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JOURNAL OF HAZARDOUS MATERIALS · 2013 · IF 3.925

Enhanced decomposition of dyes by hemin-ACF with significant improvement in pH tolerance and stability

Yuyuan Yao,Yajun Mao,Qunfeng Huang,Lie Wang,Zhengfu Huang,Wangyang Lu,Wenxing Chen

In this study, we evaluated a novel heterogeneous catalytic system (hemin-ACF/H 2 O 2 ) based on activated carbon fiber supported hemin for the rapid removal of dyes. Contrast experiments, effects of pH and temperature, and sustained catalytic stability of hemin-ACF for the catalytic decomposition of azo dye RR195 used as a model pollutant were investigated. Surprisingly, the introduction of ACF significantly enhanced the decomposition of dyes by hemin with an obvious improvement in pH tolerance and stability. Inhibition and probe studies combined with electron paramagnetic resonance (EPR) were conducted to ascertain the role of several radicals ( OH, O 2 − /HO 2 , 1 O 2 and Fe IV O) on dye degradation. ACF are rich in free electrons, and the π-conjugated macrocyclic structure of hemin may present convenient channels for the transfer of free electrons from the ACF, promoting the generation of hydroxyl radicals and high-valence iron species. These results are promising because they offer new insight for the application of hemin as a catalyzer upon treatment of organic pollutants and contribute to identification of the interaction between support material and catalyzer from a new perspective.

CAS / MDL: 16009-13-5
研究领域: 环境科学 · 催化化学
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JOURNAL OF HAZARDOUS MATERIALS · 2013 · IF 3.925

Spectrophotometric analysis of phenols, which involves a hemin–graphene hybrid nanoparticles with peroxidase-like activity

Ruiling Sun,Yong Wang,Yongnian Ni,Serge Kokot

Phenols are well known noxious compounds, which are often found in various water sources. A novel analytical method has been researched and developed based on the properties of hemin–graphene hybrid nanosheets (H–GNs). These nanosheets were synthesized using a wet-chemical method, and they have peroxidase-like activity. Also, in the presence of H 2 O 2 , the nanosheets are efficient catalysts for the oxidation of the substrate, 4-aminoantipine (4-AP), and the phenols. The products of such an oxidation reaction are the colored quinone-imines (benzodiazepines). Importantly, these products enabled the differentiation of the three common phenols – pyrocatechol, resorcin and hydroquinone, with the use of a novel, spectroscopic method, which was developed for the simultaneous determination of the above three analytes. This spectroscopic method produced linear calibrations for the pyrocatechol (0.4–4.0   mg   L −1 ), resorcin (0.2–2.0   mg   L −1 ) and hydroquinone (0.8–8.0   mg   L −1 ) analytes. In addition, kinetic and spectral data, obtained from the formation of the colored benzodiazepines, were used to establish multi-variate calibrations for the prediction of the three phenol analytes found in various kinds of water; partial least squares (PLS), principal component regression (PCR) and artificial neural network (ANN) models were used and the PLS model performed best.

研究领域: 环境科学 · 分析化学 · 纳米材料科学
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Small · 2023 · IF 13.3

Specific Chemiluminescence Imaging and Enhanced Photodynamic Therapy of Bacterial Infections by Hemin-Modified Carbon Dots

Ke Cheng,Henggang Wang,Shan Sun,Mingyu Wu,Hongzhe Shen,Ke Chen,Zhiyuan Zhang,Si Li,Hengwei Lin

Antibacterial photodynamic therapy (aPDT) is a promising antibiotics-alternative strategy for bacterial infectious diseases, which features broad-spectrum antibacterial activity with a low risk of inducing bacterial resistance. However, clinical applications of aPDT are still hindered by the hydrophobicity-caused inadequate photodynamic activity of conventional photosensitizers and the hypoxic microenvironment of bacterial infections. To address these problems, herein, a promising strategy is developed to achieve specific chemiluminescence (CL) imaging and enhanced PDT of bacterial infections using hemin-modified carbon dots (H-CDs). The H-CDs can be facilely prepared and exhibit favorable water solubility, augmented photodynamic activity, and unique peroxidase-mimicking capacity. Compared with the free CDs, the photodynamic efficacy of H-CDs is significantly augmented due to the increased electron–hole separation efficiency. Moreover, the peroxidase catalytic performance of H-CDs enables not only infection identification via bacterial infection microenvironment-responsive CL imaging but also oxygen self-supplied aPDT with hypoxia-relief-enhanced bacteria inactivation effects. Finally, the enhanced aPDT efficiencies of H-CDs are validated in both in vivo abscess and infected wound models. This work may provide an effective antibacterial platform for the selective imaging-guided treatment of bacterial infections.

研究领域: 生物医学工程 · 纳米技术 · 药学 · 传染病 · 治疗诊断学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2023 · IF 4.4

Smartphone and paper-based device for glucose monitoring using acetylene black-hemin nanozyme as catalyst

Xiaojuan Yi,Yonghua Yuan,Min Qing,Lulu Wang,Huizhen Li,Lijuan Bai

Glucose management is an important part of disease control for diabetes patients, thus the development of a rapid and real-time point of care testing (POCT) device for monitoring blood glucose is of great significance. In this work, a paper-based analytical device (PAD) is constructed by combining acetylene black (AB)-hemin complex modified filter paper as sensing platform with a smartphone as signal detector. Large specific surface area of AB decreases the self-associate and aggregate of hemin in aqueous solution, resulting in improved peroxidase-like activity of hemin. Compared with graphene oxide supported hemin, AB-hemin exhibits superior signal response on paper. Glucose oxidase (GOx) catalyzes the conversion of blood glucose to hydrogen peroxide, and then AB-hemin complex catalyzes the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue TMB oxidized products (TMB + ) in the presence of hydrogen peroxide, thus achieving the visual detection of blood glucose. In optimal conditions, PAD provides an applicable linear range from 0.2 mM to 30 mM and a low limit of detection (LOD) (0.06 mM). Notably, the detection accuracy of the developed paper-based sensor is in good agreement with that of the commercially available blood glucose meter (p > 0.05). Moreover, the proposed PAD presents high recoveries from 95.4% to 112% (RSD ≤ 3.2%), and therefore holds great potential for glucose monitoring and diabetes diagnosis.

研究领域: 生物医学工程 · 分析化学 · 即时检测 · 糖尿病管理
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TALANTA · 2018 · IF 4.244

Graphitic C3N4 nanosheet and hemin/G-quadruplex DNAzyme-based label-free chemiluminescence aptasensing for biomarkers

Ke Li Lin,Tong Yang,Hong Yan Zou,Yuan Fang Li,Cheng Zhi Huang

Here we first reported that graphitic carbon nitride nanosheet (g-C 3 N 4 NS) could effectively quench the chemiluminescence (CL) of luminol-hydrogen peroxide (H 2 O 2 ) system. According to the new discovery, a label-free and homogeneous CL aptasensing platform was designed for sensitive detecting of biomarkers. In the absence of target, DNA probe containing hemin/G-quadruplex DNAzyme structure was adsorbed on the surface of g-C 3 N 4 NS, causing the CL quenching of luminol through an electron transfer process. However, in the presence of the target, a DNA-DNA duplex was formed due to DNA hybridization reaction and target recognition effect, which could not be adsorbed onto the g-C 3 N 4 NS surface because of its weak affinity. Thus, the electron transfer was blocked and the CL emission of luminol could be enhanced. The proposed CL aptasensor could detect carcinoembryonic antigen (CEA) with a detection limit of 63.0 pg/mL and it can also be used as a general detecting strategy for adenosinetriphosphate (ATP) detection. This aptasensing platform exhibited high sensitivity toward biomarkers and the probe need not be labeled, showing great promise for disease diagnosis.

CAS / MDL: 16009-13-5 108-78-1
研究领域: 生物化学 · 分析化学 · 医学诊断
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ChemPlusChem · 2018 ·Vol. 83 ·期 11 ·1038-1043 · IF 3.205

Enantioselective Activity of Hemin in Supramolecular Gels Formed by Co-Assembly with a Chiral Gelator

Song Wang,Hejin Jiang,Li Zhang,Jian Jiang,Minghua Liu

Graphical Supramolecular gels formed from hemin and histidine amphiphiles were tested as artificial enzymes to catalyse the oxidation of the chiral substrate L-DOPA to L-dopachrome. The supramolecular gel made up of left-handed helices enhanced the catalytic activity of hemin effectively, and more interestingly, it exhibited enantioselectivity. Supramolecular co-assembly provides an efficient way to combine structural and functional units through noncovalent interactions and produce materials with enhanced performance. Here, using a chiral amphiphilic histidine derivative (LHC18 or DHC18) as a gelator, we have successfully co-assembled the gelator and hemin through gelation. During the co-assembly, the chiral information of the gelator was transcribed into the assemblies, and thus right- and left-handed helical ribbons from LHC18-Hemin and DHC18-Hemin co-assemblies were obtained, respectively, which were confirmed by CD spectra and SEM observations. These helical ribbons were used as artificial enzymes to catalyse the oxidation reaction of 3,4-dihydroxy-L-phenylalanine (L-DOPA). The catalytic activity of hemin in supramolecular gels can be effectively enhanced over that of free hemin. Moreover, by virtue of induced chirality, the supramolecular gels of LHC18-Hemin and DHC18-Hemin exhibited obvious enantioselective activity. This work provides a way to combine chirality transfer and supramolecular asymmetric catalysis.

CAS / MDL: 59-92-7
研究领域: 生物化学 · 材料科学
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TALANTA · 2019 · IF 4.916

Peptide-conjugated hemin/G-quadruplex as a versatile probe for “signal-on” electrochemical peptide biosensor

Zhuo Ye,Gaiping Li,Lingling Xu,Qian Yu,Xiaoyue Yue,Yongmei Wu,Baoxian Ye

In this work, a novel “signal-on” electrochemical peptide biosensor based on peptide-conjugated hemin/G-quadruplex (DNAzyme-peptide) hybrid and rosebud-like MoSe 2 @reduced graphene oxide (MoSe 2 @rGO) nanocomposite, was developed for detection of prostate-specific antigen (PSA). Interestingly, the peptide not only served as recognition probe to detect PSA, but also acted as the enhancer to improve the enzyme activity of hemin/G4, which promoted the detection sensitivity. Up addition of PSA, Fe 3 O 4 -labeled DNAzyme-peptide probe was cleaved, followed by the magnetic separation. The cleaved DNAzyme-peptide was then captured onto the cysteine-modified electrode via the interaction between carboxyl groups of peptide and amino group of cysteine. A strong electrochemical signal was obtained from hemin and further was amplified by the enhanced electrocatalysis of DNAzyme-peptide. Compared to the original DNAzyme, DNAzyme-peptide exhibited more than 3-fold enhancement in signal amplification. And MoSe 2 @rGO amplified the electrochemical signal due to its good conductivity and large surface area. So the proposed strategy detected PSA down to 0.3 fg/mL, and it showed the advantages of simplicity, low cost by avoiding the use of expensive protein enzyme and additional electroactive species. Therefore, the proposed biosensor potentially provided a very effective tool for early diagnosis of cancer by the detection of PSA.

研究领域: 生物化学 · 医学诊断 · 纳米材料科学
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MICROCHIMICA ACTA · 2022 ·Vol. 189 ·期 8 ·1-9 · IF 6.408

Hemin-graphene oxide-gold nanoflower-assisted enhanced electrochemiluminescence immunosensor for determination of prostate-specific antigen

Liu Gengjun,Guan Xiaohan,Li Binxiao,Zhou Hong,Kong Na,Wang Haiyan

An ultrasensitive luminol electrochemiluminescence (ECL) immunosensor was constructed for the detection of prostate specific antigen (PSA) using glucose oxidase–decorated hemin-graphene oxide-gold nanoflowers ternary nanocomposites as probes. Graphene oxide was first modified with hemin and then with gold nanoflowers through an in situ growth method, which has significantly boosted the catalytic activity of this graphene oxide–based peroxidase mimetics. The biocatalytical activity of this ECL immunosensor was thoroughly investigated to achieve selective recognition of the analyte molecules (PSA) by specific binding between antigens and antibodies. The limit of detection was calculated to be 0.32 pg mL −1 with a signal-to-noise ratio of 3. A broad linear range from 7.5 × 10 −4 to 2.5 ng mL −1 was obtained. Such step-by-step assembled biosensor showed controlled nanostructure and exhibited promising application in analysis of human serum samples with a recovery range of 90.6–111.8% and a RSD range of 3.9–5.5%. Graphical abstract

研究领域: 生物医学工程 · 分析化学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Ratiometric fluorescence detection of artemisinin based on photoluminescent Zn-MOF combined with hemin as catalyst

Kunming Sun,Tinghui Deng,Jing Sun,Shuo Gao,Huwei Liu,Shuyun Zhu,Xian-En Zhao

Artemisinin (ART) is a type of frontline drug to treat drug-resistant falciparum malaria. Simple, accurate and selective determination of ART is significant to monitor its clinical pharmaceutical efficacy. Herein, a new ratiometric fluorescence method has been designed for the determination of ART with Zn-MOF as fluorescence reference and hemin as catalyst, respectively. Zn-MOF possesses intrinsic fluorescence at 443 nm owing to 2-aminoterephthalic acid ligand. When o -phenylenediamine (OPD) is mixed with hemin, a weak fluorescent signal at 570 nm ascribed to oxidized product of OPD (oxOPD) is observed. In the presence of ART, hemin can catalyze ART to break its peroxide bridge and release a large number of reactive oxygen species, which effectively oxidize OPD into luminescent oxOPD. Therefore, the fluorescence at 570 nm is enhanced significantly while the fluorescence of Zn-MOF remains basically unchanged. Thus, a ratiometric fluorescence sensing platform has been constructed for the detection of ART. This method exhibits wider linear range (0.15 μM-150 μM) with detection limit of 50 nM. This novel and selective method has been used to detect ART in compound naphthoquinone phosphate tablets.

研究领域: 药学 · 分析化学 · 生物医学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2022 ·Vol. 169 ·期 8 ·087517 · IF 4.386

An Ultrasensitive Glypican‑3 Electrochemical Aptasensor Based on Reduced Graphene Oxide-Carboxymethylchitosan-Hemin/Palladium Nanoparticles

Shengnan Li,Xinhao Li,Liping Cao,Chaoxian Wang,Jintao Liang,Zhide Zhou,Guiyin Li

Glypican-3 (GPC3) is a serum marker for hepatocellular carcinoma (HCC) and has excellent specificity and sensitivity. Herein, the construction of an electrochemical aptasensor based on reduced graphene oxide-carboxymethyl chitosan-hemin-palladium nanoparticles (RGO-CMCS-Hemin/Pd NPs) and GPC3 aptamer (GPC3apt) has the function of GPC3 identification and analysis. RGO-CMCS-Hemin/Pd NPs has excellent biocompatibility, large specific surface area and good electrical conductivity, which is not only used as advanced sensing materials to modify the electrode surface to reduce the resistance and increase the signal amplitude, but also used as an electroactive substance to provide electrical signals. GPC3apt as a biometric element makes the aptasensor has good specificity and sensitivity. The GPC3apt can combine with GPC3 and form GPC3-aptamer conjugation, which increases the electron transfer impedance and changes the electrical signal. Under the optimum conditions, the aptasensor had a good linear relationship with the GPC3 concentration in the range of 1.0–100.0 ng ml−1 with R2 of 0.9573. The lower limit of detection was 1.0 ng ml−1. When the aptasensor was applied to GPC3 detection in human serum samples, the recovery was 93.73%–118.83%. In addition, the GPC3 aptasensor has excellent specificity, reproducibility and stability, which is anticipated to be applied for the clinical detection of GPC3.

CAS / MDL: 16903-35-8
研究领域: 生物医学工程 · 分析化学 · 纳米技术 · 癌症诊断
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MOLECULES · 2022 ·Vol. 27 ·期 20 ·6779 · IF 4.927

Nanozyme Based on Dispersion of Hemin by Graphene Quantum Dots for Colorimetric Detection of Glutathione

Zhaoshen Li,Xiaochun Deng,Xiaoping Hong,Shengfa Zhao

Compared with natural enzymes, nanozymes have the advantages of good catalytic performance, high stability, low cost, and can be used under extreme conditions. Preparation of highly active nanozymes through simple methods and their application in bioanalysis is highly desirable. In this work, a nanozyme based on dispersion of hemin by graphene quantum dot (GQD) is demonstrated, which enables colorimetric detection of glutathione (GSH). GQD was prepared by a one-step hydrothermal synthesis method. Hemin, the catalytic center of heme protein but with low solubility and easy aggregation that limits its catalytic activity, can be dispersed with GQD by simple sonication. The as-prepared Hemin/GQD nanocomplex had excellent peroxidase-like activity and can be applied as a nanozyme. In comparison with natural horseradish peroxidase (HRP), Hemin/GQD nanozyme exhibited a clearly reduced Michaelis–Menten constant (Km) when tetramethylbenzidine (TMB) was used as the substrate. With H2O2being the substrate, Hemin/GQD nanozyme exhibited a higher maximum reaction rate (Vmax) than HRP. The mechanisms underlying the nanozyme activity were investigated through a free radical trapping experiment. A colorimetric platform capable of sensitive detection of GSH was developed as the proof-of-concept demonstration. The linear detection range was from 1 μM to 50 μM with a low limit of detection of 200 nM (S/N = 3). Determination of GSH in serum samples was also achieved.Keywords:nanozyme;graphene quantum dot;hemin;peroxidase-like activity;colorimetric determination of glutathione

研究领域: 生物化学 · 纳米技术 · 分析化学
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MATERIALS LETTERS · 2023 · IF 3

Cu-hemin multilayer nanosheets with integration of peroxidase and photothermal properties for efficient synergistic sterilization

Zitong Wang,Haotian Wu,Yuan Fang,Hao Yang,Xiaomin Wang

The increasing drug resistance of bacteria due to the inappropriate use of various antibiotics has become an ongoing public health problem around the world. In this work, a novel Cu-hemin nanosheet with multilayer structure was synthesized by a simple green method. Integrating the peroxidase properties of hemin with the excellent photothermal conversion performance of IR780, the as-prepared Cu-hemin@IR780 can not only effectively catalyze hydrogen peroxide to produce reactive oxygen species (ROS), but also has a highly efficient and stable photothermal effect for sterilization. The antibacterial efficiency against MRSA can reach up to 98.96% by using chemodynamic therapy (CDT) and photothermal therapy (PTT) for synergistic sterilization.

CAS / MDL: 54827-17-7
研究领域: 纳米技术 · 生物医学工程 · 材料科学 · 微生物学
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