ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Abubakar Abdussalam,Hongzhan Liu,Islam Mohamed Mostafa,Baohua Lou,Dmytro Viktorovych Snizhko,Yuriy Tymofiiovych Zholudov,Wei Zhang,Guobao Xu
Chemiluminescence (CL)-based analytical methods utilize luminophores that need to be activated with an oxidizing agent to trigger CL emission. Despite its susceptibility to decomposition when exposed to external light or trace metals, hydrogen peroxide (H2O2) has been widely used to develop chemiluminescent methods due to the limited number of suitable alternatives for activating chemiluminescent luminophores. Also, analytical methods based on the well-known luminol/H2O2 CL system have low sensitivity. Dissolved oxygen (DO) is a naturally abundant and environmentally benign alternative oxidant for luminol and other CL luminophores. However, DO alone is inactive and needs an efficient catalyst or a coreaction accelerator for its activation. Because of the narrow bandgap of VS4 (ca. 1.12 eV), it can facilitate fast electron-transfer kinetics with an acceptor molecule such as DO. Here, we introduce vanadium tetrasulfide (VS4) to boost CL for the first time. Under the optimized conditions, VS4 nanodendrite catalyzes the generation of reactive oxygen species by activating DO which subsequently reacts with luminol to generate intense CL. It enhances the CL intensity of luminol/DO by about 10,000 times. Surprisingly, hemin remarkably quenches the generated CL of luminol/DO/VS4 nanodendrites, which is completely opposite to its typical enhancement of luminol CL. Based on the remarkable concentration-dependent quenching of the luminol/DO/VS4 nanodendrite CL by hemin, we have developed a sensitive CL method that can selectively detect hemin in the linear concentration range of 1–250 nM and achieved a limit of detection of 0.11 nM. The practical utility of the developed method was demonstrated by the determination of hemin in a pharmaceutical drug for the treatment of acute intermittent porphyria and in human serum. This study demonstrates that VS4 holds great promise in analytical method development.
研究领域:
分析化学
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环境科学
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
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2025
·
IF 10.5
Hang Ao,Jinshan Xiong,Wencheng Xiao,Wenrui Hu,Jie Wu,Huangxian Ju
Owing to the continuous mutations of the coronavirus, the sensitive and accurate detection of the SARS-CoV-2 nucleocapsid protein is still necessary in clinical diagnosis. Aim to the challenge of sensitivity in chemiluminescence (CL) imaging detection and the need for high-throughput clinical screening, this work used imidazole (Im) as an enhancer for hemin-DNA/luminol/H 2 O 2 CL system to propose a CL imaging method for SARS-CoV-2 nucleocapsid protein detection. In this system Im could reduce the hemin-DNA catalyzed oxidation energy of luminol by H 2 O 2 to promote the CL emission through the accelerated breaking of O-O bond of dianionic cyclic peroxide. The enhancement mechanism was demonstrated with theoretical calculations and several characterization techniques. By combining the proximity-induced initiator release with immunological recognition, an initiator-triggered DNA nanomachine was designed to achieve the release of abundant primers for activating hemin-DNA switch. This signal amplification strategy led to strong CL emission for highly sensitive imaging detection of the target. The Im-enhanced hemin-DNA/luminol/H 2 O 2 CL imaging assay exhibited a linear detection range over 4 orders of magnitude with a detection limit down to 2.75 pg/mL for SARS-CoV-2 nucleocapsid protein, exhibiting promising potential of both Im sensitization and the proposed DNA nanomachine to improve the sensitivity of high-throughput CL biosensing for the early diagnosis and clinical screening of the coronavirus and other diseases.
研究领域:
生物分析化学
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生物传感器
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临床诊断
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病毒学
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纳米生物技术
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Hongchao Ma,Xifeng Ma,Tiantian Dong,Xinyu Bian,Xiaokang Zhang,Yanhui Wei
Bioinspired nanozymes hold promise for simulating natural processes and creating optimized functional systems, but their application is hindered by limited catalytic activity and selectivity. These challenges can be addressed by reconstructing enzymatic active sites to enhance catalytic efficiency and integrating biological recognition units for specificity. In this work, we developed a peroxidase-mimicking nanozyme by stabilizing hemin on a supramolecular scaffold of diphenylalanine (FF) and glutaraldehyde (GA). To enable specific recognition, we conjugated a tetrodotoxin (TTX) aptamer, yielding the He@FF/GA-Apt composite nanozyme. This nanozyme demonstrated robust catalytic activity in 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation. The TTX aptamer conferred specific TTX recognition, with the aptamer-TTX complex blocking the nanozyme active site and reducing its activity. Based on this mechanism, we created a dual-mode TTX detection method using UV–vis spectroscopy and smartphone RGB analysis. The UV–vis mode achieved a linear range of 1.0–40.0 ng mL −1 and a limit of detection (LOD) of 0.61 ng mL −1 , while the smartphone mode had a LOD of 1.43 ng mL −1 in a linear range of 2.0–40.0 ng mL −1 . Both methods performed well in real samples, with recoveries of 96.29 %–102.57 % (UV–vis mode) and 92.07 %–109.46 % (RGB mode). In comparation, the UV–vis mode offers high sensitivity but requires lab equipment, whereas smartphone RGB mode enables rapid on-site detection despite a little lower sensitivity. This work provides a promising approach for developing target-specific nanozyme sensors.
研究领域:
生物化学
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分析化学
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纳米技术
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PubMed
高影响因子
ANALYST
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2018
·Vol. 143
·期 11
·2501-2507
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IF 3.864
Yong Liu,Xiaolin Xu,Haitang Yang,Ensheng Xu,Shuangshuang Wu,Wei Wei,Jin Chen
Poly(ADP-ribose) polymerase-1 (PARP-1) is a highly conserved nuclear enzyme, which binds tightly to damaged DNA and plays a key role in DNA repair, recombination, proliferation, and genomic stability. However, due to the poor electrochemical and optical activity of PARP-1 and its product PAR, only a few studies on its activity detection method have been reported. Herein, we report a simple and sensitive colorimetric strategy to monitor PARP-1 activity based on enzyme-initiated auto-PARylation-controlled aggregation of hemin-graphene nanocomposites (H-GNs). PARP, activated by dsDNA, catalyzed its substrate nicotinamide adenine dinucleotide (NAD+) to polymerize as a poly(ADP-ribose) polymer (PAR). PAR possesses several negative charges, and its charge density is twice that of a single-stranded DNA, which greatly impacts the dispersibility of H-GNs; due to their peroxidase-like catalytic activities, H-GNs can catalyze the chromogenic reaction of TMB and H2O2. As a result, in the presence of different PARP-1 activities, the supernatant of the corresponding solution contained different amounts of dispersed H-GNs and showed different colors after the chromogenic reaction that could be discerned easily by the absorbance or the color changes of the solution. The method was simple, sensitive, and reliable. The proposed method displays a linear range from 0.05 to 1 U with a detection limit of 0.03 U. In addition, this new method has been successfully applied to detect PARP-1 activity in human serum and different cancer cells and evaluate PARP-1 inhibitors.
研究领域:
生物化学
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分子生物学
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癌症研究
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纳米技术
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
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2017
·
IF 7.78
Yongmei Wu,Lina Zou,Sheng Lei,Qian Yu,Baoxian Ye
In this work, we first conjugated a short peptide to thrombin binding aptamer (TBA) and bond hemin to the hybrid, effectively rendering hemin/G4-peptide more active over the original hemin/G4, so that a highly sensitive electrochemical thrombin (TB) aptasensor was developed based on it and [email protected] nanocomposite . It was the first report on the application of hemin/G4-peptide in electrochemical aptasensor. [email protected] with large surface area served as excellent nanocarrier for high loading of hemin/G4-peptide hybrids, resulting in the formation of hemin/G4-peptide– [email protected] bioconjugate as the secondary aptamer and further signal enhancement. The specific affinity of aptamer for target TB made the secondary aptamer go into the sensing interface, and then a noticeable current signal was obtained from hemin without additional redox mediators . Due to the collaborative electrocatalysis of hemin/G4-peptide and PtNTs toward H 2 O 2 , which was formed in situ during the process of hemin/G4-peptide-catalyzed oxidation of NADH with dissolved O 2 , the current intensity increased dramatically. Such an electrochemical aptasensing system could be used to detect TB with a linear range of 0.05 pM–60 nM and very lower detection limit of 15 fM. Notably, this method exhibited a higher sensitivity than that of many hemin/G4-based electrochemical strategies for TB detection due to the improvement of the catalytic activity of hemin/G4-peptide. The present works opened a new way for expanding the application of hemin/G4 in biological detection. With the mediator-free, proteinous enzyme-free yet high-sensitivity advantages, this electrochemical aptasensor held great promise for other biomarker detections in clinical diagnostics.
研究领域:
生物化学
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分析化学
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生物医学工程
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电化学
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PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2011
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IF 1.77
Wenwen Liu,Wei Cao,Weihua Liu,Kang Du,Pixue Gong
This study established a novel flow injection (FI) methodology for the determination of phenol in aqueous samples based on luminol chemiluminescence (CL) detection. The method was based on the inhibition that phenol caused on the hemin-catalysed chemiluminescence reaction between luminol and hydrogen peroxide in alkaline solution. Optimum conditions and possible mechanisms have been investigated. The linear range was 2.0 × 10 −9 to 4.0 × 10 −7 g mL −1 for phenol. The proposed method is sensitive with a detection limit of 4.0 × 10 −10 g mL −1 . The relative standard deviation for 11 measurements was 2.3% for 1.0 × 10 −7 g mL −1 phenol. The method was applied for the determination of phenol in waste water samples. The results obtained compared well with those by an official method.
研究领域:
分析化学
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环境科学
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DOI
PubMed
高影响因子
ANALYST
·
2023
·
IF 4.2
Wei Li,Huili Wang,Xinxin Ying,Zhen Liang,Jianna Li,Xiangjuan Chen,Lei Su,Xueji Zhang
Zr-metal–organic frameworks (Zr-MOFs) have received increasing interest for their use as the signal marker in the development of sandwich-structured aptasensors for the detection of exosomes. However, Zr4+ ions of the Zr-MOFs can interact with not only the exosomes, but also the aptamers, leading to possible false positives and a large background response. In the present study, we report for the first time aptasensors with Pd nanoparticle (NP)-decorated and hemin-embedded UiO-66 MOFs serving as the signal amplification marker to eliminate false positives and decrease the background response of aptasensors. To construct aptasensors for detection of exosomes, CD63-specific aptamers were tethered onto magnetic Fe3O4 particles coated with polydopamine (PDA) and UiO-66-NH2 using glutaraldehyde crosslinking for capturing the exosomes. To prepare highly catalytic Zr-MOF-based signal markers, UiO-66 MOFs were modified with hemin followed by Pd NPs. The as-prepared Pd-decorated hemin-embedded MOFs showed high catalytic activity towards the chromogenic oxidation reaction of TMB by H2O2. Moreover, the decoration with Pd NPs led to the change of the surface charge state of the catalytic hemin-embedded UiO-66 MOFs from positive to negative, weakening the interaction between the signal marker and the negatively charged aptamers. Therefore, the as-prepared aptasensors showed an improved sensing performance towards exosomes with a linear concentration range from 4.28 × 102 to 4.28 × 105 and a limit of detection (LOD) of 86.2 particles per μL. The as-prepared aptasensors also showed high sensitivity and selectivity to the exosomes from different origins including the HeLa cell line and MCF-7 cell line.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lei Qin,Wenjing Chen,Yukui Fu,Jing Tang,Huan Yi,Ling Li,Fuhang Xu,Mingming Zhang,Weicheng Cao,Danlian Huang,Cui Lai
Heterogeneous electro-Fenton (HEF) technology has become a hot topic for degradation of organic pollutants in water. However, it remains a challenge to design effective catalysts for high H 2 O 2 utilization and pollutant degradation. In this work, we explored a novel iron and nitrogen-doped carbon catalyst derived from hemin (Fe-N-C) using KHCO 3 -MgO as dual-porogen. The results suggested that the KHCO 3 -MgO dual-porogen could not only improve the porous characteristics of catalyst, but also expose iron sites and change the proportion of nitrogen species. The pollutant degradation results demonstrated that the Fe-N-C-700/HEF system exhibited high ciprofloxacin degradation efficiency of 93.82% within 50 min and mineralization efficiency of 87.87% within 90 min by low energy consumption. Moreover, cycle experiments and metal ions leaching experiments revealed that the catalyst had good stability and recyclability. Electron spin resonance (ESR) test and radical capturing experiment showed that • OH was the dominant active species in this HEF system. In addition, the Fe-N-C-700/HEF system achieved satisfactory performance in the treatment of real water matrix, indicating the possibility for practical application in wastewater purification.
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高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Hang Ao,Wencheng Xiao,Wenrui Hu,Jie Wu,Huangxian Ju
This work designed a DNA conformation-regulated hemin switch for rapid chemiluminescent (CL) detection of a monoclonal antibodies. This switch was performed with an affinity probe and an inhibition probe, which were conveniently prepared by hybridizing hemin-labeled DNA1 with KHL peptide-labeled DNA2 and binding biotin-labeled DNA3 to streptavidin, respectively. In the absence of the target antibody, streptavidin-DNA3 could hybridize with hemin-DNA1/KHL-DNA2 to release KHL-DNA2, which led to the loss of hemin activity due to the affinity hindrance of streptavidin-DNA3. After the KHL peptide was recognized by the target antibody, the strand replacement hybridization could be inhibited by the bound antibody, which retained the high catalytic activity of hemin overhung on the antibody-bound affinity probe for a CL reaction, leading to a “signal-on” process for CL antibody detection. Using a KHL-specific antibody, anti-proprotein convertase subtilisin/kexin type 9 antibody (PCSK9-Ab), as a target model and common L012–1,2,4-triazole–H2O2 CL system, the designed switch showed a detection range of 10 ng mL–1 to 1 μg mL–1 with a detection limit of 4.16 ng mL–1 (56.2 pM) and a short analytical time of 6.5 min. The proposed quick method could simply be used for lab-on-chip CL detection of PCSK9-Ab in situ-secreted from PCSK9-6E3 hybridoma cells, which showed an accuracy of 90.2% compared with the statistical results from general fluorescence imaging, providing a potential technique for screening specific hybridoma cells.
研究领域:
生物化学
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分析化学
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生物技术
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分子生物学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wendong Liu,Lin Chu,Chenghui Zhang,Pengjuan Ni,Yuanyuan Jiang,Bo Wang,Yizhong Lu,Chuanxia Chen
Revealing the relationship between composition and enzyme-like activities is essential for the rational designs of nanozymes and related assays with improved performances. Here, a series of Fe-N co-doped porous carbon (Fe-N-C) nanozymes containing different Fe contents have been successfully prepared by facilely pyrolyzing hemin trapped zeolitic-imidazolate-frameworks (Hemin@ZIF-8). The special doping agent hemin will endow Fe-N-C with exceptionally high peroxidase-mimetic activities due to the hierarchically porous structure, high specific surface area, and high dispersed Fe-N x sites. Notably, the optimal Fe 55 -N-C nanozymes are used to detect bio-enzymes, by taking alkaline phosphatase (ALP) as a model, based on the inhibition of nanozymatic activity by ascorbic acid (AA). A linear activity range of 0.05–20 U/L is obtained with a low detection limit of 0.03 U/L, which is superior to the most published optical ALP assays. This work provides not only a new method for the design of the transition metal-N-C nanozyme with enhanced peroxidase-like activity but also a promising strategy for the detection of ascorbic acid-generating bio-enzymes with the assistance of specific substrates.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 19
·8608-8618
·
IF 3.591
Min Chen,Haimei Li,Xueming Su,Runqiang Wu,Huafu Feng,Xiaohang Shi,Jintao Liang,Jiejing Chen,Guiyin Li
Glypican-3 (GPC3) is a potential hepatocellular carcinoma (HCC) serum marker with good sensitivity and specificity. Herein, a label-free electrochemical aptasensor for the detection of GPC3 was developed using a reduced graphene oxide–hemin–chitosan (RGO–H–CS) nanocomposite-modified screen-printed electrode (SPE) as a biosensing platform and GPC3 aptamer as the recognition element. When GPC3 was present, the aptamer could specifically bind with the target GPC3 by specific recognition reaction and form GPC3–aptamer conjugations on the sensing surface, which could alter the electrochemical redox signal of hemin (Fe(III)/hemin(Fe(II))) in the RGO–H–CS nanocomposite recorded by differential pulse voltammetry (DPV). The electrochemical GPC3 aptasensor was characterized via scanning electron microscopy (SEM), Raman spectroscopy, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). Under optimal conditions, currents originating from the oxidation of hemin had a linear relationship with the concentration of GPC3 in the range of 0.01 µg mL−1 to 10.0 µg mL−1 with a detection limit of 7.9 ng mL−1 (S/N = 3). The developed aptasensor was applied to detect the GPC3 level in the human serum samples with the recovery rate of 101.04–104.9%. Moreover, the label-free aptasensor exhibited considerable anti-interfering ability, acceptable stability and good reproducibility. Therefore, this study provides a reliable and objective analysis method to achieve high screening for the early diagnosis of HCC.
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高影响因子
Frontiers in Neuroscience
·
2019
·
IF 3.648
Chen Xiao,Xi Zhiyu,Liang Huaibin,Sun Yuhao,Zhong Zhihong,Wang Baofeng,Bian Liuguan,Sun Qingfang
Secondary injuries mediated by oxidative stress lead to deterioration of neurological functions after intracerebral hemorrhage (ICH). Cortical astrocytes are among the most important cells in the central nervous system (CNS), and play key roles in maintaining redox homeostasis by providing oxidative stress defense. Hemin is a product of hemoglobin degradation, which has strong toxicity and can induce reactive oxygen species (ROS). Melatonin (Mel) and its metabolites are well tolerated without toxicity, prevent tissue damage as well as effectively assist in scavenging free radicals. We evaluated the hemin neurotoxicity to astrocytes and the resistance of Mel-treated astrocytes to hemin neurotoxicity. And we found Mel induced PKCα phosphorylation (p-PKC), nuclear translocation of Nrf2 in astrocytes, and upregulation of HO-1, which contributed to the reduction of ROS accumulation and cell apoptosis. Nrf2 and HO1 protein expression upregulated by Mel were decreased after administration of PKC inhibitor, Ro 31-8220 (Ro 31). Luzindole (Luz), a melatonin receptor inhibitor, suppressed p-PKCα, HO-1, and Nrf2 expression upregulated by Mel and increased cell apoptosis rate. The upregulation of HO-1 induced by Mel was depressed by knocking down Nrf2 expression by siRNA, which also decreased the resistance of astrocytes to toxicity of hemin. Mel activates astrocytes through PKCα/Nrf2/HO-1 signaling pathway to acquire resistance to toxicity of hemin and resist from oxidative stress and apoptosis. The positive effect of Mel on PKCα/Nrf2/HO-1 signaling pathway may become a new target for neuroprotection after intracerebral hemorrhage.
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高影响因子
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