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1.
Chem Commun (Camb) ; 60(34): 4581-4584, 2024 Apr 23.
Artículo en Inglés | MEDLINE | ID: mdl-38576349

RESUMEN

A study of an integrated OPECT biosensor gate and the EC color-changing region on the same chip was carried out, achieving sensitive detection through bioetching-induced signal changes. Enzymatic bioetching enables specific alkaline phosphatase (ALP) detection by catalyzing the production of CdS, which modulates the channel current and generates a visual signal.


Asunto(s)
Fosfatasa Alcalina , Técnicas Biosensibles , Técnicas Electroquímicas , Fosfatasa Alcalina/metabolismo , Fosfatasa Alcalina/análisis , Transistores Electrónicos , Compuestos de Cadmio/química , Sulfuros/química , Procesos Fotoquímicos
2.
Inorg Chem ; 63(16): 7356-7363, 2024 Apr 22.
Artículo en Inglés | MEDLINE | ID: mdl-38602040

RESUMEN

The photoactive material was of significant importance in organic photoelectrochemical transistor (OPECT) bioanalysis as it influences the photoinduced voltage and the µC* product, resulting in a varying sensor sensitivity. The utilization of metal-organic frameworks (MOFs) as photoactive materials in OPECT analysis is promising, yet it remains a grand challenge due to the inherently narrow light absorption range and high electron-hole recombination rate. Herein, Pd NPs were encapsulated as electron acceptors into the Cu-MOF using a double-solvent method, followed by pyrolysis at the proper temperature. After pyrolysis, Cu-MOF transformed into a carbon defect-rich composite of CuO and Cu2O while retaining its high porosity and structural morphology. The resulting carbon defect-rich pyrolysis Cu-MOF (p-Cu-MOF) served as an active support, facilitating the separation of electrons and holes. The photoelectrons trigger the electron transfer of adjacent active metal components and the formation of a Schottky junction between Pd and the MOFs. This effect induces the electron donation from the MOFs. Moreover, Pd/pyrolysis Cu-MOF exhibits significantly higher visible light absorption, better water stability, and higher electrical conductivity compared to Cu-MOF and Pd/Cu-MOF. An OPECT sensor was fabricated by utilizing Pd/p-Cu-MOF as the photoactive material and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as the channel material on an integrated laser-etched FTO. The aptamer was used as the recognition element, enabling sensitive and efficient detection of residual isocarbophos.

3.
Sci Total Environ ; 921: 171085, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38387584

RESUMEN

The development of both detection and removal technologies for heavy metal ions is of great importance. Most of the existing adsorbents that contain oxygen, nitrogen or sulfur functional groups can remove heavy metals, but achieving both selective detection and removal of a single metal ion is difficult because they bind to a wide range of heavy metal ions. Herein, we selected zeolite imidazolium hydrochloride framework-71 (ZIF-71) with sufficient chlorine functional groups to fabricate magnetic ZIF-71 multifunctional composites (M-ZIF-71). M-ZIF-71 had a large specific surface area, excellent water stability, and good magnetic properties, which made M-ZIF-71 conducive to the separation and recovery of adsorbents and the assembly of electrodes. M-ZIF-71 exhibited high selectivity, wide linear range (1-500 µg/L), and low detection limit (0.32 µg/L) for electrochemical detection of mercury ions (Hg2+). Meanwhile, M-ZIF-71 demonstrated rapid Hg2+ adsorption with a high capacity of 571.2 mg/g and excellent recyclability. The high selectivity for Hg2+ was attributed to the powerful affinity of highly electronegative chlorine and Hg2+. Moreover, XPS spectra demonstrated the interaction between chlorine and Hg2+. This work provides a new inspiration for applications in the targeted monitoring and removal of heavy metal pollution.

4.
Chem Commun (Camb) ; 60(21): 2934-2937, 2024 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-38372635

RESUMEN

The synergistic effect between surface metal vacancies and a Schottky junction on enhanced transconductance, and the gating effect of an organic photoelectrochemical transistor was reported.

5.
Inorg Chem ; 62(37): 15022-15030, 2023 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-37661907

RESUMEN

Engineering the activity of enzyme-like catalysts should be a top priority to make them superior substitutes for natural enzymes. Herein, a Ce/Zr bimetal-organic framework (Ce/Zr-MOF) was designed and synthesized by a one-pot hydrothermal method, which has enhanced performance in mimicking peroxidase (POD) than its single-metal counterparts. To further comprehend the mechanism of activity enhancement, the role of the bimetallic synergistic catalysis process in H2O2 decomposition and reactive oxygen species formation was elucidated, and the possible dual cycle synergistic catalysis pathway of bimetallic catalysis is proposed for the first time. The enhanced POD-like activity mainly depends on the introduction of Ce, which improved the conductivity and electron-transfer capability of Ce/Zr-MOF and promoted the generation of •OH. Integrated with a hydrogel substrate, a wearable all-solid-state H2O2 sensor for early diagnosis of plant health was produced. The detection limit can be as low as 3.3 µM, which is lower than that of some instrument-based colorimetric methods and has great potential in the development of visualized sensing applications. The concept of dual cycle synergistic catalysis pathway we proposed not only deepens the comprehension regarding sensing and catalytic mechanisms but also provides novel perspectives into the design of enzyme-like catalysts for extensive usage.


Asunto(s)
Peroxidasa , Dispositivos Electrónicos Vestibles , Hidrogeles , Peróxido de Hidrógeno , Peroxidasas , Catálisis , Colorantes
6.
Anal Chem ; 95(40): 15049-15056, 2023 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-37755312

RESUMEN

The polarity of the photocurrent can be modulated by tunable bipolar photoelectrochemical (PEC) behavior, which is anticipated to address the issues of high background signal caused by traditional unidirectional increasing/decreasing response and false-positive/false-negative problems. Here, a new approach is suggested for the first time, which employs a target-induced enzyme-catalyzed reaction and in situ oxygen vacancy (OV) generation to achieve heterojunction photocurrent switching for highly sensitive detection of alkaline phosphatase (ALP). Among them, the ALP can catalyze the decomposition of ascorbic acid phosphate to produce ascorbic acid, which not only acts as an electron donor to change the redox environment but also acts as a reducing agent to introduce OVs into BiOBr semiconductors in cooperation with illumination. The introduction of vacancies can effectively modulate the energy band structure of BiOBr, while with the change of redox conditions, the transfer path of photogenerated carriers is changed, thus realizing the switching of photocurrents, which leads to its use in the construction of a negative-background anti-interference PEC sensing platform, achieving a wide linear range from 0.005 to 500 U·L-1 with a low detection limit of 0.0017 U·L-1. In conclusion, the photocurrent switching operation of this system is jointly regulated by chemistry, optics, and carrier motion, which provides a new idea for the construction of a PEC sensing platform based on photocurrent polarity switching.

7.
Food Chem ; 423: 136285, 2023 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-37156141

RESUMEN

Detection of T-2 toxin is of great significance to environment and human health, as T-2 toxin is one of the main toxins that contaminate crops, stored grain and other food. Herein, a zero-gate-bias organic photoelectrochemical transistor (OPECT) sensor was proposed based on nanoelectrode arrays as gate photoactive materials which can result in the accumulation of photovoltage and preferable capacitance leading to better sensitivity of the OPECT. For comparison, the channel current of OPECT was 100 times higher than photocurrent of conventional photoelectrochemical (PEC) attributing to remarkable signal amplification of OPECT. It was also found that the detection limit of OPECT aptasensor was as low as 28.8 pg/L, lower than 0.34 ng/L of the conventional PEC method, further indicating the advantage of the OPECT devices in T-2 toxin determination. This research has been successfully applied in real sample detection which provided a general platform of OPECT for food safety analysis.


Asunto(s)
Aptámeros de Nucleótidos , Técnicas Biosensibles , Nanotubos , Toxina T-2 , Humanos , Animales , Leche , Técnicas Electroquímicas/métodos , Técnicas Biosensibles/métodos , Límite de Detección
8.
Chem Commun (Camb) ; 59(1): 75-78, 2022 Dec 22.
Artículo en Inglés | MEDLINE | ID: mdl-36468236

RESUMEN

A novel strong solvent coordination leaching method was developed to prepare surface zinc vacancies in ZnO nanorod arrays. Remarkably, the surface-zinc-vacancy-rich ZnO nanorod arrays exhibit high electron-hole separation efficiency and excellent photoelectrochemical performance for use as a promising candidate for the next generation of organic photoelectrochemical transistor aptasensors.


Asunto(s)
Nanotubos , Óxido de Zinc , Zinc , Electrones
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