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Enhanced Electrochemiluminescence of Porphyrin-based Metal-Organic Frameworks Controlled via Coordination Modulation
摘要： Precise control over composition, morphology and size of porphyrin-based metal-organic frameworks is challenging but the extension of these hybrid materials will enable the creation of novel electrochemiluminescence (ECL) emitters. The coordination of various entities are made from Zn2+ ions and meso-tetra(4-carboxyphenyl)porphine (TCPP), modulated by both solvent and bathophenanthrolinedisulfonic acid disodium salt (BPS) as capping agent, resulting in limited crystal growth of Zn-TCPP in DMF/H2O (V/V, 1:1) and the formation of nanoscale TCPP-Zn-BPS. The role of BPS is also evaluated using Zn-TCPP and BPS-Zn-TCPP as control, prepared in the absence of BPS and different coordinating sequence of ligands, respectively. The newly obtained TCPP-Zn-BPS exhibits a variety of different morphologies, as well as, spectral, and optoelectronic properties. The ECL behavior of the TCPP-Zn-BPS is investigated by using H2O2 as co-reactant. The amplification of ECL is further studied by ECL spectroscopies and cyclic voltammetry, with the corresponding mechanism proposed.
关键词： bathophenanthrolinedisulfonic acid disodium salt (BPS),Electrochemiluminescence,meso-tetra(4-carboxyphenyl)porphine (TCPP),coordination modulation
更新于2025-09-12 10:27:22
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Analysis of aqueous systems using all-inorganic perovskite CsPbBr3 quantum dots with stable electrochemiluminescence performance using a closed bipolar electrode
摘要： All-inorganic perovskite CsPbX3 (X = Cl, Br, I) quantum dots (QDs) have emerged as a new class of semiconductor nanocrystals, but the stability of CsPbX3 QDs in polar solvents is still a significant challenge. Since most targets in analytical chemistry, especially for biological detection, exist in an aqueous medium, this weakness seriously hampers practical analytical applications of CsPbX3 QDs. In this work, we introduce a closed bipolar electrode (BPE) to extend the application of perovskite QDs to aqueous systems. Based on the principle of conservation of charge in the electrode reactions at opposite ends of the BPE, the concentration of H2O2 in an aqueous medium can be detected by measuring the ECL intensity of CsPbBr3 QDs in an organic solution. Thus, for the first time, H2O2 in an aqueous system has been successfully analyzed using all-inorganic perovskite CsPbBr3 QDs with stable electrochemiluminescence performance combined with a closed bipolar electrode chip.
关键词： Bipolar electrode,Electrochemiluminescence,Perovskite,CsPbBr3 QDs
更新于2025-09-11 14:15:04
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Electrochemiluminescence of gold nanoparticles and gold nanoparticle-labelled antibodies as co-reactants
摘要： Gold nanoparticles (AuNPs) and AuNP-labelled antibodies can participate in the electrochemiluminescence (ECL) reaction of tris(2,20-bipyridyl) ruthenium(II) (Ru(bpy)3 2+) as a co-reactant. The electrochemical and spectral characteristics of this new ECL system were con?rmed by experiments, and its reaction mechanism was speculated to be di?erent from that of typical ECL. The experimental results showed that the new ECL system exhibited higher ECL e?ciency, and AuNP-labelled substances can be sensitively measured with the help of AuNPs. Based on the dual role of AuNPs as a co-reactant and marker, the AuNP–Ru(bpy)3 2+ ECL system will be a useful tool in biochemical analysis.
关键词： co-reactant,Ru(bpy)3 2+,Electrochemiluminescence,biochemical analysis,gold nanoparticles
更新于2025-09-11 14:15:04
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Biosynthesized Quantum Dot for Facile and Ultrasensitive Electrochemical and Electrochemiluminescence Immunoassay
摘要： Nanomaterials are commonly utilized for amplified immunoassay of biomarkers. However, traditional nanomaterial-based immunoassay usually requires time-consuming and labor-intensive nanoparticle modification and conjugation process, which impedes their practical applications. Here, a new immunoassay method based on biosynthesized nanomaterials is developed with versatile functions for facile and ultrasensitive detection of cancer biomarker. In this method, the utilized biosynthesized quantum dots (BQDs) allow convenient antibody conjugation and electrode modification, and demonstrate excellent electrochemical and electrochemiluminescent responses. The differential pulse voltammetric, impedance spectroscopy, and electrochemiluminescent measurements with the BQD-modified electrode show detection limits at picomolar levels as well as good specificity towards human prostate-specific antigen (PSA) detection. The inherent recognization capability as well as the inherent electrochemical and electrochemiluminescence features thus enable BQDs good candidates for facile immunosensors with high sensitivity. Such a biosynthesized nanomaterial-based approach opens up the possibility of using innovative designs for nanoparticle-based assays, and developing reliable and practical methods for early disease diagnosis.
关键词： Biosynthesized quantum dots,Immunoassay,Electrochemical,Electrochemiluminescence,Cancer biomarker
更新于2025-09-11 14:15:04
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Confined electrochemiluminescence in vertically ordered silica mesochannels for the imaging of hydrogen peroxide released from single cells
摘要： Here, the confined electrochemiluminescence (ECL) of luminol and hydrogen peroxide is achieved in vertically ordered silica mesochannels (SMCs) and applied to map the efflux of hydrogen peroxide from single living cells. The vertical alignment of SMCs on indium tin oxide (ITO) slides restricts the lateral diffusion of species generated in the ECL process. Accordingly, the cross-talk of luminescence intensity from nearby microregions is minimized for higher-spatial-resolution ECL imaging. The characterization of luminol ECL on these SMC-coated slides yields a detection range of hydrogen peroxide between 5 μM and 1 mM, providing high sensitivity in imaging the efflux of hydrogen peroxide from cells. Compared with the luminescence from individual cells on bare ITO slides, ~ 4-fold intensity is observed for SMC-coated ITO, suggesting a better electrode surface for single-cell ECL imaging.
关键词： single-cell imaging,hydrogen peroxide,silica mesochannels,confined electrochemiluminescence,luminol
更新于2025-09-10 09:29:36
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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2025-09-10 09:29:36
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Light enhanced electrochemistry and electrochemiluminescence of luminol at glassy carbon electrodes
摘要： We report in this work the enhancement effect of light irradiation on the electrochemistry and electrochemiluminescence (ECL) of luminol at the bare glassy carbon electrode (GCE). Light irradiation on the GCE surface induced the formation of hot electron-hole pairs. In alkaline solutions, hot holes can oxidize hydroxide anions to hydroxyl radicals that are capable of promoting the oxidation of luminol to generate larger current and stronger ECL. Moreover, the stability of current and ECL is also significantly improved upon light irradiation. This study provides a simple method to enhance the electrochemistry and ECL of luminol that have promise in improving the sensitivity of luminol-based chemical analysis and bioanalysis.
关键词： light irradiation,electrochemiluminescence,glassy carbon electrode,luminol,hot hole
更新于2025-09-10 09:29:36
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Single Nanostructured Gold Amalgam Microelectrode Electrochemiluminescence: From Arrays to a Single Point
摘要： Here we show a technique to prepare an array of Au nanostructured electrodes by selective co-deposition of AuxHgy with subsequent electrochemical dealloying of Hg resulting in branched microstructures with Hg free surface ≈824×greater with respect to the original area defined by lithography. We studied the kinetics of the electrochemoluminescence reaction using the Ru(bpy)3 2+ based system. The microstructured nontoxic AuxHgy can also find numerous applications in electrochemistry, especially for DNA and proteins.
关键词： array of microelectrodes,electrochemiluminescence,dealloying,single-spot observation,gold amalgam
更新于2025-09-09 09:28:46
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A Novel Solid-State Electrochemiluminescence Sensor Based on poly(3-amino-4 hydroxybenzenesulfonic acid) /Ru(bpy)32+ Modified Electrode for Determination of Malachite Green
摘要： The poly(3-amino-4-hydroxybenzenesulfonic acid)/Ru(bpy)3 2+ modified glassy carbon electrode (PAHBS/Ru(bpy)3 2+/GCE) is a novel solid-state electrochemiluminescence (ECL) sensor. It was prepared by electropolymerization of 3-amino-4-hydroxybenzenesulfonicacid (AHBS) followed by soaking into Ru(bpy)3 2+ solution. Ru(bpy)3 2+ was entrapped on the electrode via the electrostatic interactions between sulfonic acid groups and Ru(bpy)3 2+ cation. The morphology and composition of the modified electrodes were analysed using scanning electron microscope and energy-dispersed spectrum. Cyclic voltammetry and electrochemical impedance spectroscopy were used to compare the electrochemical behavior of the electrodes before and after modification. Under the optimal conditions, the ECL intensity of the quenching value (ΔECL) versus the logarithm of the concentration of malachite green (MG) was linear over a concentration range from 5.0 × 10-8 to 1.0 × 10-5 mol L-1 (r = 0.9931) and the limit of detection (LOD) was 2.5 × 10-8 mol L-1. This method has been successfully applied to the determination of MG in pond water.
关键词： Ru(bpy)3 2+,electrochemiluminescence,malachite green,sensor,3-amino-4-hydroxybenzenesulfonic acid
更新于2025-09-04 15:30:14
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Monolayer rubrene functionalized graphene-based eletrochemiluminscence biosensor for serum cystatin C detection with immunorecognition-induced 3D DNA machine
摘要： Only surficial molecules of eletrochemiluminscent (ECL) nanomaterials are the most reactive species in the typical ECL reaction. Herein, monolayer rubrene was assembled on the surface of graphene sheet to obtain monolayer rubrene functionalized graphene composite (G/mRub) with strong ECL emission by maximizing the surficial rubrene molecules. Based on G/mRub as the strong ECL emitter, an ultrasensitive “on-off” biosensor was developed to detect cystatin C (Cys C) in human serum with the help of a novel immunorecognition-induced enzyme-free 3D DNA machine. Benefiting from the strong ECL emission of G/mRub and the efficient signal amplification of 3D DNA machine, the established biosensor achieved high sensitivity for Cys C detection with linear range from 1.0 fg mL-1 to 10 ng mL-1 and limit of detection down to 0.38 fg mL-1. In addition, this enzyme-free biosensing method was adopted to successfully detect the concentration of Cys C in human serum. Therefore, the G/mRub based ECL biosensor might provide a potential tool for protein detection in clinical diagnosis and a new avenue to prepare high-performance luminescent nanomaterials.
关键词： electrochemiluminescence,graphene,cystatin C,monolayer rubrene,3D DNA machine
更新于2025-09-04 15:30:14