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Electrochemiluminescence sensing platform for ultrasensitive DNA analysis based on resonance energy transfer between graphitic carbon nitride quantum dots and gold nanoparticles
摘要： Electrogenerated chemiluminescence (ECL) of semiconductor quantum dots (QDs) is considered as a powerful technique in the fabrication of biosensor, however, the inherent toxicity of the heavy metal ion containing in QDs limits their further applications. Thus, searching for environment-friendly luminescent nanomaterials with high electrochemiluminescence (ECL) e?ciency is an urgent goal. In this work, a solid-state method under low temperature was adopted to prepare graphitic carbon nitride quantum dots (g-CNQDs). By using coreactant K2S2O8, a strong cathodic ECL signal of g-CNQDs could be observed in phosphate bu?er. A novel ECL resonance energy transfer procedure was constructed between g-CNQDs (emitter) and gold nanoparticles (acceptor). A signal probe was formed by connecting gold nanoparticles at the hairpin DNA (Hai-DNA) terminal. When the signal probe was anchored on g-CNQDs, ECL resonance energy transfer occurred due to the ECL quenching of gold nanoparticles to g-CNQDs. This phenomenon decreased the ECL signal. In the presence of target DNA (T-DNA), the looped structure of Hai-DNA could be destroyed by T-DNA, and gold nanoparticles were separated from g-CNQDs. Accordingly, the ECL resonance energy transfer procedure was hindered, and the ECL signal was recovered again. The ECL intensities exhibited linear correlation with the logarithm of T-DNA concentration from 0.02 fM to 0.1 pM, and the limit of detection was 0.01 fM (3σ). With the developed ECL resonance energy transfer system, good selectivity and high sensitivity were achieved in T-DNA detection.
关键词： Graphitic carbon nitride quantum dots,Electrochemiluminescence,DNA,Resonance energy transfer,Biosensor
更新于2025-11-14 17:04:02
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Extraction of High-Quality Quantum Dot Photocatalysts via Combination of Size Selection and Electrochemiluminescence
摘要： Quantum dots (QDs) represent one of the most promising photocatalytic systems for solar hydrogen production. Tremendous works have been devoted to the design of QDs photocatalysts, but their further development is limited by the unwanted mix of high- and low-quality QDs with different activities. With multinary Ag-In-Zn-S (AIZS) QDs as an example, here, we present a simple method for the extraction and screening of efficient photocatalysts by combination of gradient centrifugation and electrochemiluminescence (ECL). With controllable introduction of poor solvent, the crude QDs were separated into five individual samples by gradient centrifugation, from which ECL tests were performed to get the surface state information for photocatalyst screening. By the combination of size-selective centrifugation and ECL screening, we were able to get the high-activity component (AIZS-#4), which achieved 1.68 mmol·g?1 h?1, 6 times higher than that of the initial AIZS QDs. This work provides an alternative useful pathway for obtaining high-quality QD photocatalysts, beyond pursuing of perfect synthetic conditions.
关键词： size selection,electrochemiluminescence,quantum dots,photocatalysis,I-III-VI
更新于2025-11-14 15:32:45
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Hot electron-induced electrochemiluminescence at cellulose derivatives-based composite electrodes
摘要： The possibility of using cellulose derivative films as (i) insulating material on metal electrodes or (ii) in composite electrode films on metal to produce hot electron-induced electrochemiluminescence (HECL) was studied. It was shown that the luminophores known to produce HECL at thin insulating film coated cathodes (e.g. Si/SiO2 and Al2O3 electrodes) produced HECL with the present novel electrodes. In the case of composite films consisting of cellulose material doped with conducting carbon particles, the optimal cellulose/carbon black ratios were investigated by measuring the time-resolved HECL (TR-HECL) of an aromatic Tb(III) chelate. In addition to Tb(III) chelate, other well-known labels, fluorescein and Ru(bpy)3 2+ chelate, were demonstrated to produce strong HECL at the present composite electrodes, which are more environmental friendly in disposable assay cartridges as the plastic-based composites we have studied previously. Thus, it is now possible on the present basis to manufacture biodegradable paper-based assay cartridges with HECL detection of labels at biodegradable electrodes. It was shown that the present composite films are stable over wide pH range, and also time-resolved detection of Ru(bpy)3 2+ chelate is possible although its luminescence lifetime if quite short. The calibration curves were measured for presently used aromatic Tb(III) chelate and for Ru(bpy)3 2+. The detection limit (s/n = 3) was 2 · 10?10 M for the Tb(III)-chelate and 4 · 10?9 M for Ru(bpy)3 2+ in time-resolved detection mode. The relative standard deviation for Tb(III)-L1 (n = 5) emission at 10?5 M concentration was 2%. Wide linear range and low detection limits suggests that cellulose based composite electrodes can be used in HECL bioaffinity assays which was finally demonstrated here by an immunometric immunoassay.
关键词： Bioaffinity assays,Cellulose derivatives,Lanthanide electrochemiluminescence,Immunoassays,Electrochemiluminescence,Hot electron electrochemistry
更新于2025-09-23 15:23:52
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Self-electrochemiluminescence of poly[9,9-bis(3‘-(N,N- dimethyl amino)propyl)-2,7-fluorene]-alt- 2,7-(9,9- dioctylfluorene)] and resonance energy transfer to aluminum tris(8-quinolinolate)
摘要： In this paper, the electrochemiluminescence (ECL) behavior of a hole-transport polymer, poly [9,9-bis(3'-(N,N-dimethylamino) propyl)-2,7-fluorene]-alt-2,7-(9,9-dioctylfluorene)] (PFN) was examined with the purpose of finding a novel organic ECL emitter. It was found that the PFN exhibits self-electrochemiluminescence (self-ECL) without any exogenous co-reactants. Quite different from the traditional ECL, the addition of tripropyl amine (TPA) quenched the self-ECL of PFN. PFN ECL intensity reaches a peak during electrochemical oxidation process due to the superposition of self-enhanced ECL, and aggregation quenching of excited state by PFN excimer formation. Aluminum tris(8-quinolinolate) (AlQ3) doped with PFN recovers luminescence intensity with restraining quenching effect via ECL resonance energy transfer from PFN to AlQ3, giving rise to a stable luminescence signal, and hence sensory detection of nitroaromatics. The limits of detections for nitroaromatics can reach down to a level of 10^-22 M. This work sets the stage for a novel organic polymer-based ECL emitter without using any toxic exogenous co-reactant, and presents a practical avenue for a prototype of realising sensory detection through signal stabilization via energy resonance energy transfer (ERET).
关键词： poly[9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene]-alt-2,7-(9,9-dioctylfluorene),Sensor,Resonance energy transfer,Self-electrochemiluminescence
更新于2025-09-23 15:23:52
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Electrochemiluminescence sensor based on upconversion nanoparticles and oligoaniline-crosslinked gold nanoparticles imprinting recognition sites for the determination of dopamine
摘要： For the determination of dopamine (DA) in serum samples, a quenching-type electrochemiluminescence sensor was constructed in this study. Upconversion nanoparticles (UCNPs) enhanced by covalent organic frameworks (COFs)-based hybrid and oligoaniline-crosslinked gold nanoparticles (AuNPs) imprinting recognition sites were introduced in electrochemiluminescence (ECL) system at first time. The porous COFs-based hybrid with large specific surface area was modified on the electrode firstly to hold more UCNPs and imprinting recognition sites. AuNPs, here, was employed in developed sensor for two objectives: 1) AuNPs on COFs-based hybrid enabled the hybrid to tunnel the electrons, which helped to improve the ECL intensity; 2) AuNPs-based thioaniline units (PATP@AuNPs) electropolymerized on the electrode in the presence of template to form oligoaniline-crosslinked AuNPs matrix. Then the exclusion of template from matrix yielded molecularly three-dimensional imprinted contours with conductivity, conducive to specific recognition and further amplify the ECL. The double recognition mode in this work involves the recognition effect of imprinted contours and quenching effect of o-benzoquinone species. The quantum chemical calculation was performed to analyzing the possible recognition and binding mechanisms of molecularly three-dimensional imprinted contours. The results showed imprinted contours could bind the target by complementary spatial cavities and weak interactions. The proposed approach yields a wide detection range (10-14-10-6 M), low limit of detection (LOD=2×10-15 M) and acceptable recoveries (93.25%-112.97%) in rat serum sample, demonstrating that the developed method holds great promise to be applied to DA detection in practical samples.
关键词： Electroconductibility molecular imprinting polymer,Covalent organic frameworks,Oligoaniline-crosslinked gold nanoparticles,Dopamine,Electrochemiluminescence
更新于2025-09-23 15:23:52
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Electrochemiluminecence nanogears aptasensor based on MIL-53(Fe)@CdS for multiplexed detection of kanamycin and neomycin
摘要： A dual gears electrochemiluminecence (ECL) aptasensing strategy for multiple selective determination of kanamycin and neocycin was designed on the basis of the combination of kannamycin and neocycin induced dual gears conversion, the loading platform of metal-organic frameworks (MOFs), surface plasmon resonance (SPR) and ECL resonance energy transfer (ERET) between CdS QDs and AuNPs (or PtNPs). In the absence of target, the dual gears were "off". Then the B1-AuNP (gear B) and aptamer 1-PtNPs acted as signal quenching elements to quench ECL intensity due to ERET process. Upon addition of kanamycin, the aptamer 1-PtNPs were removed from the gear gradually, the ECL was enhanced due to SPR process between AuNPs and CdS QDs. After the incubation of aptamer 2, the dual gears were "off" again and ECL intensity was decreased by ERET process between AuNPs and CdS QDs. In the presence of neomycin, dual gears were "on" again, the ECL signal was enhanced by SPR process between AuNPs and CdS QDs. Under optimal condition, the proposed aptasensor exhibited wide linear ranges of kanamycin (10-10- 10-6 M) and neomycin (10-9 -10-5 M), and relatively low detection limits to kanamycin (1.7×10-11 M) and neomycin (3.5×10-10 M). The developed aptasensor realized the multiple ECL detection of kanamycin and neomycin with single luminophore, and was successfully applied to the detection of kanamycin and neomycin in food samples.
关键词： electrochemiluminecence resonance energy transfer,electrochemiluminescence,antibiotic,nanogears,surface plasmon resonance
更新于2025-09-23 15:23:52
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Miniaturized electrochemiluminescent biochip prepared on gold nanoparticles-loaded mesoporous silica film for visual detection of hydrogen peroxide released from living cells
摘要： Au nanoparticles (NPs) has been widely used for the detection of intracellular H2O2 to enhance the electron transfer process. But AuNPs are easy to aggregate in the live cells environment. Herein we report a rapid, reliable and low-cost electrochemiluminescent (ECL) biochip integrated by AuNPs-loaded mesoporous silica film (MSF) to detect H2O2 released by macrophage cells. The MSF was employed as a template to load AuNPs within the nanochannels to avoid aggregation. H2O2 could be catalyzed by AuNPs to promote the ECL reaction of luminol molecules in solution. The ECL intensity was significantly enhanced, and the peak potential was negatively shifted by 400 mV due to the excellent electrocatalytic ability of AuNPs. The integrated biochip demonstrated good reproducibility, with a wide linear range of 0.1–200 μM and an LOD of 25.3 nM. The reliability was evaluated by applying for the assessment of antioxidant activity of resveratrol using RAW 264.7 macrophage model. The AuNPs-loaded MSF integrated biochip can be easily adapted to the development of improved devices in biosensing, lab-on-a-chip, and nanofluidic systems.
关键词： Gold nanoparticles,Biochip array,Electrochemiluminescence,Reactive oxygen species,Mesoporous silica
更新于2025-09-23 15:23:52
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Fingerprints mapping and biochemical sensing on smartphone by electrochemiluminescence
摘要： Electrochemiluminescence (ECL) is a kind of optical radiation process triggered by electrochemistry, which has been one of the most important strategies in analytical chemistry and biosensing. Recently, smartphone, as one of the widely-used mobile device, has provided a attractive solution as simple yet powerful sensing platform to satisfy the needs of on-site inspection. Here, ECL on smartphone was put forward for fingerprints mapping and biochemical sensing. The smartphone-based system integrated both electrochemical excitation and optical analysis by built-in functional modules “all in one phone”. Typical enhanced luminescence analysis of nicotine, quenched luminescence analysis of trinitrotoluene (TNT) demonstrated the availability of the phone-based ECL system for biochemical sensing. Furthermore, multimode imaging analysis including color induction, gray processing, and binary extraction on smartphone were used for fingerprints mapping. The grain information of fingerprints was clearly displayed on the luminescence images, even the sweat pores on fingerprints were visible to naked eyes. Finally, in situ sensing of exogenous substances on fingerprints, such as nicotine and TNT were also accomplished by the phone. Results indicated the remarkable performances of the system in ECL, especially in the fields of biochemical sensing and imaging analysis. Because fingerprints were widely used to unlock phones, the combination of fingerprints imaging and sensing on smartphone would be contributed to the development of personal medicine, public health monitoring, and mobile care testing.
关键词： Nicotine,Smartphone,Electrochemiluminescence (ECL),Trinitrotoluene (TNT),Fingerprints mapping
更新于2025-09-23 15:23:52
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Ultrasensitive electrochemiluminescence immunosensor with wide linear range based on a multiple amplification approach
摘要： An ultrasensitive and highly selective electrochemiluminescence (ECL) immunosensor is proposed for the detection of prostate specific antigen (PSA) based on multiple amplification via glucose oxidase (GOx) and platinum nanoparticles (Pt NPs) conjugated with polyglutamic acid (PGA). The proposed immunosensor has a wide linear range (1.0 pg/mL–150 ng/mL) and low detection limit (0.6 pg/mL) for PSA detection, which is due in part to the excellent catalytic activity of the Ab2-GOx-PGA-Pt NPs probe toward the luminol ECL reaction.
关键词： Multiple amplification,Ultrasensitive,PSA,PGA,Electrochemiluminescence
更新于2025-09-23 15:23:52
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An Enzyme-free “ON-OFF” Electrochemiluminescence Biosensor for Ultrasensitive Detection of PML/RARα based on Target-Switched DNA Nanotweezer
摘要： Herein, an enzyme-free "ON-OFF" electrochemiluminescence (ECL) biosensor for ultrasensitive detection of fusion gene PML/RARα is constructed based on a simple target-switched DNA nanotweezer as hemin concentration controller. In this biosensor, the hemin concentration is primarily controlled by the conversion of "opened-closed" DNA nanotweezers and low concentration hemin is first used as electrochemically regenerable enhancer. In the absence of the target, the nanotweezers are in an opened state which lead to a low concentration of hemin in the solution, resulting in an enhanced Ru(bpy)3 2+ ECL signal. In the presence of the target, the closed nanotweezers absorbed onto the surface of electrode can capture the hemin, which achieves a high concentration of hemin and then quenches the ECL signal. The developed method achieves ultrasensitive detection of PML/RARα with a wide linear range from 1 fM to 1 nM and limit of detection as low as 0.125 fM. In addition, the ECL biosensor shows excellent specificity to the other subtypes of PML/RARα (subtype "S", "V", "PML" and "RARα"). Moreover, due to the high designable character of DNA nanotweezer, this method might provide a pragmatic Ru(bpy)3 2+ ECL platform for ultrasensitive detection of nucleic acid in the future.
关键词： Hemin,DNA nanotweezer,Enzyme-free,Electrochemiluminescence,PML/RARα
更新于2025-09-23 15:22:29