Fundamental Research
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2021
·
IF 0
Ping Zhou,Shujie Hu,Weiliang Guo,Bin Su
Electrochemiluminescence (ECL) of luminol is a luminescence process that proceeds in the presence of reactive oxygen species (e.g. hydrogen peroxide (H 2 O 2 )) at a suitable electrode potential, the reaction mechanism of which is complicated and remains ambiguous. In this work, we report a visualization approach for measuring the thickness of the ECL layer (TEL) of the luminol/H 2 O 2 system to decipher the reaction process by combined use of the microtube electrode, ECL microscopy, and finite element simulations. With the increase of solution pH, the ECL image captured with the microtube electrode tends to vary from spot to ring, corresponding to the decrease of TEL from >9.1 μm to ca. 4.3 μm. We propose that different intermediates are involved in the course of ECL reaction. At a low pH (e.g. pH < 9), a relatively large TEL is most likely determined by the diffusion of oxidized and deprotonated luminol intermediate that is neutral and has a long lifetime. While at a high pH (e.g. pH in the range of 10 to 12), the ECL reaction is controlled by short-lived radical intermediates of both luminol and superoxide anion. The proposed mechanism is proved theoretically by finite element simulations and experimentally by the apparent effect of concentration ratio of luminol/H 2 O 2 .
研究领域:
分析化学
·
电化学
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MICROCHIMICA ACTA
·
2025
·Vol. 193
·期 1
·32
·
IF 5.3
Shi Xiao-Jie,Wang Yue,Wang Lin,Zhang Ting-Ting,Song Tian-Shun,Li Xiang-Ling,Xie Jing-Jing
Electrochemiluminescence (ECL) based on the luminol-O 2 system is attractive for biosensing, yet its efficiency under neutral conditions remains extremely limited due to the poor reactivity of dissolved oxygen. Herein, we develop a phosphorus-doped cerium single-atom catalyst (Ce-N/P-C SAC) that significantly enhances luminol-O 2 ECL in neutral media. The introduction of P atoms effectively modulates the electronic structure of Ce sites, promotes the Ce 3+ /Ce 4+ redox cycle, and accelerates the one-electron oxygen reduction reaction to generate abundant ·O 2 ⁻, leading to a 12.73-fold ECL enhancement compared with the bare electrode and a 2.13-fold increase over undoped Ce-N-C. Based on these catalytic properties, a highly sensitive ECL platform was constructed for the detection of gallic acid, achieving a wide linear range (10 nM − 10 µM) and a low detection limit of 7.42 nM. This work provides an efficient strategy for boosting neutral-pH luminol-O 2 ECL and demonstrates the practical potential of rare-earth single-atom catalysts in antioxidant determination and bioanalytical sensing.
Section
Graphical abstract
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高影响因子
ACS Omega
·
2021
·
IF 3.512
Weifeng Chen,Liwei Cui,Yanyan Song,Wei Chen,Yuan Su,Weidan Chang,Wentao Xu
A capture probe was constructed using a combination of magnetic Fe3O4 nanoparticles and an aptamer directed towardListeria monocytogenes. A signal probe was prepared by combining luminol-functionalized flowerlike gold nanoparticles, obtained by combining luminol with chitosan bearing a complementary sequence of the aptamer. The complex consisting of the capture probe and signal probe could be removed through magnetic separation. Where the target was present within a sample, it competed with the complementary sequence for binding to the aptamer, causing a change of the chemiluminescent signal. The results indicated that a good linear relationship existed over the concentration range 1.0 × 101–1.0 × 105 CFU·mL–1. It was established that it was feasible to use this approach to detect L. monocytogenes at levels as low as 6 CFU·mL–1 in milk samples.
研究领域:
食品科学
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微生物学
·
纳米技术
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Catalysts
·
2024
·Vol. 14
·期 12
·895
·
IF 3.8
Kuangjun Li,Yuting Li,Rong Feng,Jing Wu
Chemiluminescence (CL) is regarded as a better method for the detection of reactive oxygen species (ROS). However, the weak CL intensity prevents its further application. Many nanomaterials have been developed to enhance CL intensity, and mixed-ligand MOFs incorporating additional metals or organic ligands exhibit high efficiency in catalyzing. In this work, one kind of bimetallic mixed-ligand metal–organic framework (Ni-Co m-MOF) was synthesized using solvothermal methods. The material was morphologically characterized and demonstrated to be a dense and spherical flower-like structure. The addition of Ni-Co m-MOFs significantly enhanced the CL intensity of the luminol-H2O2system by nearly 2,000-fold. The enhancement was found through further research as hydrogen peroxide was catalyzed to create hydroxyl radicals, etc., which reacted more easily with luminol. Herein, significant enhancement of the CL system by Ni-Co m-MOFs was identified, which provides ideas for improving the sensitivity and signal-to-noise ratio development of CL detectors.
研究领域:
分析化学
·
纳米材料科学
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Solomon Sime Tessema,Hongzhan Liu,Shiyu Xia,Tadele Eticha,Mohammed Yahya Suleiman,Yu Tian,Guobao Xu
A chemiluminescence (CL) system with high intensity and long-lasting emission is crucial for accurate CL measurements. The luminol/hydrogen peroxide (H 2 O 2 ) CL system has recently attracted significant attention. However, the CL emission from the luminol/H 2 O 2 system is typically weak, which limits its application for quantitative measurements. In this study, we synthesized a high-entropy metal–organic framework nanosheet (HE-MOFs) containing five homogeneous and nearly equally dispersed metal ions using a solution-phase strategy at room temperature. The resulting HE-MOFs exhibited exceptional peroxidase-mimicking catalytic activity. Their intrinsic peroxidase-like properties allowed HE-MOFs to efficiently catalyze H 2 O 2 , generating reactive oxygen species (ROS) and producing a strong, efficient, and stable CL emission in the luminol/H 2 O 2 /HE-MOFs system. The remarkable enhancement of CL emission can be attributed to the synergistic effects of the multi-metal ions in the unique crystal structure of HE-MOFs. Consequently, we developed a fast, sensitive, and selective luminol/H 2 O 2 /HE-MOFs CL sensor to detect dopamine (DA), leveraging the potential inhibitory effect of DA on CL emission. This sensor effectively detected dopamine and demonstrated good linearity over a 10–500 nM concentration range, with a low detection limit (LOD) of 3.90 nM (S/N = 3). As a proof of concept, we applied the method to detect DA in real samples, achieving excellent recoveries ranging from 95 % to 105 % (RSD < 1.19 %, n = 3). Our findings provide a new perspective on designing high-entropy-based MOFs nanozymes and lay the groundwork for developing highly sensitive CL biosensors for real-time bioassays.
研究领域:
分析化学
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生物传感
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材料科学
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高影响因子
TALANTA
·
2020
·
IF 5.339
Xi Ju Yang,Rong Sheng Li,Chun Mei Li,Yuan Fang Li,Cheng Zhi Huang
Cobalt oxyhydroxide nanoflakes (CoOOH NFs), a typical two-dimensional (2D) nanomaterials , were found to induce chemiluminescence (CL) of luminol since the oxidase-like activity of CoOOH NFs enables the dissolved oxygen to generate various radicals ( OH, O 2 − and 1 O 2 ) even if without the addition of oxidants such as hydrogen peroxide, and these radicals could be scavenged by glutathione (GSH), making GSH could be detected sensitively in the range of 10 nM to 1 μM with the detection limit of 6.4 nM.
研究领域:
生物分析化学
·
纳米材料科学
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高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Li He,Zhe Wei Peng,Zhong Wei Jiang,Xue Qian Tang,Cheng Zhi Huang,Yuan Fang Li
Novel metal–organic gels (MOGs) consisting of iron (Fe3+) as the central ion and 1,10-phenanthroline-2,9-dicarboxylic acid (PDA) as the ligand were synthesized by a mild facile strategy. The Fe(III)-containing metal–organic xerogels (Fe–MOXs), obtained after removing the solvents in MOGs, were found to exhibit outstanding performance in the catalysis of luminol chemiluminescence (CL) for the first time even in the absence of extra oxidants such as hydrogen peroxide. The possible CL mechanism was discussed according to the electro/optical measurements, including electron paramagnetic resonance (EPR), UV–vis absorption, and CL spectra, as well as the effects of radical scavengers on Fe–MOXs-catalyzed luminol CL system, suggesting that the CL emission of luminol might originate from the intrinsic oxidase-like catalytic activity of Fe–MOXs on the decomposition of dissolved oxygen. Additionally, the potential practical application of the resulting luminol–Fe–MOXs system was evaluated by the quantitative analysis of dopamine. Good linearity over the range from 0.05 to 0.6 μM was obtained with the limit of detection (LOD, 3σ) of 20.4 nM and acceptable recoveries ranging from 98.6 to 105.4% in human urine. These results may open up the promising application of novel metal–organic gels as highly effective catalysts in the field of chemiluminescence.
研究领域:
材料科学
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分析化学
·
生物医学工程
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SENSORS AND ACTUATORS B-CHEMICAL
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2015
·
IF 4.097
Haili Yu,Yi He,Wenhao Li,Tao Duan
We report that graphitic carbon nitride (g-C 3 N 4 ) nanosheets can enhance the chemiluminescence (CL) of luminol and hydrogen peroxide (H 2 O 2 ) system. The reaction mechanism of the luminol-H 2 O 2 -g-C 3 N 4 nanosheets system was investigated by CL spectrum, UV–vis absorption spectroscopy, and radical scavengers. The g-C 3 N 4 nanosheets-enhanced CL mechanism was attributed to the fact that g-C 3 N 4 nanosheets were able to catalyze the decomposition of H 2 O 2 to form reactive hydroxyl radical. The produced hydroxyl radical further reacted with luminol and H 2 O 2 anion, generating a light emission. Moreover, 2,4,6-trinitrotoluene (TNT) was observed to inhibit the CL effectively. On this basis, a sensitive and selective sensing approach was successfully developed for the detection of TNT. The linearity ranged from 1 pM to 1 nM with a detection limit of 0.75 pM based on a signal-to-noise ratio of 3. This sensitivity increased about six orders of magnitude over that of g-C 3 N 4 nanosheets-based fluorescence sensor.
研究领域:
分析化学
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环境科学
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材料科学
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高影响因子
ANALYST
·
2016
·Vol. 141
·期 6
·2061-2066
·
IF 4.033
Man Li,ZhuanZhuan Shi,ChangMing Li,Ling Yu
The complement fixation test (CFT) is a serological test that can be used to detect the presence of either a specific antibody or antigen to diagnose infections. In a conventional CFT, the assay result is determined by observing the clarity of the reaction solution or the sediment of red cells by the naked eye. Although the assay conditions are thereafter simplified, the sensitivity of the assay would be sacrificed due to the limitation of bulk observation. Inspired by the forensic scientists to examine blood at the scene of the crime, we rationally argued that the luminol chemiluminescence (CL) reaction could be applied in the CFT to sense physiological complement-mediated haemolytic phenomena for sensitive protein detection. The combination of the CFT and the luminol CL system was demonstrated in detection of rH7N9, a recombinant avian influenza virus protein. The testing can be accomplished within 2.5 h and the linear detection range covers 0.25 fg mL−1 to 25 ng mL−1. The feasibility of the CL based CFT in assaying a real biopsy was successfully demonstrated by specifically detecting rH7N9 and the carcinoembryonic antigen (CEA) in human serum. This new type of protein detection approach inherits the beauty of complement-mediated assay, such as being fast, and no protein immobilization, blocking and washing. In addition, the participation of luminol CL enables us to quantitatively analyse the intensity of a haemeolysis process, ameliorating the limitation of bulk observation in traditional CFT. It is anticipated that the luminol CL-CFT assay would be particularly suitable for investigation of small molecules, toxins, and short peptides.
研究领域:
免疫学
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分子生物学
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病毒学
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分析化学
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 10
·1-11
·
IF 5.3
Chen Wenxia,Hu Shuangyi,Zhou Bingqian,Ren Yueran,Xue Yangyang,Yang Rui
Lung cancer, as one of the cancers with the highest morbidity and mortality rates in the world, requires accurate detection of its vital serum marker, neuron-specific enolase (NSE), which is a key challenge for early detection of lung cancer. However, traditional chemiluminescence immunoassay (CLIA) methods rely on labeled antibodies (Abs) and suffer from complex operations and high costs. In this work, a label-free CLIA based on CL-functionalized mesoporous magnetic nanoparticles (CuFe 2 O 4 @mSiO 2 -Cys-Luminol-Au NPs) is developed for the rapid and sensitive detection of NSE. The material combines the advantages of magnetic separation, mesoporous loading, catalytic enhancement, and biorecognition. CuFe 2 O 4 NPs offer efficient magnetic separation, while the mesoporous silica (mSiO 2 ) layer is effectively loaded with luminol to amplify CL signals. L-cysteine (L-Cys) ensures the uniform distribution of luminol and gold nanoparticles (Luminol-Au NPs), with these Au NPs immobilizing Abs through Au–S and Au–N bonds, achieving high-density biocoupling. The constructed label-free CLIA enables highly sensitive detection of NSE without Abs labeling. The results show that the NSE concentration is linearly correlated with the CL intensity in the range 1.0 × 10 −13 ~ 1.0 × 10 −8 g/mL, and the detection limit is as low as 2.3 × 10 −14 g/mL. The proposed method demonstrates excellent selectivity, stability, and anti-interference capability for the detection of NSE in human serum samples. Graphical
研究领域:
生物医学工程
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分析化学
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纳米技术
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癌症诊断
·
生物传感器
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Haidong Li,Zhenxing Yang,Nidong Yangan,Xianjing Huang,Danli Zhong,Zhenzhen Wang,Chengyin Wang
The efficient activation of molecular oxygen to generate reactive oxygen species (ROS) offers great promise for achieving potential-resolved electrochemiluminescence (ECL) in the luminol/O2 system, though it typically relies on sophisticated catalysts. In this work, we demonstrate that carbonized polydopamine nanospheres (C-PDANSs) serve as an effective metal-free electrocatalyst to enhance the oxygen reduction reaction (ORR), thereby enabling the potential-resolved ECL of luminol. Mechanistic studies indicate that the ORR catalyzed by C-PDANSs proceeds via a two-electron pathway, yielding both superoxide radicals (O2–•) and hydrogen peroxide (H2O2). This ORR behavior facilitates the generation of sufficient ROS, which significantly boosts both cathodic and anodic luminol ECL, leading to 11.6-fold and 5.1-fold intensity enhancements, respectively. Based on the dual-potential ECL response, a ratiometric sensing platform was constructed for the detection of alkaline phosphatase (ALP). This study not only presents a different electrocatalyst for regulating dual-potential luminol ECL but also opens the avenue for designing biosensing schemes.
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TALANTA
·
2026
·
IF 6.7
Weiqiang Chen,Qian Wang,Zhiying Jin,Tingting Zhang,Zihong Li,Yi Huang,Yushan Cai,Jianshe Huang,Xiurong Yang
A novel Co-based MOF (Co 2 DDA), was successfully synthesized. • Co 2 DDA enhanced luminol–H 2 O 2 chemiluminescence by about 6000-fold. • Co 2 DDA catalyzed H 2 O 2 to generate 1 O 2 , .•OH and O 2 •− under alkaline conditions. • A cascade catalytic CL platform based on ChOx and Co 2 DDA was developed for choline sensing. • Choline was detected from 5 to 150 μM with an LOD of 4.21 μM. A cobalt-based metal-organic framework (Co 2 DDA, DDA = 1,5-diamino-4,8-dihydroxy-9,10-anthracenedione) was synthesized in this study. Under the catalysis of Co 2 DDA, the chemiluminescence (CL) intensity of the luminol–H 2 O 2 system increased by approximately 6000-fold. The catalytic mechanism of Co 2 DDA was elucidated through CL spectrum, UV–vis absorption spectroscopy, radical scavenger experiments, and electron spin resonance (ESR) spectroscopy. The results demonstrated that Co 2 DDA exhibited excellent catalytic activity, facilitating the decomposition of H 2 O 2 under alkaline conditions and enhancing the production of reactive oxygen species (ROS), including 1 O 2 , •OH, and O 2 •− . These ROS rapidly react with luminol to produce the excited-state oxidation product 3-aminophthalate anion (3-APA*), which emits strong CL at 440 nm when transitioning to the ground state. Under the cascade catalysis of choline oxidase (ChOx) and Co 2 DDA, the system exhibited a remarkable response toward choline. Based on this finding, a sensitive CL method for the detection of choline was developed. Under optimized conditions, the proposed CL system showed a good linear relationship in the concentration range of 5–150 μM, with a detection limit as low as 4.21 μM (3 σ /K). Significantly, this strategy can be further extended to the detection of other biomolecules that generate H 2 O 2 as a reaction product. Download: Download high-res image (299KB) Download: Download full-size image
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