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MICROCHEMICAL JOURNAL · 2021 · IF 4.821

A label-free ECL aptasensor for sensitive detection of carcinoembryonic antigen based on CdS QDs@MOF and TEOA@Au as bi-coreactants of Ru(bpy)32+

Xiu-hua Wei,Xing Qiao,Jie Fan,Yuan-qiang Hao,Yin-tang Zhang,Yan-li Zhou,Mao-tian Xu

Herein, a label-free electrochemiluminescence (ECL) biosensor for sensitive determination of carcinoembryonic antigen (CEA) was fabricated based on CdS quantum dots loaded onto metal organic framework (CdS QDs@MOF) and triethanolamine modified on gold nanoparticles (TEOA@AuNPs) as bi-coreactants of Ru(bpy) 3 2+ ECL system. The TEOA@AuNPs served as not only coreactant of Ru(bpy) 3 2+ but also nanocarrier for CEA aptamer which was bonded to the TEOA@AuNPs through Au–S bond. After incubated in CEA solution, the ECL signals decreased due to the poor conductivity of CEA and there was a linear correlation between the ECL intensity and log(C CEA ). Based on this result, a label-free ECL biosensor has been developed successfully and used to detect CEA with a detection limit of 8.5 × 10 −5 ng/mL. The proposed ECL aptasensor had good analytical performance in the detection of CEA in human serum samples.

研究领域: 生物传感 · 医学检测 · 纳米技术
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MICROCHIMICA ACTA · 2022 ·Vol. 189 ·期 11 ·1-15 · IF 6.408

Construction of efficient electrochemiluminescence resonance energy transfer sensor based on SnO2/SnS2QDs-Ru@IRMOF-3 composite for sensitive detection of procalcitonin

Qin Dongmiao,Meng Shuo,Wu Yusheng,Luo Zhi,Deng Biyang

An efficient electrochemiluminescence resonance energy transfer (ECL-RET) method is proposed which combines the luminescent materials of tris(4,4′-dicarboxylicacid-2,2′-bipyridyl) ruthenium(II) (energy donor) and tin dioxide and tin disulfide quantum dots (SnO 2 /SnS 2 QDs) (energy acceptor) into the isoreticular metal − organic framework-3 (IRMOF-3) material to form a composite. In this mode, the distance between the energy donor and the acceptor was greatly shortened, reducing the energy loss, and thereby effectively improving RET efficiency and further significantly improving the ECL signal. The obtained composite (SnO 2 /SnS 2 QDs-Ru@IRMOF-3) was combined with sandwich immunoreaction to construct an ECL immunosensor for the sensitive detection of procalcitonin (PCT). Under the optimized experimental conditions with a working potential of − 1.48 V (vs Ag/AgCl), the proposed PCT biosensor exhibited a linear concentration range of 1 × 10 −4 –200 ng mL −1 , with a detection limit of 0.029 pg mL −1 ( S / N  = 3). The biosensor was used to detect PCT in actual samples. The biosensor has broad application prospects in biological analysis and clinical diagnosis due to its high sensitivity, good selectivity, and good stability. Graphical abstract

研究领域: 分析化学 · 生物传感器 · 临床诊断
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Entropy-driven assisted T7 RNA polymerase amplification-activated CRISPR/Cas13a activity for SARS-CoV-2 detection in human pharyngeal swabs and environment by an electrochemiluminescence biosensor

Jihua Wei,Zichun Song,Jiuying Cui,Yuanxun Gong,Qianli Tang,Kai Zhang,Xinlei Song,Xianjiu Liao

In this study, we introduce an electrochemiluminescence (ECL) sensing platform based on the "Entropy-driven triggered T7 amplification-CRISPR/Cas13a system" (EDT-Cas). This platform combines a programmable entropy-driven cycling strategy, T7 RNA polymerase, and the CRISPR/Cas13a system to amplify the determination of the SARS-CoV-2 RdRp gene. The Ti 3 C 2 T x -compliant ECL signaling molecule offers unique benefits when used with the ECL sensing platform to increase the assay sensitivity and the electrode surface modifiability. To obtain the T7 promoter, the SARS-CoV-2 RdRp gene may first initiate an entropy-driven cyclic amplification response. Then, after recognizing the T7 promoter sequence on the newly created dsDNA, T7 RNA polymerase starts transcription, resulting in the production of many single-stranded RNAs (ssRNAs), which in turn trigger the action of CRISPR/Cas13a. Finally, Cas13a/crRNA identifies the transcribed ssRNA. When it cleaves the ssRNA, many DNA reporter probes carrying -U-U- are cleaved on the electrode surface, increasing the ECL signal and allowing for the rapid and highly sensitive detection of SARS-CoV-2. With a detection limit of 7.39 aM, our method enables us to locate the SARS-CoV-2 RdRp gene in clinical samples. The detection method also demonstrates excellent repeatability and stability. The SARS-CoV-2 RdRp gene was discovered using the "Entropy-driven triggered T7 amplification-CRISPR/Cas13a system" (EDT-Cas). The developed ECL test had excellent recoveries in pharyngeal swabs and environmental samples. It is anticipated to offer an early clinical diagnosis of SARS-CoV-2 and further control the spread of the pandemic.

研究领域: 生物技术 · 分子生物学 · 病毒学 · 诊断技术 · 纳米技术
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ANALYST · 2023 · IF 4.2

Ultrasensitive detect of CA125 based on triple signal amplification strategy with huge amount of loaded probes via exonuclease cyclic cleavage, rolling cyclic amplification and strand self-growth

Li He,Ciping Chen,Yongge Liu,Hong Hai,Jianping Li

A novel electrochemiluminescence(ECL) aptamer biosensor with high sensitivity and selectivity for the detection of tumor biomarker carbohydrate antigen CA125 was constructed, and a strategy of triple amplification of signals was proposed by using exonuclease cyclic cleavage aptamer, combined with rolling ring amplification technologies, generating multi-branched dendritic double-stranded DNA to load a large number of probes through "strand self-growth". The double-stranded DNA, which abbreviated as CP/CA dsDNA, formed by hybridizing the single strand of capture DNA (CP DNA) with the single strand DNA of the CA125 aptamer(CA Apt) was modified on the Fe3O4@Au. When the carbohydrate antigen CA125 was added, CP/CA dsDNA were unwound, and CA125 specifically combined with CA Apt to form a protein-aptamer complex, leaving only CP DNA on the surface of the Fe3O4@Au. RecJf exonuclease cleaved the aptamer in the protein–aptamer complex and released CA125, which recombined to other CA125 aptamers, to form a cycle that produces more CP DNA on the Fe3O4@Au. Three ssDNA (H1, H2, H3) were introduced and hybridized with CP DNA to form a dsDNA with "+" configuration structure. Then phi29 DNA polymerase, T4 DNA ligase, deoxy-ribonucleoside triphosphate (dNTPs) and padlock probes were added to form a large number of complementary strands of padlock probes (CS padlock probes) by rolling cyclic amplification. CS padlock probes were linked to the "+" type dsDNA; then the ssDNA H4 was added and hybridized with CS padlock probe to form multi-branched dendritic dsDNA. A large number of Tris(2,2'-bipyridyl)ruthenium(II) probes were embedded in the double strands, resulting in an extremely strong ECL signal in the presence of the co-reactant tri-n-propylamine (TPA). There is a linear relationship between the ECL signals and CA125 concentrations in the range of 1.0×10-15~1.0×10-8 mg/mL, and the detection limit was 2.38 × 10-16 mg/mL. It has been used for the determination of CA125 in serum samples.

研究领域: 生物传感器 · 分析化学 · 癌症标志物 · 分子生物学
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FOOD CHEMISTRY · 2026 · IF 10.4

Dual-signal cross-validation via ECL quenching and DPV oxidation on a MIP sensor: ultrasensitive detection of sulfadiazine in complex food matrices with a CD-COF core

Xuran Zhang,Rongxian Ma,Zhili Li,Jing Cao,Haoqi Ma,Yeyu Wu,Xuecai Tan,Kejing Huang

The excessive use of sulfadiazine (SDZ) poses significant health risks due to toxic residues in food and ecosystems. This work introduces a novel molecularly imprinted polymer (MIP) sensor featuring a carbon dot-based covalent organic framework (CD-COF) core as a high-performance electrochemiluminescence (ECL) emitter. Upon SDZ rebinding to imprinted sites, the sensor leverages SDZ's inherent redox activity to enable complementary differential pulse voltammetry (DPV) detection alongside ECL quenching. This dual-signal output establishes an intrinsic cross-validation mechanism that inherently corrects environmental interferences. The sensor achieves ultrasensitive detection of SDZ, with impressively low detection limits of 0.28 nM (ECL) and 1.6 nM (DPV). Validation in food matrices demonstrates exceptional accuracy and reliability, yielding recoveries of 91–110%. This study not only provides a robust tool for trace SDZ monitoring but also establishes a new paradigm for CD-COF-powered MIP sensors integrating dual-mode signals for highly reliable contaminant analysis in real-world samples.

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Polymer Chemistry · 2016 ·Vol. 7 ·期 37 ·5880-5887 · IF 5.687

Simultaneous utilization of a bifunctional ruthenium complex as an efficient catalyst for RAFT controlled photopolymerization and a sensing probe for the facile fabrication of an ECL platform

Tao Chen,Yuanhong Xu,Zhi Peng,Aihua Li,Jingquan Liu

Ruthenium (Ru)-complex (Ru(bpy)32+) catalyzed reversible addition–fragmentation chain transfer (RAFT) photopolymerization is an attractive technique for preparing polymer-functionalized biomaterials because of its gentle reaction conditions. Until now, negatively charged polymers prepared by this polymerization method have been seldom reported, which should be due to the difficulty in removing the positively charged catalyst Ru(bpy)32+ from the negatively-charged polymer owing to the strong electrostatic attraction between them. However, the difficulty in removing Ru(bpy)32+ from the negatively charged polymer should not always be regarded as just a shortcoming, on the contrary, it can be utilized as an advantage for developing a stable and efficient solid-state electrogenerated chemiluminescence (ECL) sensor. Herein, pyrene-functionalized poly(sodium p-styrene sulfonate) (PSS) was successfully synthesized by RAFT photopolymerization catalyzed via the Ru-complex based photoredox catalyst (Ru(bpy)32+) under visible light (λ = 460 nm). It turned out to be a well-controlled RAFT polymerization as evidenced by 1H NMR and gel permeation chromatography (GPC) analyses. Based on the stable electrostatic attraction of Ru(bpy)32+ with PSS and a non-covalent π–π stacking interaction between the pyrene moiety and the highly oriented pyrolytic graphite surface, a stable and efficient solid-state ECL sensor was successfully fabricated. The as-proposed sensor was investigated using tripropylamine as a representative analyte and a low detection limit of 0.1 nM (S/N ≥ 3) was reached. It also exhibited excellent reproducibility (relative standard deviations of 0.56% for 112 continuous cycles) and long-term stability (about 90% of its preliminary ECL intensity can be retained after intermittent use over a 90-day period).

研究领域: 材料科学 · 分析化学 · 高分子化学 · 电化学
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ANALYST · 2020 ·Vol. 146 ·期 4 ·1295-1302 · IF 3.978

A novel signal amplified electrochemiluminescence biosensor based on MIL-53(Al)@CdS QDs and SiO2@AuNPs for trichlorfon detection

Defen Feng,Fucun Wei,Yeyu Wu,Xuecai Tan,Fang Li,Yongkuai Lu,Gaochao Fan,Heyou Han

An ultrasensitive electrochemiluminescence (ECL) biosensor was developed based on MIL-53(Al)@CdS QDs and SiO2@AuNPs for trichlorfon detection. Metal–organic frameworks (MOFs) were used as a loading platform that provided a large surface area to load targets and modified materials onto the electrode. At the same time, SiO2@AuNPs loaded plenty of AuNPs which effectively increased the ECL resonance energy transfer between the CdS QDs, so that the ECL signal was strongly quenched and resulted in an amplified response. In the range of 10−11–10−4 M, the ECL response showed a linear relationship with the concentration (logarithm) of trichlorfon, and the detection limit was 5.1 × 10−12 M (S/N = 3). When the biosensor was applied to detect trichlorfon in lettuce, broccoli, cucumber, and chives, the recoveries obtained from the spiked samples were 97%–105%, 102%–104%, 100%–104%, and 98%–104%, respectively. Thus, this novel ECL biosensor has potential applications for the analysis of trichlorfon in food samples.

研究领域: 分析化学 · 环境科学 · 材料科学 · 食品安全
✓ 已验证 DOI PubMed 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Electrogenerated chemiluminescence method for sensitive detection of hydroxylated double-stranded DNA through multifunctional polyadenine probe and hybridization chain reaction

Wanqiao Bai,Wenyu He,Huan Wang,Sijia Li,Xia Yang,Huiping Sun,Yan Li

5-Hydroxymethylcytosine (5-hmC), as the sixth base in the mammalian genome, is increasingly regarded as an epigenetic marker with crucial biological functions. Herein, a highly sensitive electrogenerated chemiluminescence (ECL) sensing platform for double-stranded DNA containing 5-hmC (5-hmC-dsDNA) in genome was fabricated, which based on polyadenine-gold interaction combining with signal amplification of hybridization chain reaction (HCR). This biosensing strategy could be executed to detect 5-hmC in the native double-stranded DNA, irrespective of the specific sequences of DNA. Firstly, DNA methyltransferase (M.HhaI) was introduced to chemically modify the hydroxyl of 5-hmC in double-stranded DNA, which converted 5-hmC-dsDNA to amino-derived 5-hmC-dsDNA. Subsequently, DNA sequence containing polyadenine (polyA) was used as an anchor probe to incorporate the derivatized 5-hmC-dsDNA by amide reaction to form compound DNA and then completely assembled onto the gold electrode surface through preferential polyA-gold interaction. Subsequently, two designed DNA hairpin probes which can alternately hybridize with each other were linked to the signal amplification part of multifunctional polyA probes, forming ultra-long nicked double helix structures. Finally, ECL indicator of Ru(phen) 3 2+ molecules were intercalated into the groove of the nicked DNA double helices, resulting greatly increased ECL intensity. Therefore, the quantitatively analysis of 5-hmC-dsDNA could be obtained relied on the relationship between the ECL intensity and 5-hmC-dsDNA content. The detection limit of this method for 5-hmC-dsDNA was 0.0001 % (S/N = 3). Moreover, the biosensing platform was successfully applied to detect 5-hmC-dsDNA in mice tissue samples with satisfactory results, manifesting its great potential application in clinical analysis.

研究领域: 生物化学 · 分子生物学 · 分析化学 · 基因组学
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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

Dual-signal amplification strategy for electrochemiluminescence sandwich biosensor for detection of thrombin

Yingjie Li,Yuqin Li,Ning Xu,Jiahong Pan,Tufeng Chen,Yaowen Chen,Wenhua Gao

In the present study, the authors report a novel sandwich biosensor for detection of thrombin using electrochemiluminescence method based on dual-signal amplification strategy. Firstly, the gold nanoparticles graphene composite (GNPs-graphene) was obtained by simultaneously depositing the chloroauric (III) acid tetrahydrate [HAuCl 4 ·4H 2 O] and graphene solution with a cyclic voltammetry. Secondly, one thiol-modified thrombin aptamer (TBA1) was immobilized the glassy carbon electrode (GCE) via Au-S bonding. And then the other thiol-modified biotinylated thrombin aptamer (TBA2) that were modified with Ru(bpy) 3 2+ were anchored on the surface of the gold nanoparticles in solution. This proposed assay took dual signal amplification strategies. On the one hand, a single gold nanoparticle can connect many TBA2 to come into being a signal cluster (Ru-TBA2-AuNPs), thus when a little thrombin were present the system the ECL intensity will have a strong signal response; On the other hand, the GNPs-graphene can promote the electron transfer efficiency and increase the signal response. The ECL signal had a good linear relationship with thrombin concentration in range of 0.01–10   nM, and the detection limit for thrombin was determined to be as low as 6.3 pM. This biosensor also showed good selectivity for thrombin without being affected by some other proteins, such as BSA and lysozyme and so on. Moreover, this proposed method was successfully applied to thrombin analysis in diluted human serum samples.

研究领域: 生物化学 · 分析化学 · 纳米技术 · 生物医学工程
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

g-C3N4-heme bound to amyloid β peptides: In-situ generation of the secondary co-reactant for dual-enhanced electrochemiluminescence assay of amyloid β detection

Mengjie Zhang,Zixuan Chen,Haixin Qin,Xiaoyan Yang,Wei Cao,Shufeng Liu

Abtract Heme binds to amyloid β -peptide (A β ) in the brain of Alzheimer΄s disease (AD) patients, thus forming heme-A β complexes and leading the characteristic pathological features of AD. The heme-A β complexes reduce O 2 by 2e − to obtain co-reactant H 2 O 2 . In this work, two-dimensional graphite-like carbon nitride (g-C 3 N 4 ) was hybridized with heme via π-π interaction to construct an electrochemiluminescence (ECL) biosensor for detection of A β peptides. The capture aptamer was firstly immobilized on the gold electrode, and then incubated with target A β peptides and g-C 3 N 4 -heme. The g-C 3 N 4 -heme-A β composite was subsequently anchored on the electrode and showed a signal-on, label-free ECL emission based on dual co-reactants enhancement attributed to in-situ generated H 2 O 2 and original K 2 S 2 O 8 in PBS buffer. Under the optimum experimental conditions, the ECL biosensor has a sensitive response to A β peptides with a linear range of 10 fM-0.1 μM and a detection limit of 3.25 fM. Considering prominent specificity, reproducibility, and stability, the proposed biosensor was used to assess recovery of A β peptides in human serum and the result was satisfactory. We believe that the established method would offer a useful analytical means for quantifying A β peptides in a biological matrix.

研究领域: 生物化学 · 分析化学 · 神经科学 · 材料科学
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ANALYST · 2020 ·Vol. 145 ·期 10 ·3569-3574 · IF 3.978

A portable electrochemiluminescence bipolar electrode array for the visualized sensing of Cas9 activity

Rui Guo,Shanwen Hu,Zonghua Wang

CRISPR/Cas9 has become a powerful tool for genomic manipulation, and the evaluation of the Cas9 activity is essential for the precise control of the CRISPR system. Herein, we develop a point-of-care platform for the rapid and visible determination of the Cas9 activity. A bipolar electrochemiluminescence (ECL) biosensor platform comprises an Au electric circuit fabricated on a glass substrate and the PDMS layer acts as a reservoir. DNA probes are then modified on electrodes and hybridization chain reaction (HCR) is applied to introduce ferrocene-labeled DNA. The CRISPR/Cas9 system can recognize the immobilized DNA probes and cleave them from the electrode surface as well as the labeled H1 and H2. Therefore, the cleavage activity is closely related to the labeled ferrocene. The modified electrode is then embodied in a closed bipolar system such that the oxidation reaction on sensing poles could be detected by the anodic ECL reactions on isolated luminescent poles due to charge balance, leading to the changes in ECL signals. This portable, integrated and convenient platform may become a meaningful tool for the discovery of a new CRISPR/Cas9 system or additional Cas9 inhibitors.

研究领域: 生物技术 · 分子生物学 · 分析化学
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ANALYTICAL CHEMISTRY · 2020 · IF 6.785

Kill Three Birds with One Stone: Poly(3,4-ethylenedioxythiophene)-Hosted Ag Nanoclusters with Boosted Cathodic Electrochemiluminescence for Biosensing Application

Yamin Nie,Xiuli Tao,Ying Zhou,Xiaoding Yuan,Ying Zhuo,Ya-qin Chai,Ruo Yuan

Metal nanoclusters (NCs) have attracted extensive interest in electrochemiluminescence (ECL) field, but it is still a significant challenge to prepare high ECL efficiency NCs, which tremendously precludes their application in sensing and imaging. Herein, we report poly(3,4-ethylenedioxythiophene) (PEDOT) as a functional ligand for NCs with a “kill three birds with one stone” role, acting as a stabilizer like existing templates, excitingly, excellent electrical conductivity to accelerate the injection of interfacial electrons, and outstanding electrocatalytic activity toward coreactants (S2O82–), which breaks the convention that traditional ligands act as a double-edged sword in ECL field. As an illustration, PEDOT-hosted Ag NCs were prepared with an unprecedented ECL intensity with S2O82– as a cathodic coreactant, which indicates that this novel ligand strategy will bring exciting opportunities, not only in opening up new horizons for rational development of high ECL efficiency metal NCs but also in advancing their potential applications in light-emitting devices and clinical biosensing. As a proof of concept, the PEDOT-hosted Ag NCs were applied as neoteric ECL emitters to achieve sensitive detection of dopamine (DA), which showcased a wide linear response from 1 nM to 10 mM and a low detection limit of 0.17 nM.

研究领域: 材料科学 · 分析化学 · 纳米技术 · 生物医学工程
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