting the constructed Z-scheme heterostructure, but also as electron mediators to accelerate the transfer of photogenerated carriers and improve the capture of visible light of the Z-scheme heterostructure by surface plasmon resonance (SPR). Compared with single Ag2CO3 and ZnIn2S4, the photocurrent of the designed Z-scheme heterostructure increased more than 20 and 60 times respectively. The fabricated PEC biosensor based on a ZnIn2S4/Ag2CO3 Z-scheme heterostructure exhibits sensitive detection to NSE, and presents a linear range of 50 fg·mL-1 ~ 200 ng·mL-1 with a limit of detection of 4.86 fg·mL-1. The proposed PEC biosensor provides a potential approach for clinical diagnosis.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Nanopartículas del Metal/química , Técnicas Electroquímicas , Plata , Fosfopiruvato Hidratasa , Límite de Detección
11.
Mikrochim Acta ; 190(6): 249, 2023 06 02.
Artículo en Inglés | MEDLINE | ID: mdl-37266715

RESUMEN

A sandwich-type electrochemical immunosensor was designed by highly efficient catalytic cycle amplification strategy of CuFe2O4-Pd for sensitive detection of cardiac troponin I. CuFe2O4 with coupled variable valence metal elements exhibited favorable catalytic performance through bidirectional cycling of Fe2+/Fe3+ and Cu+/Cu2+ redox pairs. More importantly, Cu+ acted as the intermediate product of the catalytic reaction, promoted the regeneration of Fe2+ and ensured the continuous recycling occurrence of the double redox pairs, and significantly amplified the current signal response. Pd nanoparticles (Pd NPs) loaded on the surface of amino-functionalized CuFe2O4 (CuFe2O4-NH2) served as electrochemical mediators to capture labeled antibodies (Ab2), and also as co-catalysts of CuFe2O4 to further enhance the catalytic efficiency, thus improving the sensitivity of the electrochemical immunosensor. Under the optimal experimental conditions, the linear range was 0.001 ~ 100 ng/mL, and the detection limit was 1.91 fg/mL. The electrochemical immunosensor has excellent analytical performance, giving a new impetus for the sensitive detection of cTnI.


Asunto(s)
Técnicas Biosensibles , Grafito , Nanopartículas del Metal , Troponina I , Anticuerpos Inmovilizados , Inmunoensayo
12.
Anal Chem ; 94(45): 15873-15878, 2022 11 15.
Artículo en Inglés | MEDLINE | ID: mdl-36322926

RESUMEN

Herein, a novel dual mode detection system of split-type photoelectrochemical (PEC) and visual immunoassay was developed to detect neuron specific enolase (NSE), which achieved simultaneous and reliable NSE detection due to the completely different signal readouts and transduction mechanism. Specifically, specific reactions of antigens and antibodies were performed in 96-microwell plates. Gold nanoparticle (Au NP)-loaded Fe3O4 (Au@Fe3O4) NPs were used as secondary antibody markers and signal regulators, which could produce a blue-colored solution in the presence of 3,3',5,5'-tetramethylbenzidine (TMB) and H2O2 because of its peroxidase-like activity. Therefore, the visual detection of NSE was realized, making the results more intuitive. Meanwhile, the above biological process could also be used as part of the split-type PEC sensing platform. Oxidized TMB and Fe3+ were consumptive agents of the electron donor, which both realized the double quenching of PEC signal generated by the SnO2/MgIn2S4/Zn0.1Cd0.9S composites. Owing to the waterfall band structure, SnO2/MgIn2S4/Zn0.1Cd0.9S composites partially absorb visible light and effectively inhibit the electron-hole recombination, thereby providing significantly enhanced and stable initial signal. On the basis of the multiple signal amplification strategy and the split-type mode, NSE could be sensitively detected with a low detection limit of 14.0 fg·mL-1 (S/N = 3) and a wide linear range from 50.0 fg·mL-1 to 50.0 ng·mL-1.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Oro/química , Técnicas Electroquímicas/métodos , Cadmio , Nanopartículas del Metal/química , Técnicas Biosensibles/métodos , Límite de Detección , Peróxido de Hidrógeno/química , Inmunoensayo/métodos , Fosfopiruvato Hidratasa , Zinc
13.
Anal Chem ; 94(37): 12852-12859, 2022 09 20.
Artículo en Inglés | MEDLINE | ID: mdl-36075077

RESUMEN

The self-luminescence behavior of lanthanide MOFs (Ln-MOFs) due to the unique antenna effect is considered to be a promising electrochemiluminescence (ECL) emission for biosensors. It is more challenging for Ln-MOFs on account of the difficulty to stimulate Ln ions with the desired energy-transfer efficiency to produce stronger ECL emissions at a low potential. Here, guided by a second ligand-assisted energy-transfer strategy, we present an efficient self-enhanced luminescence mixed-ligand Eu-MOF as an ECL signal probe for an oriented antibody-decorated biosensing platform with a low detection limit and a broad detection range. Diamino terephthalic acid (NH2-H2BDC) and 1,10-phenanthroline (Phen) were selected as the first and second ligands, respectively, to form highly conjugated structures, as well as suppress the nonradiative energy transfer. Impressively, Phen precisely adjusts the energy gap between the triplet ligand and the excited state of Eu3+, realizing the self-enhancement of ECL efficiency of the Eu-MOF. The mixed ligand adjusted the molar ratio to obtain the stable and strong ECL signal at a lowered triggering potential (0.83 V). In addition, FeCo@CNT features densely active FeCo sites along with a rich hierarchy conductive carbon nanotube (CNT) network, which is efficiently a co-reaction accelerator to produce more TPA•+ radicals to accelerate the reduction process of the Eu-MOF for achieving the ECL emission amplification. FeCo@CNT with heptapeptide HWRGWVC (HWR) constructed a matrix biosensing interface that allowed the fragment antigen-binding (Fab) regions to target specific antigens and enhance the incubation efficiency. The present study has gone some way toward designing a self-enhanced luminous Eu-MOF, thus giving new fresh impetus to develop high-performance ECL emitters for biological analysis.


Asunto(s)
Técnicas Biosensibles , Elementos de la Serie de los Lantanoides , Nanotubos de Carbono , Anticuerpos , Técnicas Electroquímicas , Ligandos , Límite de Detección , Mediciones Luminiscentes , Fenantrolinas
14.
J Org Chem ; 87(14): 9232-9241, 2022 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-35748751

RESUMEN

We herein report the first visible-light-induced hydromono- and difluoroalkylations of alkenes with inexpensive and easily accessible α-fluoro carboxylic acids. This metal-free protocol exhibits mild conditions, high efficiency, and excellent functional-group tolerance, providing a straightforward approach to mono- and difluoroalkylated alkanes. Moreover, the fluorine effect on the hydrofluoroalkylation reaction is discussed in detail.

15.
Mikrochim Acta ; 189(9): 359, 2022 09.
Artículo en Inglés | MEDLINE | ID: mdl-36040532

RESUMEN

A sandwich-type electrochemical immunosensor was designed for the ultrasensitive detection of prostate-specific antigen (PSA), using Au nanoparticles (Au NPs) modified nitrogen-doped porous carbon (NPC) as sensor platform and trimetallic PdAgCu mesoporous nanospheres (PdAgCu MNSs) as enzyme-mimicking labels. NPC was prepared by a facile one-step pyrolysis strategy of biomimetic phylloid zeolite imidazole framework (ZIF-L) nanosheets. Through this strategy, the graphitization of the microcrystalline structure enhanced the electrical conductivity, while its enlarged specific surface area and abundant pore volume can enrich H2O2 to improve the catalytic efficiency. Moreover, Au NPs were used to modify NPC without cross-linking agents to further optimize electron transport while capturing primary antibodies, improving stability and sensitivity of the immunosensor. PdAgCu MNSs with uniform size, cylindrical open mesoporous channels, and continuous crystal frame structure were self-assembling synthesized by electrostatic adsorption and ascorbic acid (AA) co-reduction with amphiphilic dioctadecyldimethylammonium chloride (DODAC) as surfactant-cum-micelle, whose unique structure maximizes the use of polyatoms to expose catalytic sites, exhibiting good biocompatibility and electrocatalytic ability. Under the optimal conditions, the immunosensor showed superior sensitivity, a wide dynamic detection range (10 fg mL-1 ~ 100 ng mL-1) and a low limit of detection (LOD, 3.29 fg mL-1). This work provides a convenient strategy for the clinical detection of PSA.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Nanoporos , Anticuerpos Inmovilizados/química , Carbono/química , Técnicas Electroquímicas , Oro/química , Humanos , Peróxido de Hidrógeno/química , Inmunoensayo , Límite de Detección , Masculino , Nanopartículas del Metal/química , Nitrógeno , Porosidad , Antígeno Prostático Específico
16.
Mikrochim Acta ; 188(4): 109, 2021 03 04.
Artículo en Inglés | MEDLINE | ID: mdl-33660023

RESUMEN

The hepatitis B virus (HBV) can cause chronic hepatitis and hepatocellular carcinoma. Hepatitis B surface antigen (HBs-Ag) and Hepatitis B e-antigen (HBe-Ag) are key markers for the diagnosis of HBV. In this study, electrodeposited gold was used as a sensing platform. Three-dimensional (3D) SnO2-loaded graphene sheets functionalized by Thionine (Thi) and ferrocene (Fc) and hybridized by sea urchin-like bimetallic nanoparticles (GS-SnO2-BMNPs) were used as redox probes for labeling antibodies to fabricate sandwich-type immunosensors for the simultaneous determination of HBs-Ag and HBe-Ag. The bimetallic nanoparticles, gold hybrid platinum nanoparticles (Au@Pt) and L-cysteine-connected gold-silver nanoparticles (Ag-cys-Au), have large electroactive surface areas. They were prepared by an efficient and economical method. Additionally, the sea urchin morphology accelerates spatial utilization, thus increasing the number of combination sites. Therefore, the immune probe can load a mass of signal source molecules (Thi and Fc). Furthermore, GS-SnO2-BMNPs (GS-SnO2-Au@Pt and GS-SnO2-Ag-cys-Au) with excellent electrical conductivity and bimetallic synergy can enhance the square wave voltammetry (SWV) signal. SWV was used to record the electrochemical signal by scanning the potential from - 0.6 to 0.6 V (vs. SCE). The signal peaks resulted from the reduction reaction of Thi and Fc, and two signal peaks were completely separate. The peak position and current intensity reflect the identity and level of the corresponding antigens. Therefore, the simultaneous detection of two viral biomarkers was achieved by the proposed immunosensor. The fabricated immunosensor showed a linear concentration range for HBs-Ag (0.01-100 ng·mL-1) and HBe-Ag (0.01-100 ng·mL-1), with detection limits for HBs-Ag and HBe-Ag of  4.67 pg·mL-1 and 4.68 pg·mL-1, respectively.  The RSD of HBs-Ag ranged between 2.0 and 4.4%and the recovery was in the range 98.7 to 99.4%. For  HBe-Ag the RSD  was between 2.6 and 3.3% andrecoveries  in the range 99.2 to 100.5% were obtained.


Asunto(s)
Antígenos de Superficie de la Hepatitis B/sangre , Antígenos e de la Hepatitis B/sangre , Virus de la Hepatitis B/química , Inmunoensayo/métodos , Anticuerpos Inmovilizados/inmunología , Anticuerpos Monoclonales/inmunología , Técnicas Electroquímicas/métodos , Compuestos Ferrosos/química , Oro/química , Grafito/química , Antígenos de Superficie de la Hepatitis B/inmunología , Antígenos e de la Hepatitis B/inmunología , Humanos , Límite de Detección , Nanopartículas del Metal/química , Metalocenos/química , Fenotiazinas/química , Plata/química , Compuestos de Estaño/química
17.
Anal Chem ; 92(16): 10935-10939, 2020 08 18.
Artículo en Inglés | MEDLINE | ID: mdl-32806903

RESUMEN

An intramolecular photoelectrochemical (PEC) system is designed from the novel electron donor YYYHWRGWV (Y3-H) peptide ligand for the first time. The bifunctional nonapeptide cannot only rely on the HWRGWV sequence as a site-oriented immobilizer to recognize the crystallizable fragment (Fc) domains of the antibody but also acts as electron donors for PEC generation via three tyrosine (Y) of the N-terminal. The Bi2WO6/AgInS2 heterojunction with a significant visible-light absorption is utilized as a photoelectric generator, and the motivation is ascribed to a proven proposition, namely, that short-wavelength illuminant radiates proteins, causing a decline in bioactivity of immune protein. An innovative biosensor is fabricated using the above strategies for the detection of CYFRA21-1, a biomarker of squamous cell lung carcinoma. This sort of PEC-based sensing platform shows convincing experimental data and could be an effective candidate for clinical application in the future due to their extremely skillful conception.


Asunto(s)
Antígenos de Neoplasias/sangre , Biomarcadores de Tumor/sangre , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Queratina-19/sangre , Péptidos/química , Tirosina/química , Anticuerpos Inmovilizados/química , Anticuerpos Inmovilizados/inmunología , Antígenos de Neoplasias/inmunología , Biomarcadores de Tumor/inmunología , Bismuto/química , Electrones , Humanos , Indio/química , Indio/efectos de la radiación , Queratina-19/inmunología , Luz , Límite de Detección , Fotoquímica/métodos , Puntos Cuánticos/química , Puntos Cuánticos/efectos de la radiación , Compuestos de Plata/química , Compuestos de Plata/efectos de la radiación , Compuestos de Tungsteno/química , Compuestos de Tungsteno/efectos de la radiación
18.
Org Biomol Chem ; 17(3): 573-584, 2019 01 16.
Artículo en Inglés | MEDLINE | ID: mdl-30574975

RESUMEN

Without employing any transition metal, a highly enantioselective α-alkylation of cyclic ß-keto esters and ß-keto amides has been realized by phase-transfer catalysis. This improved procedure is applicable to different kinds of halides with cinchona derivatives and gives the corresponding products in excellent enantiopurities (up to 98% ee) and good yields (up to 98%). Moreover, the reaction was scalable and the phase-transfer catalyst was recyclable. This provided an alternative and competitive method to the asymmetric α-alkylation of ß-dicarbonyl compounds.

19.
Environ Sci Technol ; 53(3): 1536-1544, 2019 02 05.
Artículo en Inglés | MEDLINE | ID: mdl-30589545

RESUMEN

The individual cellular level and quantitative Polyphosphate (PolyP)-metal compositions in EBPR (enhanced biological phosphorus removal) systems have hardly been investigated and its potential link to EBPR performance therefore remain largely unknown. In this study, we applied scanning electron microscopy combined with energy dispersive X-ray spectroscopy (SEM/EDX) method that enabled detection and semiquantification of metal elemental compositions in intact intracellular PolyP granules in individual PAO (polyphosphate accumulating organism) cells. We, for the first time, revealed diverse and dynamic distributions of different metals ions in the PolyP-metal granules in different EBPR systems operated with the same influent metal composition but varying SRT of 5-30 days. We further demonstrated that the PolyP-metal composition diversity correlated with 16S rRNA gene based PAO phylogenetic diversity, suggesting the possible phylogeny-dependent PolyP-metal composition variation. The impact of PolyP metal composition in EBPR system, especially the Mg content in PolyP granules, was evidenced by the significant and strong positive correlation between PolyP-Mg content and the long-term stability of the four EBPR systems with varying SRTs. The PolyP-Mg content can therefore possibly serve as an indicator for EBPR performance monitoring. The results demonstrated that phenotyping techniques, such as PolyP-metal-based profiling, in compliment, or combined with genotyping techniques such as phylogenetic and functional gene sequencing, can provide more insights into the mechanisms and performance prediction of this important microbial ecosystem.


Asunto(s)
Ecosistema , Fósforo , Reactores Biológicos , Metales , Filogenia , Polifosfatos , ARN Ribosómico 16S , Aguas del Alcantarillado
20.
Mikrochim Acta ; 186(11): 693, 2019 10 12.
Artículo en Inglés | MEDLINE | ID: mdl-31605244

RESUMEN

A composite nanoenzyme was used in a sandwich-type electrochemical immunoassay for the carcinoembryonic antigen (CEA). Hierarchically porous palladium nanospheres (Pd NPs) were functionalized with glutathione-capped gold nanoparticles (G-Au NPs) and then loaded onto graphene oxide (GO) to obtain a peroxidase mimicking nanoenzyme of type GO-supported G-Au/Pd. The composite can catalyze the oxidation of the substrate tetramethylbenzidine (TMB) by H2O2 to give blue-colored oxidized TMB within only 20 s. This strong peroxidase activity, good conductivity and high specific surface area of the material make it a useful label for secondary antibodies (Ab2) for the detection of CEA. The cotton-like electrodeposited gold nanoparticles with good electrical conductivity were used to immobilize primary antibody (Ab1). The amperometric immunoassay has a detection range that extends from 10 fg·mL-1 to 100 ng·mL-1 at a working potential of -0.4 V with addition of 5 mmol·L-1 H2O2 as electrochemically active substrate, and the detection limit is as low as 3.2 fg·mL-1 (S/N = 3). Graphical abstract Schematic of sandwich electrochemical immunosensor for the carcinoembryonic antigen. Electrodeposited gold used as substrate material, and Graphene oxide supported G-Au NPs functionalized porous Pd nanospheres (GO supported G-Au/Pd) as signal amplification platform, which catalyze the oxidation of tetramethylbenzidine (TMB).


Asunto(s)
Materiales Biomiméticos/química , Antígeno Carcinoembrionario/sangre , Técnicas Electroquímicas/métodos , Inmunoensayo/métodos , Nanopartículas del Metal/química , Nanosferas/química , Anticuerpos Inmovilizados/inmunología , Bencidinas/química , Biomarcadores de Tumor/sangre , Biomarcadores de Tumor/inmunología , Antígeno Carcinoembrionario/inmunología , Colorantes/química , Glutatión/química , Oro/química , Grafito/química , Humanos , Peróxido de Hidrógeno/química , Límite de Detección , Paladio/química , Peroxidasa/química , Reproducibilidad de los Resultados
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