Inosine monophosphate(IMP),as a critical umami substance,is one of the most important indicators for evaluating the quality of meat products.Here,a sensitive electrochemiluminescence(ECL)biosensor based on graphdiyne(...Inosine monophosphate(IMP),as a critical umami substance,is one of the most important indicators for evaluating the quality of meat products.Here,a sensitive electrochemiluminescence(ECL)biosensor based on graphdiyne(GDY)/AuNPs/luminol nanocomposites was constructed to detect IMP.The GDY/AuNPs/luminol nanocomposites were synthesized by using simple one-pot method.GDY utilized its 2D framework to disperse and fix gold nanoparticles,which inhibited the agglomeration of gold nanoparticles and greatly improved its stability and catalytic properties.Importantly,GDY/AuNPs/luminol nanocomposites showed excellent catalytic ability and superior ECL activity towards luminol-H_(2)O_(2) systems due to the synergistic effect of GDY and AuNPs.Under optimal conditions,the prepared biosensor exhibited a wide linear range from 0.01 g/L to 20 g/L,a satisfactory limit detection of 0.0013 g/L,as well as an excellent specificity.Moreover,we carried out the precise analysis of IMP in actual meat samples with acceptable results compared to the liquid chromatography.We believe that this work could offer an efficient ECL platform for accurate and reliable report of IMP levels,which is significant for maintaining food quality and safety.展开更多
A capillary electrophoresis (CE) coupled with end-column electrochemiluminescence (ECL) detection method for the analysis of tramadol (TMD) has been investigated. ECL detection was working electrode biased at 1.2 V in...A capillary electrophoresis (CE) coupled with end-column electrochemiluminescence (ECL) detection method for the analysis of tramadol (TMD) has been investigated. ECL detection was working electrode biased at 1.2 V in a 20mmol·L-1 sodium phosphate buffer (pH = 8.0) containing 5 mmol·L-1 Ru (where bpy = 2,2’-bipyridyl). Linear correlation (r ≥ 0.997) between ECL intensity and drug concentration was obtained in the range 3 × 10-4 - 6 × 10-6 mol·L-1. The limits of detection (LODs) for tramadol in water was 3.012 × 10-8 mol·L-1(S/N = 3). The relative standard deviation values on peak size (10-5 mol·L-1 level) and migration time for the tramadol were 4.58% and 1.39% (n = 10), respectively. Applicability of the CE-ECL method to the analysis of human serum spiked with tramadol was展开更多
The electrochemiluminescence (ECL) of a new reagent 6- (2-hydroxy- 4 diethy laminophenylazo)-2,3-dihydro-1 ,4-phthalazine-1,4-dione (HDEA) in a basic aqueous so lution was studied by using the apparatus designed by ou...The electrochemiluminescence (ECL) of a new reagent 6- (2-hydroxy- 4 diethy laminophenylazo)-2,3-dihydro-1 ,4-phthalazine-1,4-dione (HDEA) in a basic aqueous so lution was studied by using the apparatus designed by ourselves. Trace amounts of silver ( Ⅰ ) shows a significant effect on the efficiency of light emission of HDEA during a positive trigonometrical wave pulse was exerted on the solution. The linear relationship between the light intensity and the concentration of silver( Ⅰ ) occurs in the range of 5. 0×10-8 to 3. 0×10-8 mol/L Ag(Ⅰ ) in a medium of KOH-KCl-HDEA (pH= 12. 8). The detection limit of the method is 2. 0×10-8 mol/LAg( Ⅰ ), and the r. s. d. for 1.0×10-7 mo)/L Ag ( Ⅰ ) is 5%. Of 21 metal ions concerned, only nickel( Ⅱ ), cerium( Ⅳ ) and cobalt( Ⅱ ) interfere the silver detection seriously; Ⅰ and Br also have some interference.展开更多
Objective To investigate the electrochemiluminescence (ECL) behavior of cloperastine hydrochloride. Methods ECL intensity of tris (2,2′-bipyridyl) rutheniumo(Ⅱ) was enhanced, the method for the determination of clop...Objective To investigate the electrochemiluminescence (ECL) behavior of cloperastine hydrochloride. Methods ECL intensity of tris (2,2′-bipyridyl) rutheniumo(Ⅱ) was enhanced, the method for the determination of cloperastine hydrochloride was established using capillary electrophoresis (CE) coupled with electrochemilumolinescence (ECL) detection. Results Under the optimum conditions, ECL intensity varied linearly with cloperastine hydrochloride concentration from 7.0×10-6g/mL to 1.0×10-4g/mL. The detection limit (S/N=3) was 8.05×10-7g/mL. The relative standard deviation of the ECL intensity and the migration time for 11 consecutive injections of 1.0×10-5g/mL cloperastine hydrochloride was 2.9% and 1.5%, respectively. This method was successfully applied to cloperastine hydrochloride tablet determination. Conclusion The method has been established, validated and applied for determination of cloperastine hydrochloride.展开更多
Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we re...Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.展开更多
Full utilization of the excited species at both singlet states(1R*)and triplet states(3R*)is crucial to improving electrochemiluminescence(ECL)efficiency but is challenging for organic luminescent materials.Here,an ag...Full utilization of the excited species at both singlet states(1R*)and triplet states(3R*)is crucial to improving electrochemiluminescence(ECL)efficiency but is challenging for organic luminescent materials.Here,an aggregation-induced delayed ECL(AIDECL)active organic dot(OD)containing a benzophenone acceptor and dimethylacridine donor is reported,which shows high ECL efficiency via reverse intersystem crossing(RISC)of non-emissive 3R*to emissive 1R*,overcoming the spin-forbidden radiative decay from 3R*.By introducing dual donor-acceptor pairs into luminophores,it is found that nonradiative pathway could be further suppressed via enhanced intermolecular weak interactions,and multiple spin-up conversion channels could be activated.As a consequence,the obtained OD enjoys a 6.8-fold higher ECL efficiency relative to the control AIDECL-active OD.Single-crystal studies and theoretical calculations reveal that the enhanced AIDECL behaviors come from the acceleration of both radiative transition and RISC.This work represents a major step towards purely organic,high-efficiency ECL dyes and a direction for the design of next-generation ECL dyes at the molecular level.展开更多
Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsula...Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsulated metal-organic frameworks(MOFs) as co-reactants and terminal deoxynucleotidyl transferase(Td T)-mediated template-free branched polymerization, a dual signal-amplified electrochemiluminescent(ECL) biosensor was constructed to detect DNA adenine methylation(Dam) MTase. The employment of WO_(3-x) dots-encapsulated MOFs(i.e., NH_(2)-UIO66@WO_(3-x) ) was not only beneficial for biomolecule conjugation because of the abundant amino groups but also led to a 7-fold enhanced ECL response due to the increased loading of WO_(3-x). Moreover, Td T-mediated template-free branched polymerization promoted the capture of ECL emitters on the electrode surface, achieving 20-fold enhanced signal amplification. The presented ECL biosensor demonstrated a low detection limit of 2.4 × 10^(-4)U/m L, and displayed high reliability for the detection of Dam MTase in both spiked human serum and E. coli cell samples, and for the screening of potential inhibitors. This study opens a new avenue for designing a dual signal amplificationbased ECL bioassay for Dam MTase and screening inhibitors in the fields of clinical diagnosis and drug development.展开更多
The electrochemiluminescence(ECL)behavior of a multiresonance thermally activated delayed fluorescence molecule has been investigated for the first time by means of ECL‐voltage curves,newly designed ECL‐time observa...The electrochemiluminescence(ECL)behavior of a multiresonance thermally activated delayed fluorescence molecule has been investigated for the first time by means of ECL‐voltage curves,newly designed ECL‐time observatory,and ECL spectroscopy.The compound,Mes3DiKTa,shows complex ECL behavior,including a delayed onset time of 5 ms for ECL generation in both the annihilation pathway and the coreactant route,which we attribute to organic long‐persistent ECL(OLECL).Triplet‐triplet annihilation,thermally activated delayed fluorescence and uncompensated solution resistance cannot be ruled out as contributing mechanisms to the ECL.A very long ECL emission decay was attributed to OLECL as well.The absolute ECL efficiencies of Mes3DiKTa were enhanced and reached 0.0013%in annihilation route and 1.1%for the coreactant system,which are superior to those of most other organic ECL materials.It is plausible that ECL materials with comparable behavior as Mes3DiKTa are desirable in applications such as ECL sensing,imaging,and light‐emitting devices.展开更多
Herein,an intense electrochemiluminescence(ECL)was achieved based on Pt hollow nanospheres/rubrene nanoleaves(Pt HNSs/Rub NLs)without the addition of any coreactant,which was employed for ultrasensitive detection of c...Herein,an intense electrochemiluminescence(ECL)was achieved based on Pt hollow nanospheres/rubrene nanoleaves(Pt HNSs/Rub NLs)without the addition of any coreactant,which was employed for ultrasensitive detection of carcinoembryonic antigen(CEA)coupled with an M-shaped DNA walker(M-DNA walker)as signal switch.Specifically,in comparison with platinum nanoparticles(Pt NPs),Pt HNSs revealed excellent catalytic performance and pore confinement-enhanced ECL,which could significantly amplify ECL intensity of Rub NLs/dissolved O_(2)(DO)binary system.Then,the tracks and M-DNA walker were confined on the Pt HNSs simultaneously to promote the reaction efficiency,whose M-structure boosted the interaction sites between walking strands and tracks and reduced the rigidity of their recognition.Once the CEA approached the sensing interface,the M-DNA walker was activated based on highly specific aptamer recognition to recover ECL intensity with the assistance of exonucleaseⅢ(ExoⅢ).As proof of concept,the“on-off-on”switch aptasensor was constructed for CEA detection with a low detection limit of 0.20 fg/m L.The principle of the constructed ECL aptasensor also enables a universal platform for sensitive detection of other tumor markers.展开更多
Due to the advantages of low background interference and high sensitivity, electrochemiluminescence (ECL)-based sensor has developed rapidly in recent years. The ECL sensors have shown the potential in the ultrasensit...Due to the advantages of low background interference and high sensitivity, electrochemiluminescence (ECL)-based sensor has developed rapidly in recent years. The ECL sensors have shown the potential in the ultrasensitive and real-time analysis. Especially, the visual ECL analysis, including visual detection, cell imaging and single particle analysis, has offered many unique sensing platforms for analysis research and point-of-care testing. The high throughput ECL image analysis can not only provide ECL intensity but also reveal more information about the chemical reaction activity of particle and the physi-ological processes of cell operation. Therefore, we review the novel ECL luminophore, sensing systems, and successful applications in the visual ECL detection and imaging in this paper. First, the different ECL luminophore is summarized. Second, we discuss the ECL sensing mechanisms, focusing on the advantages and limitations of different sensing methods. Then, we highlight the recent advances in representative examples of visual ECL analysis, including aptasensing, multiplex immunoassays, cell imaging and single-particle analysis. At last, the outlook and prospects for the future visual ECL analysis are discussed based on the current development of ECL research.展开更多
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high lumines...A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
Electrochemiluminescence(ECL)has been widely applied in imaging owing to features that distinguish it from other microscopic techniques and electrochemical methods,including its high signal-to-noise ratio,remarkable s...Electrochemiluminescence(ECL)has been widely applied in imaging owing to features that distinguish it from other microscopic techniques and electrochemical methods,including its high signal-to-noise ratio,remarkable sensitivity,wide linear range,high spatiotemporal resolution,and near-zero background light.Imaging technology based on ECL has been used in the fields of immunosensing,pathological cell detection,and drug analysis.Additionally,its simple operation and ability to detect dynamic processes and catalytic sites strengthen its potential for research on material surfaces and interfaces,in vivo biological analysis,and cell visualization.At the same time,the emergence of a variety of nanomaterials and new microscopic analysis equipment has further promoted the development of high-resolution ECL imaging technology.This paper introduces the development of ECL technology and the mechanisms of the main ECL systems.It then describes various forms of ECL imaging methods,and reviews research progress on ECL imaging technology in the fields of single-particle imaging,fingerprint structure analysis,and single-cell microscopic imaging.Finally,the authors offer their views about the prospects for ECL imaging technology.展开更多
Electrogenerated chemiluminescence, also known as electrochemiluminescence, abbreviated ECL, is a new technology combining electrochemistry and chemiluminescence. It is generated by high-energy electrons generated on ...Electrogenerated chemiluminescence, also known as electrochemiluminescence, abbreviated ECL, is a new technology combining electrochemistry and chemiluminescence. It is generated by high-energy electrons generated on the surface of the electrode in the emission process of excited state photons formed in the transfer process, and is a perfect combination of electrochemistry and spectroscopy. It not only has the advantages of good environment, high luminosity and wide dynamic range, but also has the characteristics of simple, stable and practical electrochemical methods, and nearly zero background signals. With the rapid development of nanomaterials, due to their unique electrical properties, large specific surface area, good biocompatibility and other characteristics, various nanomaterials have been widely used in the field of biosensors and sensitive detection. This review presented a general description of the research status of four different types of biosensors from the last decade years, summarized the application forms of nanomaterials in ECL biosensor, and outlines the building patterns and application example of the four main types of biosensors.展开更多
Multicolor electrochemiluminescence(ECL) of semiconductor nanocrystals tuned by size effect has been successfully achieved using quantum dots(QDs) with core-shell structure for the first time. It would open a new way ...Multicolor electrochemiluminescence(ECL) of semiconductor nanocrystals tuned by size effect has been successfully achieved using quantum dots(QDs) with core-shell structure for the first time. It would open a new way and provide a guidance for design and preparation of stable and strong multicolor ECL emitters for simultaneous multicomponent analysis application.展开更多
Sensitive and accurate detection of biological analytes,such as proteins,genes,small molecules,ions,cells,etc.,has been a significant project in life science.Signal amplification is one of the most effective approache...Sensitive and accurate detection of biological analytes,such as proteins,genes,small molecules,ions,cells,etc.,has been a significant project in life science.Signal amplification is one of the most effective approaches to improve the sensitivity of bioanalysis.Taking advantage of specific base pairing,programmable operation,and predictable assembly,DNA is flexible and suitable to perform the signal amplification procedure.In recent years,signal amplification strategies by means of DNA technology have been widely integrated into the construction of electrochemiluminescence(ECL)biosensors,achieving desirable analytical performance in clinical diagnosis,biomedical research,and drug development.To the best of our knowledge,these DNA signal amplification technologies mainly include classical polymerase chain reaction,and various amplification approaches conducted under mild conditions,such as rolling circle amplification(RCA)or hyperbranched RCA,cleaving enzyme-assisted amplification,DNAzyme-involved amplification,toehold-mediated DNA strand displacement amplification without enzyme participation,and so on.This review overviews the recent advancements of DNA signal amplification strategies for bioanalysis in the ECL realm,sketching the creative trajectory from strategies design to ultrasensitive ECL platform construction and resulting applications.展开更多
Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reacta...Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reactant, tripropylamine (TPA), is toxic, corrosive and volatile. Therefore, the search for safe, sensitive and economical co-reactants is critical. Herein, three aminocarboxylic acids, ethylenediamine-tetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and 2-hydroxyethylethylene diaminetriacetic acid (HEDTA), have been investigated as potential co-reactants for promoting Ru(bpy)32+ ECL behaviour. A possible ECL mechanism is also presented. The experimental results suggested that the co-reactants have a different ECL behaviour compared to TPA, such as different pH- and surfactant-responses. The detection limits of Ru(bpy)32+ using NTA, EDTA and HEDTA as co-reactants are 1, 60 and 680 fmol·L-1, respectively. The results indicate that NTA has a much higher efficiency than TPA to excite Ru(bpy)3 2+ ECL under their own optimal conditions. NTA could be widely used in many fields because it is less toxic, corrosive and volatile than TPA. Moreover, using Ru(bpy)3 2+ ECL, a sensitive method for the detection of aminocarboxylic acids is also developed. An improvement of four orders of magnitude in detection limits is obtained for EDTA compared to the known Ru(bpy) 3 2+ chemiluminescent methods.展开更多
Trace Ir(Ⅲ)complex enhanced aggregation-induced electrochemiluminescence(AIECL)of poly-tetraphenylethene(p TPE)in aqueous media was investigated for the first time.The poly-TPE end-capped by Ir(Ⅲ)complex(Ir@p TPE)an...Trace Ir(Ⅲ)complex enhanced aggregation-induced electrochemiluminescence(AIECL)of poly-tetraphenylethene(p TPE)in aqueous media was investigated for the first time.The poly-TPE end-capped by Ir(Ⅲ)complex(Ir@p TPE)and its corresponding model polymer poly-TPE(Ph@pTPE)could be synthesized by Suzuki coupling polymerization reaction of 1,2-bis(4-bromophenyl)-1,2-diphenylethene(M-1)with 1,2-diphenyl-1,2-bis(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)phenyl)ethene(M-2)and the continuous Suzuki coupling end-capped reaction of poly-TPE-pinacol boronate with(pq)2 Ir(pico)Br and bromobenzene,respectively.Subsequently,the corresponding Ir@p TPE Pdots and Ph@p TPE Pdots encapsulated with poly(styrene-co-maleicanhydride)(PSMA)could be obtained by nanoprecipitation method.Compared with Ph@p TPE Pdots,the Ir@p TPE Pdots with a trace amount of Ir(Ⅲ)complex(1.34‰of Ir(Ⅲ)content,wt)could exhibit 9.9-fold enhancement of the electrochemiluminescence(ECL)signal for visual emission.This work provided a novel strategy on designing highly efficient ECL materials based on trace Ir(Ⅲ)-end capping AIE-active polymer dots.展开更多
Electrochemiluminescence(ECL)-based imaging analysis is a dominant method to inspect the electrode composition,to study electrochemical reaction kinetics at a microscopic level,and also a rapid emerging technology in ...Electrochemiluminescence(ECL)-based imaging analysis is a dominant method to inspect the electrode composition,to study electrochemical reaction kinetics at a microscopic level,and also a rapid emerging technology in bioanalysis with high spatiotemporal resolutions,high-throughput and visualization characteristics.In comparison with other imaging microscopes,an optical excitation is not involved in imaging,thus the approach is free from background noise resulting in a low detec-tion limit.In this review work,the principle of ECL,its unique natures compared to other luminescence techniques were briefed at first.Then after,the progress and basic principles of ECL imaging were summarized.Furthermore,recent and representative advances of ECL imaging for visualizing and sensing applications were reviewed.Finally,the perspectives in ECL imaging for further perspective were discussed.展开更多
Electrochemiluminescence(ECL) is a kind of luminescent phenomenon caused by electrochemical reactions. Based on the advantages of ECL including low background, high sensitivity, strong spatiotemporal controllability a...Electrochemiluminescence(ECL) is a kind of luminescent phenomenon caused by electrochemical reactions. Based on the advantages of ECL including low background, high sensitivity, strong spatiotemporal controllability and simple operation, ECL imaging is able to visualize the ECL process,which can additionally achieve high throughput, fast and visual analysis. With the development of optical imaging technique, ECL imaging at micro-or nanoscale has been successfully applied in immunoassay,cell imaging, biochemical analysis, single-nanoparticle detection and study of mechanisms and kinetics of reactions, which has attracted extensive attention. In this review, the basic principles and apparatus of ECL imaging were briefly introduced at first. Then several latest and representative applications of ECL imaging based on nanomaterials and micro-/nanostructures were overviewed. Finally, the superiorities and challenges in ECL imaging for further development were discussed.展开更多
基金supported by The National Natural Science Foundation of China(31972198,31622042)The National Key R&D Program of China(2016YFD0400803,2016YFD0401501).
文摘Inosine monophosphate(IMP),as a critical umami substance,is one of the most important indicators for evaluating the quality of meat products.Here,a sensitive electrochemiluminescence(ECL)biosensor based on graphdiyne(GDY)/AuNPs/luminol nanocomposites was constructed to detect IMP.The GDY/AuNPs/luminol nanocomposites were synthesized by using simple one-pot method.GDY utilized its 2D framework to disperse and fix gold nanoparticles,which inhibited the agglomeration of gold nanoparticles and greatly improved its stability and catalytic properties.Importantly,GDY/AuNPs/luminol nanocomposites showed excellent catalytic ability and superior ECL activity towards luminol-H_(2)O_(2) systems due to the synergistic effect of GDY and AuNPs.Under optimal conditions,the prepared biosensor exhibited a wide linear range from 0.01 g/L to 20 g/L,a satisfactory limit detection of 0.0013 g/L,as well as an excellent specificity.Moreover,we carried out the precise analysis of IMP in actual meat samples with acceptable results compared to the liquid chromatography.We believe that this work could offer an efficient ECL platform for accurate and reliable report of IMP levels,which is significant for maintaining food quality and safety.
文摘A capillary electrophoresis (CE) coupled with end-column electrochemiluminescence (ECL) detection method for the analysis of tramadol (TMD) has been investigated. ECL detection was working electrode biased at 1.2 V in a 20mmol·L-1 sodium phosphate buffer (pH = 8.0) containing 5 mmol·L-1 Ru (where bpy = 2,2’-bipyridyl). Linear correlation (r ≥ 0.997) between ECL intensity and drug concentration was obtained in the range 3 × 10-4 - 6 × 10-6 mol·L-1. The limits of detection (LODs) for tramadol in water was 3.012 × 10-8 mol·L-1(S/N = 3). The relative standard deviation values on peak size (10-5 mol·L-1 level) and migration time for the tramadol were 4.58% and 1.39% (n = 10), respectively. Applicability of the CE-ECL method to the analysis of human serum spiked with tramadol was
文摘The electrochemiluminescence (ECL) of a new reagent 6- (2-hydroxy- 4 diethy laminophenylazo)-2,3-dihydro-1 ,4-phthalazine-1,4-dione (HDEA) in a basic aqueous so lution was studied by using the apparatus designed by ourselves. Trace amounts of silver ( Ⅰ ) shows a significant effect on the efficiency of light emission of HDEA during a positive trigonometrical wave pulse was exerted on the solution. The linear relationship between the light intensity and the concentration of silver( Ⅰ ) occurs in the range of 5. 0×10-8 to 3. 0×10-8 mol/L Ag(Ⅰ ) in a medium of KOH-KCl-HDEA (pH= 12. 8). The detection limit of the method is 2. 0×10-8 mol/LAg( Ⅰ ), and the r. s. d. for 1.0×10-7 mo)/L Ag ( Ⅰ ) is 5%. Of 21 metal ions concerned, only nickel( Ⅱ ), cerium( Ⅳ ) and cobalt( Ⅱ ) interfere the silver detection seriously; Ⅰ and Br also have some interference.
文摘Objective To investigate the electrochemiluminescence (ECL) behavior of cloperastine hydrochloride. Methods ECL intensity of tris (2,2′-bipyridyl) rutheniumo(Ⅱ) was enhanced, the method for the determination of cloperastine hydrochloride was established using capillary electrophoresis (CE) coupled with electrochemilumolinescence (ECL) detection. Results Under the optimum conditions, ECL intensity varied linearly with cloperastine hydrochloride concentration from 7.0×10-6g/mL to 1.0×10-4g/mL. The detection limit (S/N=3) was 8.05×10-7g/mL. The relative standard deviation of the ECL intensity and the migration time for 11 consecutive injections of 1.0×10-5g/mL cloperastine hydrochloride was 2.9% and 1.5%, respectively. This method was successfully applied to cloperastine hydrochloride tablet determination. Conclusion The method has been established, validated and applied for determination of cloperastine hydrochloride.
基金National Natural Science Foundation of China,Grant/Award Numbers:22004001,21631001,21871001Anhui Provincial Natural Science Foundation,Grant/Award Number:2008085QB84the Ministry of Education,the University Synergy Innovation Program of Anhui Province,Grant/Award Number:GXXT-2020-053。
文摘Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.
基金National Natural Science Foundation of China,Grant/Award Numbers:22034003,22204075,22275085Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20220769+1 种基金Excellent Research Program of Nanjing University,Grant/Award Number:ZYJH004State Key Laboratory of Analytical Chemistry for Life Science,Grant/Award Number:5431ZZXM2203。
文摘Full utilization of the excited species at both singlet states(1R*)and triplet states(3R*)is crucial to improving electrochemiluminescence(ECL)efficiency but is challenging for organic luminescent materials.Here,an aggregation-induced delayed ECL(AIDECL)active organic dot(OD)containing a benzophenone acceptor and dimethylacridine donor is reported,which shows high ECL efficiency via reverse intersystem crossing(RISC)of non-emissive 3R*to emissive 1R*,overcoming the spin-forbidden radiative decay from 3R*.By introducing dual donor-acceptor pairs into luminophores,it is found that nonradiative pathway could be further suppressed via enhanced intermolecular weak interactions,and multiple spin-up conversion channels could be activated.As a consequence,the obtained OD enjoys a 6.8-fold higher ECL efficiency relative to the control AIDECL-active OD.Single-crystal studies and theoretical calculations reveal that the enhanced AIDECL behaviors come from the acceleration of both radiative transition and RISC.This work represents a major step towards purely organic,high-efficiency ECL dyes and a direction for the design of next-generation ECL dyes at the molecular level.
基金supported by the National Natural Science Foundation of China (Nos.22074015 and 22174014)。
文摘Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsulated metal-organic frameworks(MOFs) as co-reactants and terminal deoxynucleotidyl transferase(Td T)-mediated template-free branched polymerization, a dual signal-amplified electrochemiluminescent(ECL) biosensor was constructed to detect DNA adenine methylation(Dam) MTase. The employment of WO_(3-x) dots-encapsulated MOFs(i.e., NH_(2)-UIO66@WO_(3-x) ) was not only beneficial for biomolecule conjugation because of the abundant amino groups but also led to a 7-fold enhanced ECL response due to the increased loading of WO_(3-x). Moreover, Td T-mediated template-free branched polymerization promoted the capture of ECL emitters on the electrode surface, achieving 20-fold enhanced signal amplification. The presented ECL biosensor demonstrated a low detection limit of 2.4 × 10^(-4)U/m L, and displayed high reliability for the detection of Dam MTase in both spiked human serum and E. coli cell samples, and for the screening of potential inhibitors. This study opens a new avenue for designing a dual signal amplificationbased ECL bioassay for Dam MTase and screening inhibitors in the fields of clinical diagnosis and drug development.
基金supports to this study by Natural Sciences and Engineering Research Council Canada(NSERC,DG RGPIN‐2018‐06556 and SPG STPGP‐2016‐493924)Canada Foundation of Innovation/Ontario Innovation Trust(CFI/OIT,9040)The University of Western Ontario.
文摘The electrochemiluminescence(ECL)behavior of a multiresonance thermally activated delayed fluorescence molecule has been investigated for the first time by means of ECL‐voltage curves,newly designed ECL‐time observatory,and ECL spectroscopy.The compound,Mes3DiKTa,shows complex ECL behavior,including a delayed onset time of 5 ms for ECL generation in both the annihilation pathway and the coreactant route,which we attribute to organic long‐persistent ECL(OLECL).Triplet‐triplet annihilation,thermally activated delayed fluorescence and uncompensated solution resistance cannot be ruled out as contributing mechanisms to the ECL.A very long ECL emission decay was attributed to OLECL as well.The absolute ECL efficiencies of Mes3DiKTa were enhanced and reached 0.0013%in annihilation route and 1.1%for the coreactant system,which are superior to those of most other organic ECL materials.It is plausible that ECL materials with comparable behavior as Mes3DiKTa are desirable in applications such as ECL sensing,imaging,and light‐emitting devices.
基金financially supported by the National Natural Science Foundation(NNSF)of China(No.22022408)the Chongqing Talents Personnel Support Program(No.NCQYC201905067)the Fundamental Research Funds for the Central Universities(No.XDJK2019TJ002)。
文摘Herein,an intense electrochemiluminescence(ECL)was achieved based on Pt hollow nanospheres/rubrene nanoleaves(Pt HNSs/Rub NLs)without the addition of any coreactant,which was employed for ultrasensitive detection of carcinoembryonic antigen(CEA)coupled with an M-shaped DNA walker(M-DNA walker)as signal switch.Specifically,in comparison with platinum nanoparticles(Pt NPs),Pt HNSs revealed excellent catalytic performance and pore confinement-enhanced ECL,which could significantly amplify ECL intensity of Rub NLs/dissolved O_(2)(DO)binary system.Then,the tracks and M-DNA walker were confined on the Pt HNSs simultaneously to promote the reaction efficiency,whose M-structure boosted the interaction sites between walking strands and tracks and reduced the rigidity of their recognition.Once the CEA approached the sensing interface,the M-DNA walker was activated based on highly specific aptamer recognition to recover ECL intensity with the assistance of exonucleaseⅢ(ExoⅢ).As proof of concept,the“on-off-on”switch aptasensor was constructed for CEA detection with a low detection limit of 0.20 fg/m L.The principle of the constructed ECL aptasensor also enables a universal platform for sensitive detection of other tumor markers.
基金The authors gratefully acknowledge financial support from Youth Science Fund of Jilin Province(20140520081JH)“Thirteenth Five Year”Project of the Science and Technology Research in the Education Department of Jilin Province,China.
文摘Due to the advantages of low background interference and high sensitivity, electrochemiluminescence (ECL)-based sensor has developed rapidly in recent years. The ECL sensors have shown the potential in the ultrasensitive and real-time analysis. Especially, the visual ECL analysis, including visual detection, cell imaging and single particle analysis, has offered many unique sensing platforms for analysis research and point-of-care testing. The high throughput ECL image analysis can not only provide ECL intensity but also reveal more information about the chemical reaction activity of particle and the physi-ological processes of cell operation. Therefore, we review the novel ECL luminophore, sensing systems, and successful applications in the visual ECL detection and imaging in this paper. First, the different ECL luminophore is summarized. Second, we discuss the ECL sensing mechanisms, focusing on the advantages and limitations of different sensing methods. Then, we highlight the recent advances in representative examples of visual ECL analysis, including aptasensing, multiplex immunoassays, cell imaging and single-particle analysis. At last, the outlook and prospects for the future visual ECL analysis are discussed based on the current development of ECL research.
基金supported by the Natural Science Foundation of Hebei Province(Grant No.E2022209039)Key Research Project of North China University of Science and Technology(Grant No.ZD-YG-202301)Tangshan Talent Funding Project(Grant No.A202202007).
文摘A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
基金The authors thank National Natural Science Foundation of China(Nos.21874126 and 22174136)CAS President’s International Fellowship Initiative(PIFI)+1 种基金Agence Nationale de la Recherche(ELISE-ANR-21-CE42)Translation of Combination Research of First Hospital of Jilin University and Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,CAS-VPST Silk Road Science Fund 2021(GJHZ202125 and INSF 99008701)for financial support.
文摘Electrochemiluminescence(ECL)has been widely applied in imaging owing to features that distinguish it from other microscopic techniques and electrochemical methods,including its high signal-to-noise ratio,remarkable sensitivity,wide linear range,high spatiotemporal resolution,and near-zero background light.Imaging technology based on ECL has been used in the fields of immunosensing,pathological cell detection,and drug analysis.Additionally,its simple operation and ability to detect dynamic processes and catalytic sites strengthen its potential for research on material surfaces and interfaces,in vivo biological analysis,and cell visualization.At the same time,the emergence of a variety of nanomaterials and new microscopic analysis equipment has further promoted the development of high-resolution ECL imaging technology.This paper introduces the development of ECL technology and the mechanisms of the main ECL systems.It then describes various forms of ECL imaging methods,and reviews research progress on ECL imaging technology in the fields of single-particle imaging,fingerprint structure analysis,and single-cell microscopic imaging.Finally,the authors offer their views about the prospects for ECL imaging technology.
基金supported by the National Natural Science Foundation of China (Nos. 21675178, 21575167 and 21775167)the Guangdong Provincial Natural Science Foundation of China (No. 2016A030313358)+1 种基金the Research and Development Plan for Key Areas of Food Safety in Guangdong Province of China (No. 2019B020211001)the Guangzhou Science and Technology Program of China (No. 201604020165)
文摘Electrogenerated chemiluminescence, also known as electrochemiluminescence, abbreviated ECL, is a new technology combining electrochemistry and chemiluminescence. It is generated by high-energy electrons generated on the surface of the electrode in the emission process of excited state photons formed in the transfer process, and is a perfect combination of electrochemistry and spectroscopy. It not only has the advantages of good environment, high luminosity and wide dynamic range, but also has the characteristics of simple, stable and practical electrochemical methods, and nearly zero background signals. With the rapid development of nanomaterials, due to their unique electrical properties, large specific surface area, good biocompatibility and other characteristics, various nanomaterials have been widely used in the field of biosensors and sensitive detection. This review presented a general description of the research status of four different types of biosensors from the last decade years, summarized the application forms of nanomaterials in ECL biosensor, and outlines the building patterns and application example of the four main types of biosensors.
基金supported by the National Natural Science Foundation of China (21575022, 21535003)the National High Technology Research and Development Program of China (2015AA020502)+1 种基金the Open Research Fund of Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Southeast Universitythe Fundamental Research Funds for the Central Universities (KYLX15-0127)
文摘Multicolor electrochemiluminescence(ECL) of semiconductor nanocrystals tuned by size effect has been successfully achieved using quantum dots(QDs) with core-shell structure for the first time. It would open a new way and provide a guidance for design and preparation of stable and strong multicolor ECL emitters for simultaneous multicomponent analysis application.
基金financially supported by the National Natural Science Foundation of China(21834004 and 21904063)the Natural Science Foundation of Jiangsu Province(BK20190279)the Fundamental Research Funds for the Central Universities(021314380151)
文摘Sensitive and accurate detection of biological analytes,such as proteins,genes,small molecules,ions,cells,etc.,has been a significant project in life science.Signal amplification is one of the most effective approaches to improve the sensitivity of bioanalysis.Taking advantage of specific base pairing,programmable operation,and predictable assembly,DNA is flexible and suitable to perform the signal amplification procedure.In recent years,signal amplification strategies by means of DNA technology have been widely integrated into the construction of electrochemiluminescence(ECL)biosensors,achieving desirable analytical performance in clinical diagnosis,biomedical research,and drug development.To the best of our knowledge,these DNA signal amplification technologies mainly include classical polymerase chain reaction,and various amplification approaches conducted under mild conditions,such as rolling circle amplification(RCA)or hyperbranched RCA,cleaving enzyme-assisted amplification,DNAzyme-involved amplification,toehold-mediated DNA strand displacement amplification without enzyme participation,and so on.This review overviews the recent advancements of DNA signal amplification strategies for bioanalysis in the ECL realm,sketching the creative trajectory from strategies design to ultrasensitive ECL platform construction and resulting applications.
基金Supported by the National Natural Science Foundation of China (Grant No. 90717104)the Program for New Century Excellent Talents in University (Grant No. NCET-06-0214), Ministry of Education of China
文摘Due to the highly sensitive electrochemiluminescence (ECL), tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy)32+) is often used in the field of bioarrays with the help of co-reactants. However, the generally used co-reactant, tripropylamine (TPA), is toxic, corrosive and volatile. Therefore, the search for safe, sensitive and economical co-reactants is critical. Herein, three aminocarboxylic acids, ethylenediamine-tetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and 2-hydroxyethylethylene diaminetriacetic acid (HEDTA), have been investigated as potential co-reactants for promoting Ru(bpy)32+ ECL behaviour. A possible ECL mechanism is also presented. The experimental results suggested that the co-reactants have a different ECL behaviour compared to TPA, such as different pH- and surfactant-responses. The detection limits of Ru(bpy)32+ using NTA, EDTA and HEDTA as co-reactants are 1, 60 and 680 fmol·L-1, respectively. The results indicate that NTA has a much higher efficiency than TPA to excite Ru(bpy)3 2+ ECL under their own optimal conditions. NTA could be widely used in many fields because it is less toxic, corrosive and volatile than TPA. Moreover, using Ru(bpy)3 2+ ECL, a sensitive method for the detection of aminocarboxylic acids is also developed. An improvement of four orders of magnitude in detection limits is obtained for EDTA compared to the known Ru(bpy) 3 2+ chemiluminescent methods.
基金supported by the National Natural Science Foundation of China(21674046,51673093,21535003)the National Key Reaearch and Development Program of China(2016YFA0201200)。
文摘Trace Ir(Ⅲ)complex enhanced aggregation-induced electrochemiluminescence(AIECL)of poly-tetraphenylethene(p TPE)in aqueous media was investigated for the first time.The poly-TPE end-capped by Ir(Ⅲ)complex(Ir@p TPE)and its corresponding model polymer poly-TPE(Ph@pTPE)could be synthesized by Suzuki coupling polymerization reaction of 1,2-bis(4-bromophenyl)-1,2-diphenylethene(M-1)with 1,2-diphenyl-1,2-bis(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)phenyl)ethene(M-2)and the continuous Suzuki coupling end-capped reaction of poly-TPE-pinacol boronate with(pq)2 Ir(pico)Br and bromobenzene,respectively.Subsequently,the corresponding Ir@p TPE Pdots and Ph@p TPE Pdots encapsulated with poly(styrene-co-maleicanhydride)(PSMA)could be obtained by nanoprecipitation method.Compared with Ph@p TPE Pdots,the Ir@p TPE Pdots with a trace amount of Ir(Ⅲ)complex(1.34‰of Ir(Ⅲ)content,wt)could exhibit 9.9-fold enhancement of the electrochemiluminescence(ECL)signal for visual emission.This work provided a novel strategy on designing highly efficient ECL materials based on trace Ir(Ⅲ)-end capping AIE-active polymer dots.
基金the National Natural Science Foundation of China[Nos.21675148,21874126,an 21804127]Ministry of Science and Technology of the People’s Republic of China[No.2016YFA0201300]the Chinese Academy of Sciences(CAS)-the Academy of Sciences for the Developing World(TWAS)President’s Fellowship Programme[No.2016CTF032].
文摘Electrochemiluminescence(ECL)-based imaging analysis is a dominant method to inspect the electrode composition,to study electrochemical reaction kinetics at a microscopic level,and also a rapid emerging technology in bioanalysis with high spatiotemporal resolutions,high-throughput and visualization characteristics.In comparison with other imaging microscopes,an optical excitation is not involved in imaging,thus the approach is free from background noise resulting in a low detec-tion limit.In this review work,the principle of ECL,its unique natures compared to other luminescence techniques were briefed at first.Then after,the progress and basic principles of ECL imaging were summarized.Furthermore,recent and representative advances of ECL imaging for visualizing and sensing applications were reviewed.Finally,the perspectives in ECL imaging for further perspective were discussed.
基金supported by the National Natural Science Foundation of China (Nos. 21575126 and 21874117)the Natural Science Foundation of Zhejiang Province (No. LZ18B050001)
文摘Electrochemiluminescence(ECL) is a kind of luminescent phenomenon caused by electrochemical reactions. Based on the advantages of ECL including low background, high sensitivity, strong spatiotemporal controllability and simple operation, ECL imaging is able to visualize the ECL process,which can additionally achieve high throughput, fast and visual analysis. With the development of optical imaging technique, ECL imaging at micro-or nanoscale has been successfully applied in immunoassay,cell imaging, biochemical analysis, single-nanoparticle detection and study of mechanisms and kinetics of reactions, which has attracted extensive attention. In this review, the basic principles and apparatus of ECL imaging were briefly introduced at first. Then several latest and representative applications of ECL imaging based on nanomaterials and micro-/nanostructures were overviewed. Finally, the superiorities and challenges in ECL imaging for further development were discussed.
