Electrochemiluminescence Biosensor Research Articles

Facile and portable multimodal sensing platform driven by photothermal-controlled release system for biomarker detection

Portable, maneuverable and reliable versatile-integrated analytical devices are urgently demanded but still extremely challenging to meet the requirements of point-of-care testing in resource-limited areas. Herein, a multifunctional sensing platform with excellent photothermal performance was implanted into the miniature zone of a paper-based electrochemiluminescent (ECL) biosensor for accurate detection of interleukin-6, which could flexibly interconnect the visualized distance and temperature readout with ultrasensitive ECL response. Concretely, the multipurpose MBene and TaSe2 composites (MBene@TaSe2) prepared via self-assembly approach as target-associated photothermal element was introduced in the paper-based analytical device (PAD) and served as multi-signals trigger. Under the laser irradiation, MBene@TaSe2 probe not only generated heat for rapid temperature output, but also triggered the phase transition behavior of thermoresponsive poly (N-isopropylacrylamide) (pNIPAM) hydrogel to release loaded malachite green (MG) dye for distance-based visual readout. Simultaneously, the released MG was also utilized as effective quencher to decrease the ECL signal of luminol. Benefitting from this dexterous architecture, the speedy preliminary screening and precise quantitative analysis could be subsequently obtained in single-drop sample through one-step sandwich immunoreaction, which avoids additional separation operations and greatly simplifies the analysis procedure. Undeniably, this work provides ingenious insights for advancing the development of convenient and fast multifunction-integrated PAD in family surveillance and intelligent diagnosis.

Electrochemiluminescence Biosensor for Estrogen-Related Receptor Alpha (ERRα) Based on Target-Induced Change of the Steric Hindrance Effect of an Antibody-Modified Electrode.

In this work, a simple and sensitive electrochemiluminescence (ECL) biosensor has been devised based on target-induced steric hindrance of an antibody-modified electrode surface. Estrogen-related receptor alpha (ERRα) is closely related to estrogen-dependent tumors, which had been chosen as a model target. The ERRα antigen can bind to the antibody modified on the electrode surface with high specificity and results in the increase of steric hindrance, which prevented the ECL indicators (tris(2,2'-bipyridine) dichlororuthenium(II) hexahydrate) from approaching the electrode surface, and the ECL intensity of the system decreased. The ECL response of the system has a good linear relationship with ERRα concentration in the range of 1.0-60 ng/L, and the limit of detection is 0.5 ng/L. Different from the traditional sandwiched immune ECL detection system, which need the modification of ECL indicators on the secondary antibody, only one antibody had been used in this system. The system is easy to operate and has good sensitivity. The designed biosensor has been applied to detect ERRα in the serum and different cell line samples with satisfied results.

Enhancing effect of black phosphorus quantum dots on electrochemiluminescence of Ir(dF(CF3)ppy)2(bpy) in ionic liquid medium and its sensing application

Room temperature ionic liquids are increasingly used in electrochemical measurement because of their excellent properties. In the present work, a strong anodic electrochemiluminescence (ECL) of one kind of water insoluble iridium complex (Ir(dF(CF3)ppy)2(bpy)) was obtained in ionic liquid medium through immobilizing it onto the electrode via solvent evaporation method. Black phosphorus quantum dots (BPQDs) could not only enhance the anodic ECL, but also generate a new anodic ECL at lower potential. The spectral investigation indicated that BPQDs could interact with Ir(dF(CF3)ppy)2(bpy) to enhance ECL signal and induce new ECL. Dopamine could compete with Ir complex to interact with BPQDs, which exhibited apparent inhibiting effect on ECL emission. As a result, dopamine was sensitively detected in the range of 0.1 nM to 0.1 μM with a detection limit of 3.76 × 10−11 mol L−1. The present work revealed that iridium complex ECL could be obtained in ionic liquids, which provided new avenue for the fabrication of ECL biosensor.

High-Density N-Vacancy-Induced Multipath Electrochemiluminescence Improvement of 3D g-C3N4 for Ultrasensitive MiRNA-222 Analysis

Using dissolved O2 as the cathodic co-reactant of three-dimensional (3D) g-C3N4 is a convenient method to improve the electrochemiluminescence (ECL) signal, but it still suffers the disadvantages of limited luminous efficiency of 3D g-C3N4 and low content, low reactivity, and instability of dissolved O2. Here, N vacancy with high density was first introduced into the structure of 3D g-C3N4 (3D g-C3N4-NV), which could conveniently realize multipath ECL improvement by simultaneously solving the above shortcomings effectively. Specifically, N vacancy could change the electronic structure of 3D g-C3N4 to broaden its band gap, increase fluorescence (FL) lifetime, and accelerate electron transfer rate, obviously improving the luminous efficiency of 3D g-C3N4. Meanwhile, N vacancy made the excitation potential of 3D g-C3N4-NV to shift from -1.3 to -0.6 V, effectively weakening the electrode passivation. Moreover, the adsorption capacity of 3D g-C3N4-NV was obviously enhanced, which could make the dissolved O2 enrich around 3D g-C3N4-NV. And massive active NV sites of 3D g-C3N4-NV could promote O2 to more efficiently convert to reactive oxygen species (ROS) that were key intermediates in ECL generation. Using the newly proposed 3D g-C3N4-NV-dissolved O2 system as an ECL emitter, an ultrasensitive target conversion biosensor was constructed for miRNA-222 detection. The fabricated ECL biosensor exhibited satisfactory analytical performance for miRNA-222 with a detection limit of 16.6 aM. The strategy achieved multipath ECL improvement by introducing high-density N vacancy simply in the 3D structure of g-C3N4 and could open a new horizon for developing a high-performance ECL system.

Regulation of Target-activated CRISPR/Cas12a on Surface Binding of Polymer Dots for Sensitive Electrochemiluminescence DNA Analysis.

Polymer dots (Pdots) have emerged as a type of attractive electrochemiluminescence (ECL) emitter. However, the low ECL efficiency severely limits their practicability. In this work, we develop a sensitive ECL biosensing strategy for the detection of human papilloma virus subtype (HPV-16) DNA by using target-activated CRISPR/Cas12a to regulate the binding of Pdots-DNA to biosensor and local surface plasmon resonance (LSPR) effect of electrochemically deposited Au nanoparticles (depAuNPs) to enhance the ECL emission of Pdots bound on biosensor. The biosensor is prepared by simply assembling hairpin DNA on depAuNPs modified electrode. In the presence of target DNA, the designed specific CRISPR/Cas12a can be activated to digest single-stranded assistant DNA, which decreases the amount of hairpin DNA opened by assistant DNA to bind Pdots-DNA on the biosensor surface, thus reduces the ECL emission. The integration of target DNA-triggered catalysis and the LSPR effect of depAuNPs greatly improves the sensitivity of ECL analysis. Using HPV-16 DNA as a target model, the proposed method shows a limit of detection (LOD) of 3.2 fM at a signal-to-noise ratio of 3 and a detectable concentration range of 5.0 fM to 50 pM. The high sensitivity, excellent selectivity, good testing stability, and acceptable fabrication reproducibility of the designed ECL biosensing strategy demonstrate its potential application in DNA bioanalysis.

High-efficiency interparticle DNA walker amplifier combined with N-Ti3C2 quantum dots as electrochemiluminescence emitters for sensitive protein assay

In this work, an electrochemiluminescence (ECL) biosensor based on interparticle DNA walker as effective signal amplification strategy and N-Ti3C2 QDs as high-efficiency emitters was designed for sensitive assay of mucin 1 (MUC1), which is closely related to the occurrence and development of tumors. First, an interparticle DNA walker which contains walking particles (WPs) and orbit particles (OPs) was fabricated. In the presence of target MUC1 and DNAzyme, the WPs can walk along the surface of OPs, and they can continue to walk along next OPs after completing previous walk. As the moving freedom and area improved, the interparticle DNA walker could effectively improve the conversion efficiency of target. Furthermore, N-Ti3C2 QDs with high ECL luminous efficiency were synthesized by using polyethyleneimine (PEI) as nitrogen source. Due to the nitrogen-rich of PEI, the relative ECL quantum efficiency of the proposed N-Ti3C2 QDs was calculated to be 1.5 times higher than our previous reported N-Ti3C2 QDs that utilizing ethylenediamine as nitrogen source. Therefore, taking the advantage of the improved moving freedom and area of the interparticle DNA walker and high ECL efficiency of the proposed N-Ti3C2 QDs, the fabricated ECL biosensor for MUC1 determination displayed a low detection limit with a wide linear range, which provides a potential feasible method for other protein sensitive assay.

Nitrogen-, Sulfur-, and Fluorine-Codoped Carbon Dots with Low Excitation Potential and High Electrochemiluminescence Efficiency for Sensitive Detection of Matrix Metalloproteinase-2.

In this study, nitrogen-, sulfur-, and fluorine-codoped carbon dots (NSF-CDs) with high electrochemiluminescence (ECL) efficiency were developed as novel emitters to fabricate an ECL biosensor for sensitive detection of matrix metalloproteinase 2 (MMP-2). Impressively, compared to previously reported CDs, NSF-CDs with narrow band gap not only decreased the excitation voltage to reduce the side reaction and the damage on biomolecules but also had hydrogen bonds to vastly enhance the ECL efficiency. Furthermore, an improved exonuclease III (Exo III)-assisted nucleic acid amplification method was established to convert trace MMP-2 into a mass of output DNA, which greatly improved the target conversion efficiency and ECL signal. Hence, the ECL biosensor has realized the sensitive detection of MMP-2 proteins from 10 fg/mL to 10 ng/mL with a limit of detection of 6.83 fg/mL and has been successfully applied in the detection of MMP-2 from Hela and MCF-7 cancer cells. This strategy offered neoteric CDs as ECL emitters for sensitive testing of biomarkers in medical research.

Aggregation-Induced Electrochemiluminescence Based on a Zinc-Based Metal-Organic Framework and a Double Quencher Au@UiO-66-NH2 for the Sensitive Detection of Amyloid β 42 via Resonance Energy Transfer.

A novel sandwich electrochemiluminescence (ECL) biosensor based on aggregation-induced electrochemiluminescence resonance energy transfer (AIECL-RET) was designed for the sensitive detection of amyloid β42 (Aβ42). The synthesized silver nanoparticle-functionalized zinc metal-organic framework (Ag@ZnPTC) and gold nanoparticle-functionalized zirconium organic framework (Au@UiO-66-NH2) were used as the ECL donor and acceptor, respectively. AgNPs were generated in situ on the surface of ZnPTC, which further improved the ECL intensity and the loading of antibody 1 (Ab1). Under the optimized experimental conditions, the linear detection range of Aβ42 concentration was 10 fg/mL to 100 ng/mL, and the detection limit was 2.4 fg/mL (S/N = 3). The recoveries of Aβ42 were 99.5-104%. The method has good stability, repeatability, and specificity. Ag@ZnPTC/Au@UiO-66-NH2 provides an assay for the sensitive detection of disease biomarkers.

Self-assembly Induced Enhanced Electrochemiluminescence of Copper Nanoclusters Using DNA Nanoribbon Templates.

Copper nanoclusters (CuNCs) are attractive electrochemiluminescence (ECL) emitters as Cu is comparatively inexpensive, nontoxic, and highly abundant. However, their ECL yield is relatively low. Herein, we report that orderly self-assembly of CuNCs using DNA nanoribbon as the template (DNR/CuNCs) conferred the CuNCs with improved ECL properties compared with individual CuNCs in both annihilation and co-reactant processes. The DNR/CuNCs resulted in a high ECL yield of 46.8 % in K2 S2 O8 , which was ≈68 times higher than that of individual CuNCs. This strategy was successfully extended to other ECL emitters, such as gold nanoclusters and the Ru(bpy)3 2+ /TPrA system. Furthermore, as an application of DNR/CuNCs, a DNR/CuNC-based ECL biosensor with higher sensitivity was constructed for dopamine determination (two orders of magnitude lower than that previously reported), showing that DNR/CuNCs have a potential for application in ECL bioanalysis as a new type of superior luminophore candidate.

Self‐assembly Induced Enhanced Electrochemiluminescence of Copper Nanoclusters Using DNA Nanoribbon Templates

AbstractCopper nanoclusters (CuNCs) are attractive electrochemiluminescence (ECL) emitters as Cu is comparatively inexpensive, nontoxic, and highly abundant. However, their ECL yield is relatively low. Herein, we report that orderly self‐assembly of CuNCs using DNA nanoribbon as the template (DNR/CuNCs) conferred the CuNCs with improved ECL properties compared with individual CuNCs in both annihilation and co‐reactant processes. The DNR/CuNCs resulted in a high ECL yield of 46.8 % in K2S2O8, which was ≈68 times higher than that of individual CuNCs. This strategy was successfully extended to other ECL emitters, such as gold nanoclusters and the Ru(bpy)32+/TPrA system. Furthermore, as an application of DNR/CuNCs, a DNR/CuNC‐based ECL biosensor with higher sensitivity was constructed for dopamine determination (two orders of magnitude lower than that previously reported), showing that DNR/CuNCs have a potential for application in ECL bioanalysis as a new type of superior luminophore candidate.

Facile synthesis of 2D Europium-metal organic frameworks nanosheets for highly efficient electrochemiluminescence in DNA detection

Lanthanide metal organic frameworks (Ln-MOFs) with self-luminous behavior are considered promising emitters of electrochemiluminescence (ECL) due to their unique antenna effects. In this study, the novel 2D Europium-metal organic frameworks (Eu-MOFs) nanosheets were synthesized by simply blending 1, 10-phenanthroline-2, 9-dicarboxylic acid (PDA) and Eu salts at room temperature. When N, N-diethylethylenediamine (DEAEA) was used as the efficient co-reactant, the 2D Eu-MOFs exhibited stronger and steadier ECL performance compared with 2D Europium-metal organic gels (Eu-MOGs) synthesized using similar steps, due to their rigid skeletons and higher crystalline degree, which facilitated electron transfer. In addition, we designed a switching mode ECL biosensor, which was combined with an exonuclease-assisted DNA walker cycling signal amplification strategy, enabled the ultra-sensitive detection of the I27L gene, which was significantly associated with an increased risk of maturity-onset diabetes of the young (MODY). When the target DNA was present, DNA walker recycle amplification occurred driven by exonuclease III (Exo III). Subsequently, the ECL intensity of the system was reduced by introducing the ferrocene-labeled probe (H2-Fc) as a signal quencher. Under the optimal experimental conditions, a wide detection linear range of the target DNA was observed from 1 fM to 10 nM with a low detection limit of 447 aM. This research provided new possibilities for a gentle and simple method to obtain 2D MOFs with stable ECL signals for the sensitive detection of specific DNA sequences.

A Study of the Detection of SARS-CoV-2 by the Use of Electrochemiluminescent Biosensor Based on Asymmetric Polymerase Chain Reaction Amplification Strategy.

A new and reliable method has been constructed for detecting severe acute respiratory syndrome coronavirus type 2 (SARS-CoV-2) open reading frames 1ab (ORF1ab) gene via highly sensitive electrochemiluminescence (ECL) biosensor technology based on highly efficient asymmetric polymerase chain reaction (asymmetric PCR) amplification strategy. This method uses magnetic particles coupled with biotin-labeled one complementary nucleic acid sequence of the SARS-CoV-2 ORF1ab gene as the magnetic capture probes, and [Formula: see text]-labeled amino-modified another complementary nucleic acid sequence as the luminescent probes, and then a detection model of magnetic capture probes-asymmetric PCR amplification nucleic acid products-[Formula: see text]-labeled luminescent probes is formed, which combines the advantages of highly efficient asymmetric PCR amplification strategy and highly sensitive ECL biosensor technology, enhancing the method sensitivity of detecting the SARS-CoV-2 ORF1ab gene. The method enables the rapid and sensitive detection of the ORF1ab gene and has a linear range of 1-[Formula: see text] copies/[Formula: see text], a regression equation of [Formula: see text] = [Formula: see text] + 2919.301 ([Formula: see text] = 0.9983, [Formula: see text] = 7), and a limit of detection (LOD) of 1 copy/[Formula: see text]. In summary, it can meet the analytical requirements for simulated saliva and urine samples and has the benefits of easy operation, reasonable reproducibility, high sensitivity, and anti-interference abilities, which can provide a reference for developing efficient field detection methods for SARS-CoV-2.

Versatile FeMoOv nanozyme bipolar electrode electrochemiluminescence biosensing and imaging platform for detection of H2O2 and PSA

In this work, a unique FeMoOv nanozyme-bipolar electrode (NM-BPE) electrochemiluminescence (ECL) biosensing and imaging platform was proposed for the first time to realize sensitive detection of target hydrogen peroxide (H2O2) and prostate specific antigen (PSA). Considering the advantage that the cathode and anode poles of the bipolar electrode (BPE) can be modified respectively, this work was carried out using anode equipped with ECL reagent bipyridine ruthenium (Ru(bpy)32+), and cathode equipped with the Fe-doped molybdenum oxide/Au nanoparticles (FeMoOv/AuNPs) with excellent peroxidase (POD) and catalase (CAT)-like activity. Because FeMoOv/AuNPs show efficient enzyme catalysis effect and can greatly promote the decomposition of H2O2, thus the electron transfer rate in the NM-BPE system would be much accelerated to enhance the ECL signal of Ru(bpy)32+. Based on this principle, this work not only realized sensitive detection of H2O2, but also ingeniously designed an sandwich immunosensor using FeMoOv/AuNPs as recognition probe to mediate the ECL response on the anode, achieving highly sensitive detection of PSA. Furthermore, a unique mobile phone ECL imaging system was developed for assay of PSA at different concentrations, which opened a new portable imaging sensing device for bioassays. This work was the first time to combine nanozymes with bipolar electrodes for ECL analysis and imaging, which not only broadened the applications of nanozymes, but also pioneered the new joint ECL research technique of bipolar electrode and ECL imaging in bioassays, showing great application prospect for multiple detection of proteins, nucleic acids and cancer cells.

Aggregation-Induced Enhancement Electrochemiluminescence of Ag Nanoribbons as a Signal Probe for Ultrasensitive Detection of the Halogenase Gene Segment from Aspergillus Ochratoxin.

Here, an electrochemiluminescence (ECL) biosensor was developed based on aggregation-induced enhancement ECL of Ag nanoribbons (Ag NRs) as a signal probe and the mismatched bases-fueled DNA walker as the amplification strategy for ultrasensitive detection of the halogenase gene segment (target) from aspergillus ochratoxin to evaluate fungi capable of producing ochratoxin in dairy products. Compared with the existing agminated NCs, the Ag NRs displayed dramatically enhanced ECL emission due to effective electron transfer and less energy dissipation of excited-state Ag NRs based on the metallophilic interaction of Ag(I)-Ag(I). Impressively, the target was conversed mismatched bases-DNA walker to trigger a significant ECL response through toehold-mediated strand displacement amplification. Thus, the strategy realized trace analysis of the halogenase gene segment with a detection limit of 45 aM, which ushered a new detection method for toxin determination in the previous stage of toxin biosynthesis to protect people from toxic damage.

Highly Efficient Wavelength-Resolved Electrochemiluminescence of Carbon Nitride Films for Ultrasensitive Multiplex MicroRNA Detection.

The development of electrochemiluminescence (ECL) emitters of different colors with high ECL efficiency (ΦECL) is appealing yet challenging for ultrasensitive multiplexed bioassays. Herein, we report the synthesis of highly efficient polymeric carbon nitride (CN) films with fine-tuned ECL emission from blue to green (410, 450, 470, and 525 nm) using the precursor crystallization method. More importantly, naked eye-observable and significantly enhanced ECL emission was achieved, and the cathodic ΦECL values were ca. 112, 394, 353, and 251 times those of the aqueous Ru(bpy)3Cl2/K2S2O8 reference. Mechanism studies showed that the density of surface-trapped electrons, the associated nonradiative decay pathways, and electron-hole recombination kinetics were crucial factors for the high ΦECL of CN. Based on high ΦECL and different colors of ECL emission, the wavelength-resolved multiplexing ECL biosensor was constructed to simultaneously detect miRNA-21 and miRNA-141 with superior low detection limits of 0.13 fM and 25.17 aM, respectively. This work provides a facile method to synthesize wavelength-resolved ECL emitters based on metal-free CN polymers with high ΦECL for multiplexed bioassays.

Chelating and pendant dual-antenna effect modulated ratiometric electrochemiluminescence system for lung cancer marker assay

Electrochemiluminescence of lanthanide coordination polymers (LCPs) has drawn researchers' torrential interest attributed to their congenital standout optical properties. Herein, a novel electrochemiluminescent (ECL) emitter LCPs Tb-norfloxacin (Tb-NFX) was firstly reported, which originated from that NFX transferred excited state energy to Tb3+ by chelating antenna effect. Moreover, a creative ratiometric ECL biosensor was established based on an emerging pendant antenna effect mechanism between luminol and Tb-NFX. Specifically, Tb-NFX was immobilized on the electrode surface and SiO2 nanostars@luminol was introduced onto the immunosensor by the sandwich-typed immunoassay. In view of this, the luminol transferred energy to the Tb-NFX and potential resolved ratiometric strategy was implemented for self-calibrated assay target. This work innovatively demonstrates that the development of new ECL luminophores through chelating antenna effect and the establishment of a dual-potential ECL ratio measurement strategy powered by pendant antenna effect are feasible, further extending the application of LCPs in ECL immunoassays and provides new directions for the construction of ECL ratio pairs.

Controlled Growth of MoS2 on Dendritic Ferric Oxide to Enhance Electrochemiluminescence of Nitrogen-Doped Carbon Quantum Dots for Sensitive Immunoassay.

The essential expansion of electrochemiluminescence (ECL) technology into clinical detection relies on sensitive and stable signal and maintenance of the activity of the immune molecules during the analysis. This poses a critical challenge for an ECL biosensor as a luminophore in general requires high potential excitation resulting in a strong ECL signal; nevertheless, it has an irreversible effect on the activity of the antigen or antibody. Herein, a novel electrochemiluminescence (ECL) biosensor utilizing nitrogen-doped carbon quantum dots (N-CQDs) as emitters and molybdenum sulfide/ferric oxide (MoS2@Fe2O3) nanocomposites as a coreaction accelerator was developed for detection of neuron-specific enolase (NSE), a biomarker of small cell lung cancer. The doping of nitrogen allows the CQDs to exhibit ECL signals with low excitation potential, with a more viable activity possible for immune molecules. MoS2@Fe2O3 nanocomposites exhibit superior coreaction acceleration characteristics in hydrogen peroxide than any single component of them, and the highly branched dendrite microstructure provides a large number of binding sites for immune molecular, which is an inevitable factor for trace detection. In addition, ion beam sputtering gold particle technology is introduced into the sensor fabrication via an Au-N bond, which will provide sufficient density orientation for capturing the antibody load via the Au-N bonds. With excellent repeatability, stability, and specificity, the as-purposed sensing platform showed differentiated ECL responses of NSE range from 10.00 fg/mL to 500 ng/mL, and the limit of detection (LOD) was calculated of 6.30 fg/mL (S/N = 3). The proposed biosensor is prospective to provide a new avenue for the analysis of NSE or other biomarkers.

Pyronin Derivatives as Efficient Electrochemiluminescence Emitters in Aqueous Solution

The electrochemiluminescence (ECL) behavior of pyronin derivatives was reported. We found that these derivatives, as novel ECL emitters, generated an efficient emission phenomenon; that is, they showed anodic emission using tri-propylamine (TPA) as the coreactant and cathodic ECL emission using K2S2O8 as the coreactant. Because of its remarkable luminescent performance, the ECL mechanism (reductive-oxidative and oxidative-reductive) of benzylthiol-substituted pyronin (BTP) was specifically studied. Surprisingly, the cathodic ECL emission of BTP had a lower ECL peak potential at −0.54 V (vs. SCE) in aqueous solution. The potential range of −0.7 V to 0.0 V is lower than that of previously reported K2S2O8 cathodic ECL systems. Its good water solubility, easy modification, and excellent emission properties facilitate appealing (bio)analytical applications in ECL biosensors and cell imaging.

Performance enhancement of electrochemiluminescence magnetic microbiosensors by using double magnetic field actuation for cancer biomarkers and exosomes

This work reports the performance enhancement strategies on magnetic beads (MBs)-based electrochemiluminescence (ECL) platforms by using double magnetic field actuation of the ECL magnetic microbiosensors (MMbiosensors) for highly sensitive determination of cancer biomarker and exosomes. To obtain the high sensitivity and reproducibility of the ECL MMbiosensors, a series of strategies have been developed including replacing a conventional photomultiplier tube (PMT) with a diamagnetic PMT, replacing the stacked ring-disc magnets with circular-disc magnets lain-in glassy carbon electrode, adding a pre-concentration process of MBs using external magnet actuation. For fundamental research, the ECL MBs taken as the substitute of ECL MMbiosensors were prepared by binding biotinylated DNA tagged with Ru(bpy)32+ derivative (Ru1) to streptavidin-coated MB(MB@SA) were which showed that the developed strategies can enhance 45-fold sensitivity. Importantly, the developed MBs-based ECL platform was estimated by determination of prostate specific antigen (PSA) and exosomes. For PSA, MB@SA•biotin-Ab1(PSA) was taken as the capture probe and Ru1-labeled Ab2 (PSA) was done as ECL probe, while for exosomes, MB@SA•biotin-aptamer (CD63) was taken as the capture probe and Ru1-labeled Ab (CD9) was done as the ECL probe. The experiment results showed that the developed strategies can enhance 33-fold sensitivity of ECL MMbiosensors for PSA and exosomes. The detection limit is 0.28 ng mL−1 for PSA and 4.9 × 102 particle mL-1 for exosomes. This work demonstrated that a series of proposed magnetic field actuation strategies greatly increase the sensitivity of the ECL MMbiosensors. The developed strategies can be expanded to MBs-based ECL and electrochemical biosensors for clinical analysis with greater sensitivity.

A resonant energy transfer electrochemiluminescence immunosensor based on low trigger potential of Zn-metal organic framework and CoOOH nanosheets for 5-fluorouracil detection

The organic luminophores have inspired widespread interest in electrochemiluminescence (ECL). Herein, a novel rod-like metal-organic framework was formed by chelating Zn ion with 9,10-di(p-carboxyphenyl)-anthracene (DPA), defined as Zn-MOF for simplicity. In this proposal, the prepared Zn-MOF was first used as a powerful organic luminophore with low trigger potential, thus developing a competitive ECL immunoassay for ultrasensitive detection of 5-fluorouracil (5-FU) with 1,4-diazabicyclo[2.2.2]octane (D-H2) as the coreactant. The absorption spectrum of cobalt oxyhydroxide (CoOOH) nanosheets and the ECL emission spectrum of Zn-MOF could be highly matched, which ensured the occurrence of resonance energy transfer (RET). For that, ECL-RET was applied in the assembly strategy of the ECL biosensor, and Zn-MOF was used as the energy donor and CoOOH nanosheets as the acceptor. Taking advantage of the luminophore and ECL-RET, the immunoassay can be used for ultra-sensitive quantitative detection of 5-fluorouracil. The proposed ECL-RET immunosensor showed satisfactory sensitivity and accuracy with a wider linear range from 0.001 to 1000 ng/mL, and a lower detection limit (0.52 pg/mL). Hence, it is worth believing that this strategy can pave a bright research direction for the detection of 5-FU or other biological small molecules.