Electrochemiluminescence Efficiency Research Articles

A Controlled Release Aptasensor Utilizing AIE-Active MOFs as High-Efficiency ECL Nanoprobe for the Sensitive Detection of Adenosine Triphosphate.

Improving the sensitivity in electrochemiluminescence (ECL) detection systems necessitates the integration of robust ECL luminophores and efficient signal transduction. In this study, we report a novel ECL nanoprobe (Zr-MOF) that exhibits strong and stable emission by incorporating aggregation-induced emission ligands into Zr-based metal-organic frameworks (MOFs). Meanwhile, we designed a high-performance signal modulator through the implementation of a well-designed controlled release system with a self-on/off function. ZnS quantum dots (QDs) encapsulated within the cavities of aminated mesoporous silica nanoparticles (NH2-SiO2) serve as the ECL quenchers, while adenosine triphosphate (ATP) aptamers adsorbed on the surface of NH2-SiO2 through electrostatic interaction act as "gatekeepers." Based on the target-triggered ECL resonance energy transfer between Zr-MOF and ZnS QDs, we establish a coreactant-free ECL aptasensor for the sensitive detection of ATP, achieving an impressive low detection limit of 0.033 nM. This study not only demonstrates the successful combination of ECL with controlled release strategies but also opens new avenues for developing highly efficient MOFs-based ECL systems.

Pyrenecarboxaldehyde@Graphene Oxide Acted as a Highly Efficient ECL Emitter and Target-Triggered the Recyclable Cascade System as an Amplifier for Ultrasensitive APE1 Activity Detection.

Herein, pyrenecarboxaldehyde@graphene oxide (Pyc@GO) sheets with highly efficient electrochemiluminescence (ECL) as emitters were prepared by a noncovalent combination to develop a neoteric ECL biosensing platform for the ultrasensitive assessment of human apurinic/apyrimidinic endonuclease1 (APE1) activity. Impressively, the pyrenecarboxaldehyde (Pyc) molecules were able to form stable polar functional groups on the surface of GO sheets through the noncovalent π-π stacking mechanism to prevent intermolecular restacking and simultaneously generate Pyc@GO sheets. Compared with the tightly packed PAH nanocrystals, the Pyc@GO sheets significantly reduced internal filtering effects and diminished nonactivated emitters to enhance ECL intensity and achieve strong ECL emission. Furthermore, the APE1-activated initiators could trigger the recyclable cascade amplified system based on the synergistic cross-activation between catalytic hairpin assembly (CHA) and DNAzyme, which improved the signal amplification and transduction ability. Consequently, the developed ECL platform for the detection of APE1 activity displayed exceptional sensitivity with a low detection limit of 4.6 × 10-9 U·mL-1 ranging from 10-8 to 10-2 U·mL-1. Therefore, the proposed strategy holds great promise for the future development of sensitive and reliable biosensing platforms for the detection of various biomarkers.

Advanced Molecular Design for Efficient Multicolor Electrochemiluminescence and Amplified Spontaneous Emission Based on Tetra‐BF2 Complexes

AbstractAdvanced organoboron dyes, incorporating tetra‐boron difluoride (tetra‐BF2) moieties, are developed, demonstrating efficient electrochemiluminescence (ECL) emissions in the green to orange regions through direct ion annihilation. By introducing diverse alkyl modifications in the molecules, luminescence color tuning is achieved via alterations in conjugation and bending angle. A photoluminescence quantum yield of 100% in dilute solutions is successfully achieved. Notably, the introduction of alkyl groups to the methine side stabilizes the radical ionic state, resulting in a high ECL efficiency of 74% through an efficient radical‐ion annihilation pathway. The key factor is that the energy of the annihilation reaction exceeds the S1 energy required for luminescence. Spin density calculations further elucidate the substituent effects on the radical ions of complexes. Moreover, the lasing properties of these materials in the solution‐processed blend films are investigated, revealing a low amplified spontaneous emission (ASE) threshold (Eth) of 6.40 ± 0.24 µJ cm−2, which is notably lower among organic laser materials. This is attributed to their large Stokes shifts and high quantum yield. The excellent ECL and ASE performances establish these materials as a valuable addition to the existing library of organoboron dyes, offering fresh insights into the development of organic solid‐state lasers.

Porous Complex-Mediated Dual Emission of Porphyrins for the Electrochemiluminescence Bioassay.

Although porphyrins make up a promising class of electrochemiluminescence (ECL) luminophors, their aggregation-caused quenching (ACQ) characteristics lead to inferior ECL efficiency (ΦECL). Furthermore, current application of porphyrins is limited to cathodic emission. This work creatively exploited a cage-like porous complex (referred to as SWU-1) as the microreactor to recede the ACQ effect while modulating dual ECL emission of meso-tetra(4-carboxyphenyl)porphine (TCPP), which self-assembled with SWU-1 to form TCPP@SWU-1 nanocapsules (TCPP@SWU-1 NCs). As the microreactor, SWU-1 not only effectively constrained TCPP aggregation to improve electron-hole recombination efficiency but also improved stability of anion and cation radicals, thus significantly enhancing the dual emission of TCPP. Compared with TCPP aggregates, the resulting TCPP@SWU-1 NCs exhibited significantly enhanced anodic and cathodic emission, and their ΦECL was increased by 8.7-fold and 3.9-fold, respectively. Furthermore, black hole quencher-2 (BHQ2) can simultaneously quench anodic and cathodic signals. TCPP@SWU-1 NCs coupling BHQ2 conveniently achieved an ECL ratio detection of miRNA-126, and the limit of detection (S/N = 3) was 4.1 aM. This work pioneered the development of the cage-like porous complex SWU-1 as the microreactor to alleviate defects of the ACQ effect and mediate dual emission of TCPP. The coupling of dual-emitting TCPP@SWU-1 NCs and dual-function moderator BHQ2 created a novel single-luminophor-based ratio system for bioanalysis and provided a promising ECL analysis approach for miRNA-126.

Strand displacement amplification triggered 3D DNA roller assisted CRISPR/Cas12a electrochemiluminescence cascaded signal amplification for sensitive detection of Ec-16S rDNA

BackgroundEscherichia coli can cause gastrointestinal infection, urinary tract infection and other infectious diseases. Accurate detection of Escherichia coli 16S rDNA (Ec-16S rDNA) in clinical practice is of great significance for the identification and treatment of related diseases. At present, there are various types of sensors that can achieve accurate detection of Ec-16S rDNA. Electrochemiluminescence (ECL) has attracted considerable attention from researchers, which causes excellent performance in bioanalysis. Based on the previous research, it is significance to develop a novel, sensitive and efficient ECL biosensor. ResultsIn this work, an ECL biosensor for the detection of Ec-16S rDNA was constructed by integrating CRISPR/Cas12a technology with the cascade signal amplification strategy consisting of strand displacement amplification (SDA) and dual-particle three-dimensional (3D) DNA rollers. The amplification products of SDA triggered the operation of the DNA rollers, and the products generated by the DNA rollers activated CRISPR/Cas12a to cleave the signal probe, thereby realizing the change of the ECL signal. The cascade amplification strategy realized the exponential amplification of the target signal and greatly improved the sensitivity. Manganese dioxide nanoflowers (MnO2 NFs) as a co-reaction promoter effectively enhanced the ECL intensity of tin disulfide quantum dots (SnS2 QDs). A new ternary ECL system (SnS2 QDs/S2O82−/MnO2 NFs) was prepared, which made the change of ECL intensity of biosensor more significant. The proposed biosensor had a response range of 100 aM-10 nM and a detection limit of 27.29 aM (S/N = 3). Significance and noveltyHerein, the cascade signal amplification strategy formed by SDA and dual-particle 3D DNA rollers enabled the ECL biosensor to have high sensitivity and low detection limit. At the same time, the cascade signal amplification strategy was integrated with CRISPR/Cas12a to enable the biosensor to efficiently detect the target. It can provide a new idea for the detection of Ec-16S rDNA in disease diagnosis and clinical analysis.

Palladium nanospheres-embedded metal-organic frameworks to enhance the ECL efficiency of 2,6-dimethyl-8-(3-carboxyphenyl)4,4'-difluoroboradiazene in aqueous solution for ultrasensitive Cu2+ detection.

Nowadays, organic emitters suffer from insufficient electrochemiluminescence (ECL) efficiency in aqueous solutions, and their practical applications are severely restricted in the bio-sensing field. In this work, palladium nanospheres-embedded metal-organic frameworks (Pd@MOFs) were exploited to enhance the ECL efficiency of 2,6-dimethyl-8-(3-carboxyphenyl)4,4'-difluoroboradiazene (BET) prepared by a one-pot method in aqueous environment. First, the Pd@MOFs were generated via in situ reduction of Pd nanospheres anchored onto the MOFs, and fabricated by orderly coordination of palladium chloride (PdCl2) with 1,2,4,5-benzenetetramine (BTA) tetrahydrochloride. Then, the influence of protons on the ECL response of BET was studied in detail to obtain stronger ECL emission using potassium persulfate (K2S2O8) as co-reactant in aqueous environment. As a result, a 1.47-fold ECL efficiency enlargement of BET/K2S2O8 was harvested at the Pd@MOFs/GCE, where Ru(bpy)32+ behaved as a standard. Based on the fact that the ECL signals of the BET-covered Pd@MOFs modified glassy carbon electrode (simplified as BET/Pd@MOFs/GCE) can be quenched by Cu2+, the as-built ECL sensor showed a wide linear range (1.0-100.0 pM) and a limit of detection (LOD) as low as 0.12 pM. Hence, such research offers huge potential to promote the development of organic emitters in ECL biosensors and environmental monitoring.

Tunable electrochemiluminescence of TADF luminophores: manipulating efficiency and unveiling water-soluble emitters.

Thermally Activated Delayed Fluorescent (TADF) luminophores offer the potential to achieve 100% Internal Quantum Efficiency (IQE) by harvesting both singlet and triplet excitons via reverse intersystem crossing from T1 to S1. This class of molecules has therefore been embraced in the pursuit of cheaper and more efficient electrochemiluminescent (ECL) labels. The present study explores how tuning the electron-donating (D) and -accepting (A) strengths of peripheral substituents affects the ECL emission of mono- and dicyanoarene-based TADF dyes. To this end, we synthesized two series of TADF compounds, independently manipulating electron donors and acceptors by (i) halogenating electron-rich diphenylamine moieties, or (ii) mono- or di-substituting the electron-poor cyanoarene core with either fluorine or imidazole. Through a comparative analysis, we elucidate the role of each substituent in shaping the photophysics of the investigated luminophores. Despite only achieving a relative Φ ECL as high as 1.27%, this framework identifies several molecular features that boost the ECL efficiency to pave the way for designing highly efficient TADF-based ECL emitters. Ultimately, imidazole substituents are exploited as a platform for functionalization with triethylene glycol units. The resulting water-soluble TADF luminophores are characterized under conditions usual to commercial ECL bioanalysis, proving their potential as a cost-effective alternative replacement to [Ru(bpy)3]2+ in clinical diagnostic.

Supramolecular assembly-induced electrochemiluminescence enhancement of gold nanoclusters for hemoglobin detection.

Gold nanoclusters (Au NCs) with excellent optical properties and biocompatibility have become one of the most promising electrochemiluminescence (ECL) emitters. However, the low efficiency and poor stability of Au NCs restrict their applications in ECL. Herein, by supramolecular assembly of L-arginine (Arg) and 4-hydroxy-2-mercapto-6-methylpyrimidine (MTU) on the surface of Au NCs, Arg/MTU-Au NCs with enhanced ECL efficiency and stability were prepared. Compared with the MTU-stabilized Au NCs (MTU-Au NCs), the ECL efficiency of Arg/MTU-Au NCs increased by 24.8 times. As a proof-of-concept, a sensitive biosensing platform was constructed for sensitive detection of hemoglobin (Hb) in urine using Arg/MTU-Au NCs as ECL emitters. The proposed ECL detection platform provides a feasible strategy for the detection of biomarkers in urine and has broad application prospects in disease screening and clinical marker detection.

Artemisinin: a novel chiral electrochemiluminescence luminophore-assisted enantiospecific recognition and mechanism identification.

Exploring novel electrochemiluminescence (ECL) molecules with high efficiency and good stability in aqueous solutions is crucial for achieving highly sensitive detection of analytes. However, developing chiral luminophores with efficient ECL performance is still a challenge. Herein, we first uncover that artemisinin (ART), a well-known chiral antimalarial drug, features a strong ECL emission at 726 nm with the assistance of a co-reactant potassium persulfate (K2S2O8), and an ECL efficiency of 195.3%, compared to that of standard Ru(bpy)3Cl2/K2S2O8. Mechanistic studies indicate that the strong ECL signal of ART is generated when the excited state formed by the reduction of ART peroxide bonds and combination with persulfate returns to the ground state. Significantly, we found that the ECL sensor based on chiral ART could efficiently identify and detect chiral cysteine (Cys) through ECL signals, with a lower limit of detection of 3.7 nM for l-Cys. Density functional theory calculations and scanning electrochemical microscopy technology further confirm that the disparity in the ECL signals is attributed to the different affinity between chiral ART and d/l-Cys, resulting in distinct electron transfer rates. The study demonstrates a new role of ART in ECL investigation and for the first time, achieves the development of ART for the enantioselective recognition and sensitive detection of chiral substances. This will be of vital significance for ECL and chirality research.

An electrochemiluminescence device for visualized detection of lead in practical samples.

Lead (Pb2+) pollution poses a significant threat to human health due to its potential accumulation through the food chain. In response to this challenge, an array of electrochemiluminescence (ECL) devices has been developed for the accurate and visualized detection of trace Pb2+, achieving an ultra-low limit of detection (LOD) of 9.8 pg L-1. The device utilizes a Pb2+-specific aptamer DNA chain, modified on gold nanoparticles (AuNPs), to create an efficient ECL probe. The integration of this ECL probe into an indium tin oxide (ITO) substrate results in a Pb2+ specific array device. With the assistance of an up-response ECL imaging system, this setup enables the accurate and visualized determination of trace Pb2+, not only in standard solution containing interference ions, but also in practical samples of Lycium ruthenicum Murr., Glycyrrhiza uralensis and lake water. This work advances the visual detection of Pb2+ using ECL-based technology, demonstrating significant potential for enhancing food safety.

Potential-selective electrochemiluminescence of AgInS2/ZnS nanocrystals and its immunoassay application.

Potential-selective electrochemiluminescence (ECL) with tunable maximum-emission-potential ranging from 0.95 to 0.30 V is achieved using AgInS2/ZnS nanocrystals, which is promising in the design of multiplexed bioassay on commercialized ECL setups. The model system AgInS2/ZnS/N2H4 exhibits efficient ECL around 0.30 V and can be exploited for sensitive immunoassays with less electrochemical interference and crosstalk.

Combination of Ternary Electrochemiluminescence System of BNQDs/AgMOG-K2S2O8 and Electrochemiluminescence Resonance Energy Transfer Strategy for Ultrasensitive Immunoassay of Amyloid-β Protein.

In this work, based on boron nitride quantum dots (BNQDs) as energy donors and MnO2@MWCNTs-COOH as energy receptors, we designed an efficient electrochemiluminescence resonance energy transfer (ECL-RET) immunosensor for the detection of amyloid-β (Aβ42) protein, a biomarker of Alzheimer's disease (AD). First, the signal amplification of a ternary ECL system composed of BNQDs (as the ECL emitter), K2S2O8 (as the coreactant), and silver metal-organic gels (AgMOG, as the coreaction accelerator) was realized, and PDDA as stabilizer was added, a strong and stable initial ECL signal was obtained. AgMOG could not only support a large amount of BNQDs and Aβ42 capture antibody (Ab1) through Ag-N bond but also exhibit excellent ECL catalytic performance and enhance the luminescent intensity of BNQDs@PDDA-K2S2O8 system. In addition, due to the broad absorption spectrum of MnO2@MWCNTs-COOH and the extensive overlap with the ECL emission spectrum of BNQDs, the quenching probe Ab2-MnO2@MWCNTs-COOH could be introduced into the ternary system through a sandwich immune response. On this basis, the signal on-off ECL immunosensor was constructed to achieve the ultrasensitive detection of Aβ42 through signal transformation. Under the optimal conditions, the prepared ECL biosensor manifested a wide linear range (10 fg/mL-100 ng/mL) with a detection limit of 2.89 fg/mL and showed excellent stability, selectivity, and repeatability, which provided an effective strategy for the ultrasensitive detection of biomarkers in clinical analysis.

Tungsten-based polyoxometalate nanoclusters with remarkable reactive oxygen species-scavenging activity efficiently quenched luminol-based electrochemiluminescence for sensitive detection of Her-2.

This study aimed to develop a quenching-type electrochemiluminescence (ECL) immunosensor for human epidermal growth factor receptor (Her-2) detection. Firstly, Pd/NiFeOx nanoflowers decorated by in situ formation of gold nanoparticles (Au NPs) and 2D Ti3C2 MXene nanosheets were synthesized (AuPd/NiFeOx/Ti3C2) as carriers to load luminol and primary antibodies. Impressively, AuPd/NiFeOx/Ti3C2 with excellent peroxidase-like activity could accelerate the decomposition of the coreactant H2O2 generating more reactive oxygen species (ROSs) under the working potential from 0 to 0.8V, resulting in highly efficient ECL emission at 435-nm wavelengths. Theintroduction of tungsten-based polyoxometalate nanoclusters (W-POM NCs) which exhibit remarkable ROSs-scavenging activity as secondary antibody labels could improve the sensitivity of immunosensors. TheZnO nanoflowers were employed to encapsulate minute-sized W-POM NCs, and polydopamine was self-polymerized on the surface of Zn(W-POM)O to anchor secondary antibodies. The mechanism of the quenching strategy was explored and it was foundthat W-POM NCs could consume ROSs by the redox reaction of W5+ resulting in W6+. The proposed ECL immunosensor displayed a wide linear response range of 0.1pg·mL-1 to 50ng·mL-1, and a low detection limit of 0.036pgmL-1 (S/N = 3). The recoveries ranged from 93.9 to 99.4%, and the relative standard deviation (RSD) was lower than 10%. This finding is promising for the design of detecting new protein biomarkers.

Self-enhanced Electrochemiluminescence Luminophore Based on Pd Nanocluster-Anchored Metal Organic Frameworks via Ion Annihilation for Sensitive Cell Assay of Human Lung Cancer.

Electrochemiluminescence (ECL) has attracted significant interest in the analysis of cancer cells, where the ruthenium(II)-based emitter demonstrates urgency and feasibility to improve the ECL efficiency. In this work, the self-enhanced ECL luminophore was prepared by covalent anchoring of Pd nanoclusters on aminated metal organic frameworks (Pd NCs@MOFs), followed by linkage with bis(2,2'-bipyridine)-5-amino-1,10-phenanthroline ruthenium(II) (RuP). The resultant luminophore showed 214-fold self-magnification in the ECL efficiency over RuP alone, combined by promoting the interfacial photoelectron transfer. The enhanced mechanism through ion annihilation was critically proved by controlled experiments and density functional theory (DFT) calculations. Based on the above, a "signal off" ECL biosensor was built by assembly of tyrosine kinase 7 (PTK-7) aptamer (Apt) on the established sensing platform for analysis of human lung cancer cells (A549). The built sensor showed a lower detection limit of 8 cells mL-1, achieving the single-cell detection. This work reported a self-enhanced strategy for synthesis of advanced ECL emitters, combined by exploring the ECL biosensing devices in the single-cell analysis of cancers.

Ternary electrochemiluminescence quenching effects of CuFe2O4@PDA-MB towards self-enhanced Ru(dcbpy)32+ functionalized 2D metal-organic layer and application in carcinoembryonic antigen immunosensing

BackgroundCarcinoembryonic antigen (CEA) is a significant glycosylated protein, and the unusual expression of CEA in human serum is used as a tumor marker in the clinical diagnosis of many cancers. Although scientists have reported many ways to detect CEA in recent years, such as electrochemistry, photoelectrochemistry, and fluorescence, their operation is complex and sensitivity is average. Therefore, finding a convenient method to accurately detect CEA is significance for the prevention of malignant tumors. With high sensitivity, quick reaction, and low background, electrochemiluminescence (ECL) has emerged as an essential method for the detection of tumor markers in blood. ResultsIn this work, a “signal on-off” ECL immunosensor for sensitive analysis of CEA ground on the ternary extinction effects of CuFe2O4@PDA-MB towards a self-enhanced Ru(dcbpy)32+ functionalized metal-organic layer [(Hf)MOL-Ru-PEI-Pd] was prepared. The high ECL efficiency of (Hf)MOL-Ru-PEI-Pd originated from the dual intramolecular self-catalysis, including intramolecular co-reaction between polyethylenimine (PEI) and Ru(dcbpy)32+. At the same time, loading Pd NPs onto (Hf)MOL-Ru-PEI could not only improve the electron transfer ability of (Hf)MOL-Ru-PEI, but also provide more active sites for the reaction of Ru(dcbpy)32+ and PEI. In the presence of CEA, CuFe2O4@PDA-MB-Ab2 efficiently quenches the excited states of (Hf)MOL-Ru-PEI-Pd by PDA, Cu2+, and methylene blue (MB) via energy and electron transfer, leading to an ECL signal decrease. Under optimal conditions, the proposed CEA sensing strategy showed satisfactory properties ranging from 0.1 pg mL−1 to 100 ng mL−1 with a detection limit of 20 fg mL−1. SignificanceThe (Hf)MOL-Ru-PEI-Pd and CuFe2O4@PDA-MB were prepared in this work might open up innovative directions to synthesize luminescence-functionalized MOLs and effective quencher. Besides, the ECL quenching mechanism of Ru(dcbpy)32+ by MB was successfully explained by the inner filter effect (ECL-IFE). At last, the proposed immunosensor exhibits excellent repeatability, stability, and selectivity, and may provide an attractive way for CEA and other disease markers determination.

Polydopamine@ZIFs with enhanced electrochemiluminescence quenching performance for mycotoxin detection

Quench-type electrochemiluminescence (ECL) immunosensors are appealing for detecting small molecule contaminants in signal-on mode, for which efficient ECL quenchers are highly desirable. Here, the classical quencher of polydopamine (PDA) was transformed into a unique structure by introducing zeolite imidazole frameworks (ZIFs). Besides the inherent energy transfer quenching effect on ECL, the resulting PDA@ZIFs exhibits a high scavenging property against electrogenerated coreactant-radicals and inhibits the formation of excited luminophore. A quench-type ECL immunosensor for ochratoxin A (OTA) was developed using the PDA@ZIFs as a quencher and the g-C3N4 as a luminophore. The immunosensor showed a good response towards the OTA with a linear range of 10.0 fg/mL–1.0 ng/mL and a detection limit of 4.8 fg/mL. Acceptable recoveries of 85.7 to 109.2 % were achieved for the detection of OTA in spiked foods. This work offers valuable insight for improving the performance of quench-typed ECL biosensors.

A dynamic electrochemiluminescence system for continuous on-line measurements based on potential stepping pulse strategy

A dynamic electrochemiluminescence (ECL) detection system combining flow injection analysis with a potential stepping pulse strategy was developed. It contains a flow injection unit that carrying the sample solution flow through a specially designed ECL detection cell continuously, ensuring the valid renew of the test solution and thus is favorable for continuous on-line measurements. This dynamic ECL analytical system based on potential stepping pulse strategy is very efficient and time-saving. Taking the ruthenium(II) tris(bipyridine) (Ru(bpy)32+)-tripropylamine (TPA) system as an example, the ECL responses to step pulse potentials and pulse period, as well as the sample flow rate were examined. Under optimized experimental parameters, the proposed protocol was further successfully applied for the continuous detection of TPA, and malachite green based on its inhibitory effect on the ECL of Ru(bpy)32+-TPA system with a limit of detection of 17.77 nM. The relative standard deviation of 97 cycles measurements was only 0.46 % under ideal conditions. The results indicate that this system could provide reproducible and reliable ECL signals. As a versatile and efficient ECL detection protocol, it has a broad prospect of application.

Synergistic Multieffect Catalytic Amplified Cathodic Electrochemiluminescence Biosensor via Target Binding-Induced Aptamer Conformational Changes for the Ultrasensitive Detection of Synthetic Cathinone.

Signal amplification is a powerful approach to increasing the detection sensitivity of electrochemiluminescence (ECL). Here, we developed synergistic multieffect catalytic strategies based on CuCo2O4 nanorod combination of Ag NPs as coreaction accelerators to fabricate an efficient covalent organic framework (PTCA-COF)-based ternary ECL biosensor. Concretely, the high redox reversibility of Co3+/Co2+ and Cu2+/Cu+ would constantly promote the decomposition of S2O82- for ECL emission. Meanwhile, the introduction of Ag NPs with excellent electrocatalytic activity further realized multiple amplification of the ECL signal. Furthermore, the good hydrogen evolution reaction (HER) ability of Ag@CuCo2O4 nanorods could accelerate the proton transmission rate of the system to amplify ECL behavior. In the presence of the target synthetic cathinone 4-chloroethcathinone (4-CEC) as the quenching ECL signal-response probe, the Ferrocene (Fc)-labeled aptamer folded into the conformationally limited stem-loop structure, bringing Fc near the ECL luminophore and resulting in quenched ECL emission. The quenching effect was connected with target-induced aptamer conformational changes and consequently reflected the target concentration. Under optimum conditions, the proposed biosensor realized a highly sensitive assay for 4-CEC with a large dynamic range from 1.0 × 10-12 to 1.0 × 10-6 g/L and a detection limit as low as 2.5 × 10-13 g/L. This study integrated multiple amplification strategies for efficient ECL enhancement, which provided a novel approach to constructing highly bioactive and sensitive sensors.

A novel and efficient electrochemiluminescence sensing strategy for the determination of trimethylamine oxide in seafood

A novel and efficient electrochemiluminescence (ECL) sensing strategy and a solid-state ECL sensor was proposed to detect trimethylamine oxide (TMAO), which is widely presented in marine species and has important physiological functions. TMAO was reduced by Fe(II)-EDTA complex to trimethylamine, acting as coreactant, to amplify the ECL response of the Ru (bpy)32+ system. To improve the detection sensitivity and efficiency, a robust solid-state ECL probe was prepared and a flow injection ECL detection system was established with a specially designed flow ECL unit, under the excitation of stepping pulse potentials. Under optimized experimental conditions, the developed ECL sensor worked well for TMAO detection in a wide linear range of 10.00 μM to 1.00 mM with a limit of detection of 3.41 μM. It was successfully applied to determine TMAO in various species of seafood samples. This work provides a promising strategy for TMAO detection.

π-conjugated polypyrene network as new electrochemiluminescence emitters: Crosslinked conjugated backbone accelerates charge transport and enhances luminescence

Herein, π-conjugated polypyrene network (CPN) was synthesized by Suzuki-Miyaura polycondensation that exhibited high electrochemiluminescence (ECL) emission. The cross-linked network structure eliminates the aggregation-induced quenching effect of pyrene through steric hindrance. On the one hand, the extended π-conjugated backbone facilitated the acceleration of charge transfer and improved the stability of free radicals in the redox process, and on the other hand, by virtue of the porous structure, the coreactant and electrolyte could diffuse rapidly and fully penetrate into the polymer interior, thus effectively improving the ECL efficiency of the CPN. In view of the excellent ECL performance, an ECL biosensor for the ultrasensitive detection of the lung cancer biomarker microRNA let-7a was constructed by using CPN as a novel ECL probe in combination with a target-triggered rolling circle amplification strategy that exhibited a linear range from 1 aM to 10 pM with a low detection limit of 0.33 aM. In a word, this work provides an effective method to improve the ECL strength of polymers and opens up new prospects for developing new ECL emitters.