ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 29
·8223-8232
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IF 4.478
Du Ning,Zhang Hao,Wang Jiahui,Dong Xuezhe,Li Jinqiu,Wang Kexin,Guan Ruifang
Hemin with functions such as oxygen carrying, oxygen storing, promoting redox, and performing electron transfer is important for the health of organisms. In this paper, green synthetic silicon nanoparticles (Si-NPs) were synthesized and used for free hemin detection in serum (a low limit of detection (LOD), 29.5 nM). The quenching mechanism was investigated by UV–vis absorption spectra, time-resolved luminescence decay curve, and circular dichroism (CD) spectra. It was confirmed that multiple redox centers of hemin led to intensified effective collision and increased the electron transfer rate, therefore enhancing the dynamic quenching, and it was undeniable that the inner filter effect (IFE) also played a role in the quenching. Graphical abstract
研究领域:
生物化学
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纳米医学
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zhiwei Liu,Nan Ma,Shuaibing Yu,Jinming Kong,Xueji Zhang
Ultrasensitive protein detection has considerable potential for early diagnosis and screening of diseases. Here, based on Hemin-catalyzed surface-initiated reversible addition-fragmentation chain transfer (SI-RAFT) polymerization, this work developed an assay for ultrasensitive fluorescent biosensing of proteins and established a thrombin fluorescent sensor. First, the amino-modified aptamer 1 was immobilized on Fe 3 O 4 magnetic beads, and then thrombin was added to form the aptamer 1-thrombin bioaffinity complex. Another thiol-modified aptamer 2 binds to bound thrombin to form a sandwich structure. Fluorescein O-methacrylate was used as the monomer, acetylacetone (ACAC) as the initiator, and Hemin as the catalyst. Through Hemin-catalyzed SI-RAFT polymerization, a large number of thrombin molecules are labeled with fluorescein O-methacrylate, resulting in severalfold amplification of the fluorescent signal. By detecting the fluorescent signal in thrombin from 1.0 fM to 0.1 nM, the proposed super sandwich strategy can detect thrombin at 0.98 fM, which is lower than the detection limit of most other methods.
研究领域:
分析化学
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生物传感器
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高分子科学
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蛋白质检测
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DOI
高影响因子
ANALYTICAL SCIENCES
·
2016
·Vol. 32
·期 8
·887-892
·
IF 1.174
Kang Bei Hua,Li Na,Liu Shi Gang,Li Nian Bing,Luo Hong Qun
Herein is reported a simple and label-free fluorescent detection method for hemin based on using protoporphyrin IX (PPIX) as a fluorescent signal reporter. PPIX emits weak fluorescence in an aqueous solution. When PPIX binds to G-quadruplexes, the fluorescence intensity of PPIX is greatly increased. While in the presence of target hemin, hemin competes with PPIX toward G-quadruplexes because its affinity to G-quadruplexes is higher than that of PPIX. With the formation of the hemin-G-quadruplex complex, PPIX is released to the solution from the G-quadruplex accompanied by quenching of the fluorescence of the system. This fluorescence change of the system can be used to monitor hemin with a low detection limit of 36 nM. In addition, the possible binding sites for PPIX binding to the G-quadruplex are discussed based on competition between hemin and PPIX. What is more, this method might pave the way for applying G-quadruplexes and PPIX to more sensing systems.
研究领域:
分析化学
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生物化学
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分子生物学
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PubMed
高影响因子
Catalysts
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2022
·Vol. 13
·期 1
·81
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IF 4.501
Ying Zhang,Junya Liao,Hao Liang
DNA-based biomimetic enzymes have attracted extensive attention due to their unique structure and stability compared to natural enzymes. Meanwhile, the specific sequences of DNA itself also have a catalytic effect. Herein, we first designed three guanine-rich DNA sequences numbered c−Myc3c, PG4TC, and TTT to construct g−quadruplex/hemin DNAzymes. Then, the g−quadruplex/hemin DNAzymes with the best activity were selected by a comprehensive examination of activity, degradation rate, and affinity. Subsequently, the stability and reusability of UiO66−DNAzymes were investigated using UiO66 as the carrier to immobilize DNAzymes. The results showed that UiO66−DNAzymes had excellent reusability and stability. Finally, UiO66−DNAzymes were successfully used for glucose detection by cascading with glucose oxidase (GOx) with a detection limit of 0.62 μM. The constructed glucose sensor had a good specificity, which is of great significance for developing a novel, accurate, fast, and economical glucose detection sensor.Keywords:metal-organic frameworks;DNAzymes;enzyme immobilization;biomimetic enzymes;glucose detection
研究领域:
生物化学
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纳米技术
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分析化学
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DOI
高影响因子
Nanoscale
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2019
·Vol. 11
·期 26
·12603-12609
·
IF 6.97
Weiwei Wu,Qingqing Wang,Jinxing Chen,Liang Huang,He Zhang,Kai Rong,Shaojun Dong
Although various nanomaterials have been found to exhibit intrinsic enzyme-like activity, to date, there is no general strategy for designing nanozymes, and their catalytic mechanism has not been studied in depth. To realize the desired enzymatic properties, imitating the structure of natural enzymes is a commendable way to develop effective nanozymes. Inspired by the structure of natural horseradish peroxidase (HRP), we loaded hemin onto amino-modified single-walled carbon nanotubes (SWNT-NH2) to prepare an effective peroxidase-like nanozyme (SWNT-NH2@hemin). The peroxidase-like activity of hemin was enhanced by SWNT through π–π interactions, and the positively charged -NH2 groups played a similar role to arginine in HRP and stabilized the intermediate during catalysis and facilitated the cleavage of the O–O bond. This is instructive for the development of a variety of highly efficient nanozymes by simulating the adjacent environment of the active center in natural enzymes. In addition, dual sensor platforms consisting of a colorimetric method and electrochemical method were developed based on SWNT-NH2@hemin.
研究领域:
生物化学
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纳米生物学
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催化科学
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DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2013
·
IF 1.977
W. Wei,D.M. Zhang,L.H. Yin,Y.P. Pu,S.Q. Liu
A colorimetric method for detection of DNA damage was developed by using hemin-graphene nanosheets (H-GNs). H-GNs were skillfully synthesized by adsorping of hemin on graphene through π–π interactions. The as-prepared H-GNs possessed both the ability of graphene to differentiate the damage DNA from intact DNA and the catalytic action of hemin. The damaged DNA made H-GNs coagulated to different degrees from the intact DNA because there were different amount of negative charge exposed on their surface, which made a great impact on the solubility of H-GNs. As a result, the corresponding centrifugal supernatant of H-GNs solution showed different color in the presence of 3,3′,5,5′-tetramethylbenzidine (TMB) and H 2 O 2 , which could be discriminated by naked eyes or by ultraviolet (UV)–visible spectrometer. Based on this, the damaged effects of styrene oxide (SO), NaAsO 2 and UV radiation on DNA were studied. Results showed that SO exerted most serious damage effect on DNA although all of them damaged DNA seriously. The new method for detection of DNA damage showed good prospect in the evaluation of genotoxicity of new compounds, the maximum limit of pesticide residue, food additives, and so on, which is important in the fields of food science, pharmaceutical science and pesticide science.
研究领域:
生物化学
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分子生物学
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分析化学
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毒理学
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2017
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IF 7.504
Xiaoqiang Wang,Chao Wang,Meihong Pan,Junting Wei,Fuping Jiang,Rongsheng Lu,Xuan Liu,Yihui Huang,Fang Huang
Taking inspiration from biology’s effectiveness in functionalizing protein-based nanocages for chemical processes, we describe here a rational design of an artificial metalloenzyme for oxidations with the bacterial chaperonin GroEL, a nanocage for protein folding in nature, by supramolecular anchoring of catalytically active hemin in its hydrophobic central cavity. The promiscuity of the chaperonin cavity is an essential element of this design, which can mimic the hydrophobic binding pocket in natural metalloenzymes to accept cofactor and substrate without requiring specific ligand–protein interactions. The success of this approach is manifested in the efficient loading of multiple monomeric hemin cofactors to the GroEL cavity by detergent dialysis and good catalytic oxidation properties of the resulting biohybrid in tandem with those of the clean oxidant of H2O2. Investigation of the mechanism of hemin–GroEL-catalyzed oxidation of two-model substrates reveals that the kinetic behavior of the complex follows a ping-pong mechanism in both cases. Through comparison with horseradish peroxidase, the oxidative activity and stability of hemin–GroEL were observed to be similar to those found in natural peroxidases. Adenosine 5′-triphosphate (ATP)-regulated partial dissociation of the biohybrid, as assessed by the reduction of its catalytic activity with the addition of the nucleotide, raises the prospect that ATP may be used to recycle the chaperonin scaffold. Moreover, hemin–GroEL can be applied to the chromogenic detection of H2O2, which (or peroxide in general) is commonly contained in industrial wastes. Considering the rich chemistry of free metalloporphyrins and the ease of production of GroEL and its supramolecular complex with hemin, this work should seed the creation of many new artificial metalloenzymes with diverse reactivities.
研究领域:
生物化学
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酶工程
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催化化学
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PubMed
高影响因子
TALANTA
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2023
·
IF 6.1
Jingyi Dong,Xia Qiu,Mimi Huang,Xiaohu Chen,Yongxin Li
Solid-nanopores/nanopipettes have the exquisite ability to reveal the changes in molecular volume due to the advantages of adjustable size, good rigidity and low noise. Herein, a new platform for sensing application was established based on G-quadruplex-hemin DNAzyme (GQH) functionalized gold-coated nanopipettes. In this method, GQH was immobilized on gold-coated nanopipette, which could be used as a catalyst for the reaction of H 2 O 2 with 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS) to promote the conversion of ABTS to ABTS + ions inside gold-coated nanopipette, and the change of transmembrane ion current could be monitored in real time. At the optimal conditions, there was a correlation between the ion current and the concentration of H 2 O 2 in a certain range, which could be used for the hydrogen peroxide sensing. The GQH immobilized nanopipette provides a useful platform to investigate enzymatic catalysis in confined environment, which can be used in electrocatalysis , sensing and fundamental electrochemistry .
研究领域:
纳米技术
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生物化学
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分析化学
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电化学
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高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2019
·Vol. 411
·期 17
·3819-3827
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IF 3.286
Wang Xiaoqiang,Sun Haiyan,Wang Chao
The design of functionalized protein nanocages as enzyme mimics is a relatively new and promising field as these biogenic nanocapsules are inherently monodisperse with precise architectures, unattainable by purely synthetic processes. This work explored the catalytic properties of the bacterial GroEL-nanocaged hemin and its performance in label-free colorimetric assays. It is demonstrated that the hemin-GroEL biohybrid has peroxidase-like activity and follows the typical Michaelis-Menten kinetics and ping-pong mechanism in the model sensing processes. The open nature and nanoreactor effect of the GroEL cage and the addition of ATP are shown to significantly influence the catalytic activity. For glucose detection with the hemin-GroEL complex, the linearity between the analyte concentration and UV-vis absorption was determined to range from 0 to 200 μM with a limit of detection (LOD) of ~ 12 μM under the defined conditions. In addition, the colorimetric detection of catechol led to a linear dynamic range of 0–120 μM with a LOD of ~ 17 μM. This indicates that the same assay could be used as a sensing platform for the detection or even oxidative removal of phenolic contaminants in the presence of H 2 O 2 . Thus, GroEL cage is a valuable tool for the development of nanozymes and practical applications such as clinical analysis and environmental monitoring.
研究领域:
生物化学
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纳米技术
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分析化学
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生物技术
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DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2017
·Vol. 23
·期 70
·17755-17763
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IF 5.317
Huan Xu,Zhen Yang,Hailing Li,Zhonghong Gao
Graphical Selective oxidation : Hemin-graphene derivatives are synthesized. They show a pronounced effect on weakening protein tyrosine nitration. In addition, it is demonstrated that the hemin-graphene derivatives accelerate tyrosine (Tyr) and nitrite oxidation, but suppress the free-radical coupling reaction (see figure). Protein tyrosine nitration is implicated in the occurrence and progression of pathological conditions involving free radical reactions. It is well recognized that hemin can catalyze protein tyrosine nitration in the presence of nitrite and hydrogen peroxide. Generally, the catalytic efficiency is positively correlated to its peroxidase activity. In this study, however, it is found that the efficiency of hemin in catalyzing protein tyrosine nitration is largely suppressed after functionalization with graphene derivatives, even though its peroxidase-like activity is more than quadrupled. Further studies show that the oxidation of tyrosine is still observed for these composites; dityrosine formation, however, is greatly inhibited. Furthermore, these composites also exhibit strong effects on the oxidation of nitrite into nitrate. Therefore, we propose a mechanism in which hemin-graphene derivatives facilitate the oxidation of tyrosine and nitrite to produce tyrosyl radicals and nitrogen dioxide radicals in the presence of hydrogen peroxide, but graphene interlayers serve as barriers that hinder radical–radical coupling reactions; consequently, protein tyrosine nitration is restrained. This property of hemin-graphene derivatives, by which they catalyze substrate oxidation but suppress radical–radical coupling reactions, shows their great potential in selective oxidation procedures for byproduct removal.
研究领域:
生物化学
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医学
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PubMed
高影响因子
Environmental Technology & Innovation
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2022
·
IF 7.758
Xijuan Chao,Dezhi Yao,Chuxuan Chen,Chengfei Zhang
Hemin, an iron (III) complex of protoporphyrin IX dissociated from met Hb, exhibits many biological functions. The excess of hemin can be extremely toxic, such as permeabilizing cellular membranes and oxidizing proteins, lipids and nucleic acids. Therefore, it is of great significance to achieve hemin detection. Here, a simple and environmental-friendly fluorescence-based approach for hemin detection is reported by using synthesized dicyanomethylene-4H-pyrans-morpholine ( DCM-ML ) as a fluorescent signal reporter molecule in the presence of human serum albumin (HSA). DCM-ML is non-fluorescent in aqueous solution, but emits 630 nm fluorescence signal with HSA. Upon hemin addition, the specific competitive-binding towards HSA results in the release of DCM-ML reporter, accompanied by a gradual decrease of fluorescence intensity of the DCM-ML /HSA system. Importantly, the fluorescence intensity at 630 nm exhibits a good linear relationship ( R 2 > 0.99) with the added concentration of hemin at the range of 0– 2 . 8 μ m ol/L, giving a quite low detection limit of 9.84 nmol/L in PBS buffer. The DCM-ML /HSA system possesses strong anti-interference capacity against other biomolecules or ions, and fast response time (30 s) for hemin and a wide pH range of 7–10 is generally suitable for the detection system. At last, the applications of DCM-ML /HSA system for hemin detection in environmental and biological systems are successfully demonstrated, indicating its practical application potential in the future.
研究领域:
生物化学
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医学检测
·
分析化学
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DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2022
·
IF 5.895
Rong Tian,Lan Zhou,Naihao Lu
The interactions between quercetin and bovine (or human) hemoglobin (Hb) were systematically investigated by fluorescence, UV–vis absorption spectroscopy, and molecular docking to demonstrate the structural mechanism by which quercetin affected the Hb redox state and stability. Quercetin could interact with the central cavity of the Hb molecule with one binding site to generate an Hb–quercetin complex, and the hydrophobic interaction played an important role in the formation of the complex. The binding constant for the Hb–quercetin complex at 298 K was observed to be 1.25 × 104 M–1. In addition, quercetin effectively inhibited Hb-induced lipid oxidation in liposomes or washed muscles, which was ascribed to the conversion to oxy-Hb and decreased hemin dissociation from met-Hb. Consistent with its lower abilities to bind Hb and scavenge free radicals, rutin (i.e., quercetin-3-rhamnosylglucsoside) did not significantly influence the redox state of Hb nor reduce hemin release from Hb, and subsequently, it less effectively inhibited Hb-induced lipid oxidation than quercetin. Altogether, the results herein provide novel insights into the antioxidant mechanism for quercetin and are beneficial to the application of natural quercetin in Hb-containing foods.
研究领域:
生物化学
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食品科学
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分子生物学
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PubMed
高影响因子
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