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1.
Anal Chem ; 95(36): 13614-13619, 2023 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-37639529

RESUMEN

9-Mesityl-10-methylacridinium ion (Acr+-Mes) is a donor-acceptor molecule with a much longer lifetime and a higher energy electron transfer excited state than natural photosynthetic reaction centers. Unlike lucigenin with a coplanar geometry, Acr+-Mes has an orthogonal geometry. There is no π conjugation between Acr+ and Mes. Due to its special electron donor-acceptor structure, it does not rely on strong alkalinity to generate an electron transfer state like lucigenin, which makes it possible to achieve chemiluminescence (CL) under weakly alkaline or neutral conditions. In this study, we report Acr+-Mes CL for the first time. Acr+-Mes generates about 400 times stronger CL intensity than lucigenin under neutral conditions (pH = 7) using KHSO5 as the coreactant. Moreover, Co2+ can enhance Acr+-Mes/KHSO5 CL remarkably. Acr+-Mes/KHSO5 CL enables Co2+ detection with a linear range of 0.5-500 nM and a limit of detection of 28 pM (S/N = 3). This method was tested for the detection of Co2+ in lake water, and the standard recovery rate of 96.8-107% was achieved. This study provides a new way to develop efficient CL systems in neutral solutions.

2.
Anal Chem ; 95(6): 3267-3273, 2023 02 14.
Artículo en Inglés | MEDLINE | ID: mdl-36722089

RESUMEN

FeOOH nanorods, as one-dimensional nanomaterials, have been widely used in many fields due to their stable properties, low cost, and easy synthesis, but their application in the field of chemiluminescence (CL) is rarely reported. In this work, FeOOH nanorods were synthesized by a simple and environmentally friendly one-pot hydrothermal method and used for the first time as a catalyst for generating strong CL with luminol without additional oxidant. Remarkably, luminol-FeOOH exhibits about 250 times stronger CL than the luminol-H2O2 system. Its CL intensity was significantly quenched by uric acid. We established a simple, rapid, sensitive, and selective CL method for the detection of uric acid with a linear range of 20-1000 nM and a detection limit of 6.3 nM (S/N = 3). In addition, we successfully applied this method to the detection of uric acid in human serum, and the standard recoveries were 95.6-106.4%.


Asunto(s)
Luminol , Nanotubos , Humanos , Oxidorreductasas , Ácido Úrico , Peróxido de Hidrógeno , Luminiscencia , Mediciones Luminiscentes/métodos , Límite de Detección
3.
Anal Chem ; 95(2): 1747-1754, 2023 Jan 17.
Artículo en Inglés | MEDLINE | ID: mdl-36592382

RESUMEN

Metal-organic frameworks (MOFs) are ideal sensing materials due to their distinctive morphologies, high surface area, and simple calcination to remove sacrificial MOF scaffolds. Oxygen vacancies (Ovs) can be efficiently generated by the thermal annealing of metal oxides in an inert atmosphere. Herein, MIL-53-based Fe and Fe/Ni-MOFs nanorices (NRs) were first prepared by using a solvothermal method, and then one-dimensional (1D) Fe2O3 and Ni0.4Fe2.6O4 NRs were derived from the MOFs after calcination at 350 °C in an air and argon (Ar) atmosphere, respectively. It was found that Ar-annealed Ni0.4Fe2.6O4 NRs have higher Ovs concentrations (82.11%) and smaller NRs (24.3 nm) than air-annealed NRs (65.68% & 31.5 nm). Beneficially, among the synthesized NRs, the Ar-Ni0.4Fe2.6O4 NRs show a higher sensitivity to diethylamine (DEA) (Ra/Rg = 23 @ 5 ppm, 175 °C), low detection limit (Ra/Rg = 1.2 @ 200 ppb), wide dynamic response (Ra/Rg = 93.5@ 30 ppm), high stability (30 days), and faster response/recovery time (4 s/38 s). Moreover, the 1D nanostructure containing heterostructures offers excellent sensing selectivity and a wide detection range from 200 ppb to 30 ppm in the presence of DEA. The outstanding gas sensing behavior can be attributable to synergistic impact, structural advantages, high concentration of Ovs, and the heterojunction interface, which can have profound effects on gas sensor performance. This study provides a unique technique for constructing high-performance gas sensors for ppb-level DEA detection and the formation of Ovs in metal oxides without the need for any additives.

4.
Talanta ; 276: 126289, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38776779

RESUMEN

Aggregation-induced emission (AIE) has been widely used in research on electrochemiluminescence (ECL) due to its excellent luminescence intensity. In this work, copper superparticles (Cu SPs) were used to construct ECL biosensor to detect the microRNA-103a (miRNA-103a) in triple-negative breast cancer (TNBC) tumor tissues. Firstly, GSH-capped copper clusters were used as precursors to prepare Cu SPs by the AIE effect. Compared with clusters, Cu SPs possessed higher luminescence performance and energy stability, making them an ideal choice for ECL nanoprobe. The film of PVDF-HFP/CeVO4 NPs was constructed and modified with CPBA and GSH as the sensing interface (PCCG). The PCCG film displayed good conductivity and hydrophilicity, and desirable mechanical stability. Moreover, the PCCG film can induce high carrier mobility rates and dissociate large amounts of the co-reactant K2S2O8 to enhance the ECL intensity of Cu SPs. As a result, the prepared ECL sensor with the catalyzed hairpin assembly (CHA) strategy was employed to quantify miRNA-103a in the range of 100 fM to 100 nM. The biosensor provided a novel analytical approach for the clinical diagnosis of TNBC.


Asunto(s)
Técnicas Biosensibles , Cobre , MicroARNs , MicroARNs/análisis , Cobre/química , Humanos , Técnicas Biosensibles/métodos , Polivinilos/química , Mediciones Luminiscentes/métodos , Técnicas Electroquímicas/métodos , Nanopartículas del Metal/química , Límite de Detección , Neoplasias de la Mama Triple Negativas/genética
5.
Chem Commun (Camb) ; 58(73): 10214-10217, 2022 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-36000525

RESUMEN

Uniquely, thiourea dioxide not only can reduce carbonyl compounds but also generate an oxidant to trigger luminol chemiluminescence. Herein, derivatization-free carbonyl compound detection using bifunctional chemiluminescence coreactant thiourea dioxide has been developed for the first time with the second most crucial flavor benzaldehyde as a representative.


Asunto(s)
Luminiscencia , Mediciones Luminiscentes , Luminol , Tiourea/análogos & derivados
6.
Spectrochim Acta A Mol Biomol Spectrosc ; 279: 121459, 2022 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-35700613

RESUMEN

N-hydroxyphthalimide (NHPI) is an efficient organic catalyst and an important chemical raw material which can be used as an intermediate in organic synthesis of drugs and pesticides. In this study, NHPI has been used as a coreactant of lucigenin chemiluminescence (CL) for the first time. The CL of the developed system is significantly enhanced in the presence of Co2+. Therefore, we developed a novel lucigenin-NHPI CL method coupled with flow injection analysis for the sensitive, precise, and selective determination of Co2+. The linear range of this method is 1-1000 nM, and the detection limit is 67 pM (S/N = 3). In addition, this method has a good selectivity for Co2+. It has been applied to the detection of Co2+ in lake water, and the standard recovery rate is 95.9-103.2%, indicating that the method is feasible.


Asunto(s)
Acridinas , Luminiscencia , Mediciones Luminiscentes/métodos , Ftalimidas
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