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Ultrasensitive detection of protein kinase activity based on the Au NPs mediated electrochemiluminescence amplification of S2O82?–O2 system
摘要： An electrochemiluminescence (ECL) biosensor based on Au NPs enhanced ECL signal of S2O8 2?–O2 system has been constructed for ultrasensitive detection of protein kinase activity. In the presence of ATP-s and protein kinase A (PKA), Au NPs can be captured on the thoil-phosphorylated peptides modified electrode surface, generating an enhanced ECL emission of S2O8 2?–O2 system. With increasing the PKA activity, more Au NPs can be captured on the modified electrode surface, resulting in the gradually enhanced ECL intensity of S2O8 2?–O2 system. Based on the Au NPs mediated the ECL amplification of S2O8 2?–O2 system, the activity of PKA can be detected sensitively with a limit of detection of 0.0002 U/mL, which is much lower than the most sensitive method in previous reports. The good conductivity and high catalytic ability of the Au NPs are revealed to account for the enhanced sensitivity in this ECL biosensor. The ECL biosensor has been successfully used for monitoring PKA activity in biological samples and screening of protein kinase inhibition.
关键词： Protein kinase A,Electrochemiluminescence biosensor,S2O8 2?–O2 system,Inhibitor,Enhancement effect
更新于2025-09-23 15:22:29
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Dual Quenching Electrochemiluminescence Strategy Based on 3D Metal-organic Frameworks for Ultrasensitive Detection of Amyloid-β
摘要： We have proposed a dual quenching electrochemiluminescence (ECL) strategy which based on Ru(bpy)3 2+ as chromophores caged in 3D Zn-oxalate metal-organic frameworks (Ru(bpy)3 2+/Zn-oxalate MOFs) for ultrasensitive detection of amyloid-β (Aβ). The three-dimensional chromophore connectivity in Zn-oxalate MOFs provided a network for rapid excited state energy transfer migration among Ru(bpy)3 2+ units which shielded the chromophores from solvent molecules and led to a high energy Ru emission efficiency. In addition, we found that both Au nanoparticles and NiFe-based nanocube MOFs could contribute to the reduction of the ECL intensity of chromophore. And the ECL emission spectra of 3D Ru(bpy)3 2+/Zn-oxalate MOFs overlapped appropriately with the ultraviolet visible (UV-vis) absorption spectra of Au@NiFe-MOFs composites, which could trigger the resonance energy transfer (RET) behavior between Ru(bpy)3 2+/Zn-oxalate MOFs (donor) and Au@NiFe-MOFs (acceptor), achieving the dual quenching effect of Ru(bpy)3 2+ encapsulated in 3D Zn-oxalate MOFs and significantly boosting the sensitivity of the Aβ-detection immunosensor. In order to examine the clinical practicability, we have applied it to verify the content of Aβ solution ranging from 100 fg mL-1 to 50 ng mL-1 and obtained the calibration cure with high correlation coefficient, along with the low limit of detection of 13.8 fg mL-1. Above all, this work demonstrated an approach of constructing dual quenching effect ECL immunosensors in whole 3D MOFs system and its application in ECL methodology.
关键词： Ru(bpy)3 2+,Dual quenching electrochemiluminescence,Au@NiFe nanocube,3D Zn-oxalate metal-organic frameworks,Amyloid-β detection
更新于2025-09-23 15:22:29
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Signal-on Electrochemiluminescence Aptasensor for Bisphenol A based on Hybridization Chain Reaction and Electrically Heated Electrode
摘要： A simple and sensitive electrochemiluminescence (ECL) aptasensor has been developed for bisphenol A (BPA) detection. The capture DNA (CDNA) was modified on the heated indium-tin-oxide (ITO) working electrode surface firstly and then hybridized with BPA aptamer to form double strand DNA (dsDNA). The presence of target can cause the releasing of aptamer from the electrode surface since the aptamer prefers to switch its configuration to combine with BPA. Subsequently, the free CDNA will induce hybridization chain reaction (HCR) to produce long dsDNA on the electrode surface. Ru(phen)3 2+ can integrate into the grooves of dsDNA to act as an ECL reagent, thus enhanced ECL signal can be detected. The temperature control during the processes of target recognition and HCR were realized through the heated electrode instead of the bulk solution heating. Furthermore, the performance of the ECL aptasensor can be further enhanced at elevated electrode temperature. Under the optimized conditions, the ECL intensity of the system has a linear relationship with the logarithm of BPA concentration in the range of 2.0 pM-50 nM. The limit of detection (LOD) at 55 °C (electrode surface temperature) was calculated to be 1.5 pM, which was approximately 6.5-fold lower than that at 25 °C. The proposed biosensor has been applied to detect the BPA in drink samples with satisfactory results.
关键词： electrochemiluminescence,hybridization chain reaction,heated indium-tin-oxide electrode,aptamer,bisphenol A
更新于2025-09-23 15:22:29
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Investigation into the Oxygen-Involved Electrochemiluminescence of Porphyrins and Its Regulation by Peripheral Substituents/Central Metals
摘要： We provide evidence of oxygen-involved electrochemiluminescence (ECL) of metal-free porphyrins and metalloporphyrins firstly. O2?? and OH?, that are oxygen intermediates, are indispensable for the formation of excited porphyrins, which has been proven by trapping free radical strategies. The wide differences regarding emission location and mechanism between metal-free porphyrins [including meso-tetra(4-methoxyphenyl)porphine (H2TMPP), meso-tetraphenylporphyrin (H2TPP) and meso-tetra(4-carboxyphenyl)porphine (H2TCPP)] and metalloporphyrins (MTPP) depend on whether protons are present in the center of the porphin ring. Besides, the oxygen-involved ECL of porphyrins can be controlled regularly by peripheral substituents with different polarities. Because of the stretched molecular structure and the decrease in electron density around the protons located at porphin ring; electron-withdrawing groups are more conducive to protons being attacked by O2??, as well as the enhancement of porphyrins ECL. The ECL efficiency [ФECL, which is normalized with respect to Ru(bpy)3(PF6)2 (taking ФECL of Ru(bpy)3(PF6)2 = 1 )] is gradually improved from H2TMPP (ФECL = 0.16), H2TPP (ФECL = 2.20) to H2TCPP (ФECL = 3.83); and the ФECL = 4.21 of Zn(II)TPP is significantly higher than other MTPP [e.g. Co(II)TPP and Cu(II)TPP]. A deeper understanding regarding the improvement of porphyrins ECL efficiency and new application towards porphyrins-related devices can be achieved from this work.
关键词： electrochemiluminescence,oxygen intermediates,central metals,porphyrins,peripheral substituents
更新于2025-09-23 15:22:29
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Steady-state Electrochemiluminescence at Single Semiconductive Titanium Dioxide Nanoparticles for Local Sensing of Single Cells
摘要： Obtaining steady-state bright electrochemiluminescence (ECL) at single nanoparticles is crucial but challenging for the realization of the single-nanoparticle electrochemical sensing of single cells. In this work, steady-state bright ECL is implemented at single semiconductive titanium dioxide (TiO2) nanoparticles for sensing the local efflux from single living cells. Oxygen vacancies on the surface of rutile TiO2 nanoparticles have a high affinity for hydrogen peroxides that are not easily passivated upon exposure to voltage. Therefore, the steady-state adsorption of hydrogen peroxide by the TiO2 nanoparticle surface permits the continuous electrochemical generation of superoxide and hydroxyl radicals by electrons and surface-trapped holes at the nanoparticles, resulting in constant ECL under physiological conditions. This steady-state luminescence during continuous imaging is correlated with the concentration of hydrogen peroxide, leading to the local ECL visualization of hydrogen peroxide efflux from single cells. The successful local ECL imaging demonstrated herein provides an unprecedented approach to enable subcellular electroanalysis using single nanoparticles.
关键词： electrochemiluminescence,titanium dioxide,single cells,hydrogen peroxide,single nanoparticles
更新于2025-09-23 15:21:21
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Electrochemiluminescence revealing that HNO3-oxidized single-walled carbon nanotubes are essentially tubular graphene quantum dot-nanoassemblies
摘要： Graphene quantum dots (GQDs) as recently emerging 0-D graphitic nanomaterials, have attracted much attention due to their unique optical, electrical and catalytic properties. However, some properties of GQDs, such as very small size, low density, and excellent water-solubility, make it difficult to be separated and immobilized. This may limit the recycle and purification of GQDs, and thus their applications in catalysis and sensing. In this work, we prepared tubular GQD-nanoassemblies (t-GQD-NAs) by etching single-walled carbon nanotubes (SWCNTs) with concentrated HNO3. The synthesized t-GQD-NAs were characterized by TEM, SEM, XPS, Raman spectroscopy and electrochemiluminescence (ECL) in details. t-GQD-NAs were much shorter and slimmer in morphology, bore more oxygen-containing groups, and had a higher surface defect density compared with SWCNTs. t-GQD-NAs not only maintained good UV absorption property of SWCNTs but also showed strong infrared ECL emission and broad ECL spectrum, verifying that t-GQD-NAs were assembled from GQDs of various sizes and some graphene nanoribbons. This is for the first time that 0-D GQDs were reported to be assembled into 1-D tubular carbon structures. The t-GQD-NAs with abundant surface states and good ECL activity could be easily separated, purified, and immobilized, suggesting their promising applications in ECL sensing and catalysis.
关键词： Graphene quantum dots,Single-walled carbon nanotubes,Electrochemiluminescence,Tubular graphene quantum dot-nanoassemblies
更新于2025-09-23 15:21:01
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Electrochemiluminescent biosensor with DNA link for selective detection of human IgG based on steric hindrance
摘要： A highly selective DNA-based electrochemiluminescence (ECL) based biosensor is described for the detection of human IgG. It is exploiting the effect of steric hindrance that affects the strength of the ECL signal in the presence of IgG. Digoxin-linked signalling DNA was specifically bound to IgG, and this causes steric hindrance which limits the ability of DNA to hybridize with capturing DNA attached to a gold electrode. Europium (II) doped CdSe quantum dots were covalently linked to the DNA in order to generate the ECL signal. Using this steric hindrance hybridization method, the ECL signal of the biosensor were proportional to the concentration of IgG with a wide linear range and a 14 pM detection limit. Conceivably, the method can be expanded to the detection of a wide range of proteins for which homologous recognition elements are available.
关键词： Digoxin-linked signalling DNA,Electrochemiluminescence,Human IgG,Steric hindrance effects,Biosensor,Europium (II) doped CdSe quantum dots
更新于2025-09-23 15:21:01
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Paper-Based Constant Potential Electrochemiluminescence Sensing Platform with Black Phosphorus as a Luminophore Enabled by a Perovskite Solar Cell
摘要： Exploring e?cient luminophores in the electrochemiluminescence (ECL) system is highly desired to pursue a sensitive ECL sensing platform. Herein, the black phosphorus nanosheets (BP NSs) with excellent ECL properties are investigated and serve as the luminophore with the coreactant of peroxydisulfate (S2O8 2?) solution. Moreover, owing to the overlapping of emission and absorbance spectra, e?ective resonance energy transfer (RET) is realized between the BP NSs and the introduced Au nanoparticles. In order to achieve the portable and miniaturized developing trends for the paper-based ECL sensing platform, a paper-based perovskite solar cell (PSC) device is designed to act as the power source to replace the commonly utilized expensive and cumbersome electrochemical workstation. Bene?ting from that, a PSC driven paper-based constant potential ECL-RET sensing platform is constructed, thereby realizing sensitive microRNAs (miRNAs) detection. What’s more, to attain the preferable analytical performance, the duplex-speci?c nuclease (DSN) is also introduced to assist the target recycling signal ampli?cation strategy. Based on this, highly sensitive detection of miRNA-107 with a range from 0.1 pM to 15 nM is achieved by this designed sensing platform. Most importantly, this work not only pioneers a precedent for developing a high-sensitivity PSC triggered ECL sensing platform but also explores the application prospect of BP nanomaterial in the ?eld of bioanalysis.
关键词： microRNAs detection,resonance energy transfer,perovskite solar cell,black phosphorus nanosheets,electrochemiluminescence
更新于2025-09-23 15:21:01
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Auto-cleaning paper-based electrochemiluminescence biosensor coupled with binary catalysis of cubic Cu2O-Au and polyethyleneimine for quantification of Ni2+ and Hg2+
摘要： Inspired by the pop-up greeting cards, a 3D collapsible auto-cleaning paper-based electrochemiluminescence (ECL) biosensor (CAPEB) with different functions of signal collection and residual multiple cleaning, is developed for sensitive detection of Ni2+ and Hg2+ by simply regulating its 3D configurations. The multiple fluidic paths and the hollow-channel structure were firstly integrated into the paper substrate, realizing simultaneously repetitive auto-cleaning of the two working electrodes. For achieving ultrasensitive Ni2+ and Hg2+ monitoring, binary catalysis consisting of the intermolecular co-reaction (H2O2 and N-(4-Aminobutyl)-N-ethylisoluminol (ABEI)) and intramolecular catalysis (polyethyleneimine (PEI)-ABEI) were introduced. Specifically, silver nanospheres with a large specific surface area and excellent conductivity were grown on the paper working electrode and served as the sensor substrate for fixing PEI-ABEI and Ni2+-specific DNAzyme. With the assistance of DNAzyme, Cu2O-Au and ferrocene (Fc) labeled strand S2 were immobilized on electrode surface through the hybridization reaction, and catalyzed H2O2 to generate reactive oxygen species, promoting the luminescence of ABEI. In the existence of Ni2+, DNAzyme was activated followed by cleavage of strand S2 to induce the release of Fc, which quenched the ECL signal of ABEI, eventually realizing the detection of Ni2+. Similarly, for sensitive quantification of Hg2+, full thymine (T) bases strand S3 was modified on surface of Cu2O-Au and anchored Hg2+ by T-Hg2+-T pairing interaction. The ECL intensity was decreased along with increasing of Hg2+ due to the quenching effect of Hg2+ on ECL emission of ABEI. Based on this ingenious system, the detection of Ni2+ and Hg2+ had high sensitivity, wide linear ranges, and low detection limits. The results indicated that the integration of a multi-channel structure into a paper device chips opened new opportunities for designing promising paper-based devices for metal ions diagnosis.
关键词： electrochemiluminescence,N-(4-Aminobutyl)-N-ethylisoluminol,auto-cleaning,Cu2O-Au,paper-based device,heavy metal ion
更新于2025-09-23 15:21:01
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Dynamic Interplay between Transport and Reaction Kinetics of Luminophores on the Operation of AC-driven Electrochemiluminescence Devices
摘要： Electrochemiluminescence (ECL) involves light emission accompanied by a series of electrochemical processes on luminophores, which has been recently exploited in a new light-emitting device platform, referred to as the ECL device (ECLD). Here, we investigate the influence of the transport of the ECL luminophores and their reaction kinetics on the emission properties of AC-voltage-driven ECLDs. A model based on the diffusion and reaction rate equations is developed to predict the operational frequency (f)-dependent luminance properties of the ECLD. It is found that more frequent generation of the redox precursors with a shorter time interval enhances their probability of encountering each other, and therefore, the luminance of the device increases with increasing f initially. The luminance at a higher f, however, is suppressed eventually due to the decreased rate of the electrode reactions. Using the model, the influence of diffusion and reaction rates on the performance of an ECLD is analyzed separately and systematically. The results provide insight on the operation of this emerging class of light-emitting device platform.
关键词： electrochemiluminescence,ionic transition metal complex,reaction kinetics,mass transport,ionic liquid,light-emitting device
更新于2025-09-23 15:21:01