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Near-Infrared Photoluminescence and Electrochemiluminescence from a Remarkably Simple Boron Difluoride Formazanate Dye
摘要： Electrochemiluminescence involves the generation of light via electrochemical reactions and has recently shown utility for single-cell imaging. To further develop this novel imaging platform, it is necessary to produce readily available dyes that photoluminesce and electrochemiluminesce in the near-infrared region to limit absorption by biological tissue. To address this need, we prepared a boron difluoride formazanate dye that exhibits near-infrared photoluminescence in two straightforward synthetic steps. Examination of its solid-state structure suggests that the N-aryl substituents have significant quinoidal character, which narrows the S1-S0 energy gap and leads to near-infrared absorption and photoluminescence. Electrochemical properties were probed using cyclic voltammetry and revealed four electrochemically reversible waves. Electrochemiluminescence properties were examined in the presence of tri-n-propylamine, leading to maximum intensity at 910 nm, at least 85 nm (1132 cm?1) red-shifted compared to all other organic dyes. This work sets the stage for the development of future generations of dyes for emerging applications, including single-cell imaging, that require near-infrared photoluminescence and electrochemiluminescence.
关键词： NIR electrochemiluminescence,Electrochemistry,Formazanate ligands,Organic dyes,NIR photoluminescence
更新于2025-09-23 15:21:01
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Diffusion and Kinetica??Controlled Electrochemical Reactions for Improving the Performance of Solutiona??based Electrochemiluminescence Devices
摘要： Electrochemiluminescence (ECL) refers to the generation of light at an excited state owing to an electron transfer reaction between the electrochemically generated species located around the electrode. The ECL controlled by varying the potential has attracted attention for application in various fields, such as chemical analysis, immunoassay, and optoelectronic devices. Among them, ECL devices (ECLDs) have recently been considered as promising next-generation displays due to their low energy consumption, simple fabrication process, and ability to function in direct current (DC) and alternating current (AC). Most ECLDs have a single active layer, in which the ECL luminophore and electrolyte are mixed between two electrodes, acting as the anode and the cathode in a sandwich-type ECLD. Thus, the working mechanism of ECLDs differs from those of conventional light-emitting diodes (LEDs). This is due to the electrochemical system driven by the mass transfer of the mobile counter ions and luminophore present in the active layer. When external force such as current or voltage is applied to the ECLDs, the electrolyte ions acting as the mobile counter ions is redistributed to each electrode, after which the electrochemical double layers (EDLs) form at the electrode/active layer interface, leading to the generating of a high electric field. As a result, the electron transfer reaction between the electrode and the ECL luminophore occurs effectively, and an electric circuit, through which a faradaic current flows, is formed. Consequently, the redox species encounter each other in the ECLDs to form an excited state through electron exchange, followed by a self-terminating ECL. The ECL is affected both by the electron transfer rate (ko) between the ECL luminophore and electrode and by the diffusion-limited reaction associated with the mass transfer of the ECL luminophore. These factors are determined by the operational method, and the type and concentration of the electrolyte. Although several studies related to this subject have been reported, the dynamics of the electrochemical reactions involving the ko and the diffusion-limited reactions in ECLDs have not been properly elucidated.
关键词： Diffusion-limited reaction,Redox species,Electrode transfer reaction,Electrochemical reaction,Electrochemiluminescence
更新于2025-09-23 15:19:57
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A sensitive method to monitor catechol by using graphitic carbon nitride quantum dots as coreactants in Ru(bpy)32+-based electrochemiluminescent system
摘要： Graphitic carbon nitride quantum dots (g-CNQDs) with special structures have exhibited fascinating advantages over the common QDs. In this work, we report a novel Ru(bpy)3 2+/g-CNQDs electrochemiluminescence (ECL) system, and the effect of g-CNQDs on the ECL signal of Ru(bpy)3 2+ was discussed. It was found that g-CNQDs containing in proposed ECL system played an important coreactant role in ECL signal enhancement of Ru(bpy)3 2+, which was proved by electrochemical, ultraviolet, and ECL experiments. Based on the quenching effect of catechol on the ECL signal of Ru(bpy)3 2+/g-CNQDs, a quenching-based ECL system was designed for catechol determination. The ECL sensing system demonstrated high sensitivity to catechol, with a linear range from 10 nM to 2 mM and a detection limit of 2.5 nM (S/N = 3). The sensor was adopted for catechol analysis in tea samples with satisfactory results.
关键词： Detection,Ru(bpy)3 2+,Electrochemiluminescence,Graphitic carbon nitride quantum dots,Catechol
更新于2025-09-23 15:19:57
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Black phosphorus quantum dots as novel electrogenerated chemiluminescence emitters for the detection of Cu2+
摘要： For the first time, electrochemiluminescence (ECL) emission was observed from black phosphorus quantum dots (BPQDs) in the presence of K2S2O8 as the co-reactant. The potential application of BPQDs in ECL analytical chemistry was also demonstrated using Cu2+ as an example.
关键词： Cu2+ detection,black phosphorus quantum dots,electrochemiluminescence
更新于2025-09-23 15:19:57
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Development of a ZnCdS@ZnS quantum dotsa??based label-free electrochemiluminescence immunosensor for sensitive determination of aflatoxin B1 in lotus seed
摘要： In this study, we designed a ZnCdS@ZnS quantum dots (QDs)–based label-free electrochemiluminescence (ECL) immunosensor for sensitive determination of aflatoxin B1 (AFB1). A Nafion solution assembled abundant QDs on the surface of a Au electrode as ECL signal probes, with specially coupled anti-AFB1 antibodies as the capturing element. As the reduction reaction between S2O8 2? in the electrolyte and QDs on the electrode led to ECL emission, the decreased ECL signals resulting from target AFB1 in the samples were recorded for quantification. We evaluated electrochemical impedance spectroscopy and ECL measurements along each step in the construction of the proposed immunosensor. After systematic optimization of crucial parameters, the ECL immunosensor exhibited a good sensitivity, with a low detection limit of 0.01 ng/mL for AFB1 in a wide concentration range of 0.05–100 ng/mL. Testing with lotus seed samples confirmed the satisfactory selectivity, stability, and reproducibility of the developed ECL immunosensor for rapid, efficient, and sensitive detection of AFB1 at trace levels in complex matrices. This study provides a powerful and universal analytical platform for a variety of analytes that can be used in broad applications for real-time analysis, such as food and traditional Chinese medicine safety testing, environmental pollution monitoring, and disease diagnostics.
关键词： Electrochemiluminescence immunosensor,Nafion,Lotus seed,Aflatoxin B1,ZnCdS@ZnS quantum dots,Label-free
更新于2025-09-23 15:19:57
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Dual-Wavelength Electrochemiluminescence Ratiometric Biosensor for NF-?oB p50 Detection with Dimethylthiodiaminoterephthalate Fluorophore and Self-Assembled DNA Tetrahedron Nanostructures Probe
摘要： Here, we have fabricated a dual-wavelength electrochemiluminescence ratiometric biosensor based on electrochemiluminescent resonance energy transfer (ECL-RET). In this biosensor, Au nanoparticle-loaded graphitic phase carbon nitride (Au-g-C3N4) as donor, and Au-modified dimethylthiodiaminoterephthalate (TAT) analogue (Au@TAT) as acceptor are investigated for the first time. Besides, tetrahedron DNA probe is immobilized onto Au-g-C3N4 to improve the binding efficiency of transcription factor and ECL ratiometric changes on the basis of the ratio of ECL intensity of 595 nm and 460 nm are obtained through the formation of sandwich structure of DNA probe-antigen-antibody. Our biosensor achieves the assay of NF-κB p50 with a detection limit of 5.8 pM as well as high stability and specificity.
关键词： NF-κB p50,Dimethylthiodiaminoterephthalate (TAT),DNA tetrahedron nanostructures,electrochemiluminescence,ratiometric biosensor
更新于2025-09-23 15:19:57
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Photo-Controlled Thermosensitive Electrochemiluminescence Hydrogel for Isocarbophos Detection
摘要： Endowing specificity and controllability with the electrochemiluminescence (ECL) thermosensitive hydrogels is vitally crucial to expand their sensing applications. Herein, a novel photo-controlled thermosensitive electrochemiluminescence hydrogel (PT-ECL hydrogel) sensing platform with sufficient simplicity, specificity and precise controllability, for the first time, is proposed, by the integration of Ru(bpy)3 2+ derivatives (signal reporter), split aptamers (recognition unites), and Au nanorods (AuNRs) (photothermal energy converter) into the poly(N-isopropylacrylamide) (pNIPAM) matrix. In the presence of the model target isocarbophos (ICP), the conjugation of two split-aptamers initiated the ECL-Resonance Energy Transfer (ECL-RET) between the Au nanorods and the Ru(bpy)3 2+ centers. Surprisingly, under the irradiation of near-infrared (NIR) light, the photothermal effect of AuNRs prompted the shrinkage of the hydrogel, resulting in the enhancement of the ECL-RET and further ~7 times signal amplification. Consequently, the PT-ECL hydrogel sensing platform performed well for ICP detection with a low detection limit of 20 pM (S/N=3) and wide linear range from 50 pM to 4 μM, with great stability and repeatability. Obviously, the results showed that AuNRs utilized in this paper served the role as not only the ECL-RET acceptor, but also the photothermal converter to prompt the phase change of the PT-ECL hydrogel precisely and simply controlled by NIR light. Use of the proposed PT-ECL hydrogel detection scheme is a first step toward enabling a newly upgraded highly sensitive, selective hydrogel-based assays and also paving way for the application of smart photothermal reagents.
关键词： split aptamers,Au nanorods,photo-controlled,electrochemiluminescence,isocarbophos detection,thermosensitive hydrogel
更新于2025-09-23 15:19:57
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A Novel Perylene Derivative/Luminol Nanocomposite as Strong Electrochemiluminescence Emitter for Construction of Ultrasensitive MicroRNA Biosensor
摘要： In this work, an electrochemiluminescent (ECL) biosensor was constructed on the basis of amino-modified 3,4,9,10-perylenete-tracarboxylic dianhydride/luminol (PTC-NH2/Lu) nanocomposite as emitter and bipedal DNA walker signal amplification strategy for ultrasensitive detection of microRNA-21 (miRNA-21). The PTC-NH2/Lu nanocomposite was prepared as signal tag via π-π stacking molecular assembly, in which amino-modified 3,4,9,10-perylenete-tracarboxylic dianhydride (PTC-NH2) as a novel co-reaction accelerator significantly enhanced the ECL emission of luminol-H2O2 system. Moreover, target miRNA-21 triggered bipedal DNA walker was powered by toehold-mediated strand displacement reaction (TSDR) for signal amplification. Consequently, the proposed ECL biosensor achieved ultrasensitive detection of miRNA-21 with linear range from 100 aM to 100 pM and limit of detection 33 aM. Simultaneously, the biosensor was also successfully applied to detect target miRNA-21 in lysates from human cancer cells. As a result, this work constructed a new signal amplification platform, exhibiting great application potential in biomedical analysis and early clinical diagnostics.
关键词： PTC-NH2/Lu nanocomposite,electrochemiluminescence,co-reaction accelerator,π-π stacking molecular assembly,bipedal DNA walker
更新于2025-09-23 15:19:57
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Aggregation-Induced Electrochemiluminescence of Carboranyl Carbazoles in Aqueous Media
摘要： The aggregation-induced electrochemiluminescence (AIECL) of carboranyl carbazoles in aqueous media was investigated for the first time. Quantum yields, morphologies, and particle sizes were observed to determine the electrochemiluminescence (ECL) performance of these aggregated organic dots (ODs). All compounds exhibit much higher ECL stability and intensity than the carborane-free compound, demonstrating the essential role of the carboranyl motif. Moreover, the results of cyclic voltammetry (CV) suggest that redox take place at the carboranyl motif. The excited states of ODs were proposed to be generated by the mechanism of surface state transitions. More importantly, these compounds with reductive-oxidative mechanism is exclusive from other organic materials with oxidative-reductive mechanism. Our experiments and data have established the relation between AIE organic structures and ECL properties that has a strong potential for biological and diagnostic applications.
关键词： aggregation induced emission,boron cluster,organic dots,carborane,electrochemiluminescence
更新于2025-09-19 17:15:36
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The improved electrochemiluminescence behavior of glassy carbon electrode via in situ chemical bonding modification
摘要： An in situ chemical bonding method is developed for the electrochemiluminescence (ECL) modification of the oxidized glassy carbon electrode (GCEox). Bare GCE has been activated here via a fierce oxidizing etching to form GCEox. GCEox with numerous cracks and oxygen containing groups exhibits a negatively charged surface, which is tending to attract and react with the specific molecules to form chemical bonds. An ECL molecule Ru-L1 was synthesized and in situ bonded on GCEox surface to fabricate Ru-GCEox. The proposed chemical bonding modification eliminates the interface resistance to improve the electron transfer rate between Ru-L1 and the surface of GCE, which has been demonstrated by the better reversibility of Ru-GCEox than the traditional modified GCEs. The improvement of the ECL behavior of Ru-GCEox is also confirmed by its lower ECL potential than the traditional modified GCEs. Ru-GCEox is reusable to response α-naphthol with an ultrahigh sensitivity for its excellent ECL stability and scraping resistance, which decreases the consumption of Ru-L1. The successful fabrication of Ru-GCEox indicates the method of in situ chemical modification for GCEox can be applied to fabricate various glassy carbon-based sensors via coupling with various specific molecules.
关键词： ruthenium (II) complex,glassy carbon,the interfacial charge transfer,electrochemiluminescence
更新于2025-09-19 17:15:36