ACS Applied Materials & Interfaces
·
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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DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
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IF 1.5
Shiguan Xu,Lijun Yan,Hui Cheng,Hui Xie,Lina Zeng,Lin Li,Shuhai He,Wei Sun
In this paper an electrochemical sensor was fabricated by dropping a graphdiyne (GDY) and hemin suspension solution on the surface of carbon ionic liquid electrode (CILE) followed by casting the Nafion film (Nafion/hemin-GDY/CILE). The morphology of GDY was observed by scanning electron microscopy with the biomolecular structure of hemin-GDY and hemin characterized by UV-Vis absorption spectrophotometry, which proved that hemin maintained the original structure after mixing with GDY. Direct electrochemistry of hemin on the GDY modified electrode was realized with a pair of well-defined redox peaks and electrochemical performances were checked in detail with the electrochemical parameters calculated. Nafion/hemin-GDY/CILE showed excellent electrocatalytic ability towards the reduction of bromate with the detection range from 5.00 to 50.0 mmol L -1 and the detection limit of 3.3 mmol L -1 (3 σ ). In addition, the modified electrode possessed good reproducibility and stability, which was applied to the analysis of seawater samples.
研究领域:
分析化学
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电化学传感器
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高影响因子
Micromachines
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2021
·Vol. 12
·期 12
·1519
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IF 2.891
Jin-Guang Liu,Jia-Zheng Wan,Qing-Min Lin,Guo-Cheng Han,Xiao-Zhen Feng,Zhencheng Chen
Quercetin (Qu) is one of the most abundant flavonoids in the human diet. High concentrations of Qu can easily cause adverse effects and induce inflammation, joint pain and stiffness. In this study, Heme was used as a sensitive element and deposited and formed nanorods on a glassy carbon electrode (GCE) for the detection of Qu. The Heme/GCE sensor was characterized using scanning electron microscopy (SEM), cyclic voltammetry (CV), differential pulse voltammetry (DPV) and electrochemical impedance spectroscopy (EIS) techniques. Under optimized conditions, the developed sensor presented a linear concentration ranging from 0.1 to 700 μmol·L−1according to the CV and DPV methods. The detection limit for the sensor was 0.134 μmol·L−1and its sensitivity was 0.12 μA·μM−1·cm−2, which were obtained from CV analysis. Through DPV analysis we obtained a detection limit of 0.063 μmol·L−1and a sensitivity of 0.09 μA·μM−1·cm−2. Finally, this sensor was used to detect the Qu concentration in loquat leaf powder extract, with recovery between 98.55–102.89% and total R.S.D. lower than 3.70%. The constructed electrochemical sensor showed good anti-interference, repeatability and stability, indicating that it is also usable for the rapid detection of Qu in actual samples.Keywords:electrochemical sensors;quercetin;detection;heme;modified electrode
研究领域:
分析化学
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生物医学工程
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Li Lei,Qiuxia Tu,Ling Jiao,Song Xiang,Li Wang,Xia Ran,Bo Xiao,Guangwei Feng,Jian Feng,Chunlin Zhang
Mitochondrial damage mediated by reactive oxygen species (ROS) is a major contributory factor to Parkinson’s disease (PD) pathogenesis. The use of hemin-based nanomaterials to control ROS production can protect against neurological damage. Here, we report the rational design of a uniform and water-soluble artificial nanozyme based on an ultrathin graphitic carbon nitride (g-C 3 N 4 ) nanosheet with loaded hemin to reduce ROS and treat PD. The g-C 3 N 4 not only acted as a scaffold for hemin loading but also improved the stability, cytotoxicity, and catalytic action of hemin. The integration of g-C 3 N 4 increased hemin’s peroxidase activity by 31.7%, promoting effective oxidation of the substrate 3,3′,5,5′-tetramethybenzichne (TMB) in the presence of H 2 O 2 to a blue-colored solution after 10 min’ incubation at room temperature. Moreover, CN-hemin exhibited good biocompatibility and could effectively scavenge intracellular ROS and reduce cytotoxicity induced by H 2 O 2 and 6-hydroxydopamine (6-OHDA). In vivo animal studies using nematode transgenic hus111 strain and 6-OHDA pretreated C. elegan s wild-type Bristol (N2) as models further showed that CN-hemin extended their lifespan and restored dopamine-dependent behaviors such as area-restricted searching, ethanol avoidance, and the basal slowing response by reducing ROS-mediated neurotoxicity. Nanomaterials using CN-hemin enzyme mimicry have potential biomedical applications, including the treatment of PD and disorders related to ROS metabolism.
研究领域:
神经科学
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生物医学工程
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材料科学
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DOI
高影响因子
Environmental Technology & Innovation
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2025
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IF 7.1
Zhenxin Wang,Qilin Yu,Zhiqiang Zhao,Ruicheng Zhang,Hongbo Zhang,Yaobin Zhang
Anammox is limited in practical application due to the need to control the influent ratio of NO 2 - to NH 4 + . Fe(III) (hydr)oxides have been confirmed to serve as electron acceptors and induce a so-called Feammox to anaerobically oxidize ammonia in Anammox systems via extracellular electron transfer, which however is also restrained by the low activity of Fe(III) (hydr)oxides. Heme, a Fe-containing compound with high redox activity, was introduced into the Anammox system to improve NH 4 + oxidation in this study. A removal rate of 46.32 mg N/(L·d) was achieved for nitrogen through the addition of heme, which was 43.85% higher than the maximum Feammox efficiency in documents (32.20 mg N/(L·d)). Continuous experiments showed that the added heme participated in the intracellular and extracellular electron transfer of Anammox. The contribution of Feammox to nitrogen removal was affected by the influent NO 2 - -N/NH 4 + -N ratio. Under a high NO 2 - -N/NH 4 + -N ratio (1.25:1), the contribution of Feammox to NH 4 + -N removal was 8.29%. This ratio increased to 31.49% under a low NO 2 - -N/NH 4 + -N ratio (0.80). Besides increasing the nitrogen removal efficiency, heme addition may significantly lower the nitrite requirement in this biological process, leading to improved adaptability in its application.
研究领域:
环境微生物学
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污水处理
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DOI
高影响因子
TALANTA
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2025
·
IF 6.1
Rong Tang,Chenglin Zhang,Baolian Liu,Yujie Kang,Ya Wang,Xiupei Yang
Recently, it has become valuable to develop strategies based on multi-mode sensors to detect analytes related to human health, food safety and environmental pollution. In this study, KL@PPIX-hemin composite prepared by immobilizing hemin and protoporphyrin IX (PPIX) on self-assembled peptide nanotubes (PNTs) through multiple non-covalent interactions were used for colorimetric/fluorescent dual-mode sensing of tannic acid (TA). PNTs as a carrier can provide the hydrophobic microenvironment for hemin and PPIX to protect them from dimerization, thus activating their respective peroxidase-mimicking activity and fluorescence emission. Further experiments show that the composite could catalyze H 2 O 2 to oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to generate blue ox-TMB, which could exactly quench the emission of PPIX by inner filter effect. The added TA can reduce ox-TMB to TMB and further turn on the fluorescence of system. A colorimetric/fluorescent dual-mode sensing system for TA was thus constructed and a low limit of detection (13.2 nM) was obtained. In addition, the analytical strategy has been successfully applied to accurate TA determination in actual tea samples. The method was also combined with smartphone to achieve visual detection of TA, which provides a broad prospect for portable and rapid tannic acid analysis.
研究领域:
分析化学
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生物医学工程
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食品安全检测
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Xueru Zhang,Jiarong Guo,Wei Tang,Xinrui Duan
Based on the chemical structure and luminescence mechanism of luminol, the synthesis of luminol analogues has been widely studied. However, luminol and its derived reagents are still suffering from some drawbacks, such as short luminescence time and weak intensity. Herein, we designed and synthesized a novel hydroxyphenyl benzothiazole-based phthalhydrazide derivative DAH-AMPH, which has a hydroxyphenyl benzothiazole structure as a strong fluorescent site and a cyclic phthalhydrazide structure as a chemiluminescence (CL) emitting site. DAH-AMPH exhibited excellent CL properties in the DAH-AMPH/UHP/hemin CL system for hemin detection with a wide linear range of 0.1 nM to 20.0 nM and low LOD as 3 pM. It performed good selectivity in bloodstain imaging on different substrate materials. DAH-AMPH/UHP/hemin CL system supplied a powerful tool for trace detection of bloodstain. Moreover, as a new CL substrate to HRP, DAH-AMPH showed high sensitivity (0.8 pg/mL of LOD) in the DAH-AMPH/UHP/SPTZ/MORP/HRP CL system indicating a bright prospect for the use of DAH-AMPH in heme-containing peroxidase detection.
研究领域:
分析化学
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法医学
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生物化学
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DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
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2024
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IF 5.4
Ruth Antwi-Baah,Mirabel Ewura Esi Acquah,Malcom Frimpong Dapaah,Xiaoqin Chen,Joojo Walker,Heyang Liu
Instigating oxidative stress is a crucial aspect of antibacterial therapy. Yet, its behavior is poorly understood in the context of zeolitic imidazolate frameworks (ZIFs) – a group of highly promising antibacterial agents. To address this gap, a series of ZIF@Ce6 particles were synthesized to investigate the impact of particle shape, size, and metal ion type on oxidative stress and bactericidal activity. For the first time, the interplay between the physicochemical properties and antibacterial activities of different ZIF@Ce6 particles is demonstrated, while unearthing their oxidative stress strategy in photodynamic therapy. Notably, the incorporation of chlorin e6 (Ce6), combined with light irradiation, amplified the bactericidal effect of the ZIFs and achieved a rare minimum inhibition concentration (MIC) of 12.5 µgmL -1 for ZIF-8. We discovered that singlet oxygen ( 1 O 2 ) production varies with particle shape and size, while photodynamic activity reshuffles the antibacterial performance sequence from pristine to modified ZIF-8. Interestingly, reactive oxygen species (ROS) accumulation and glutathione depletion tests revealed that oxidative stress in pristine ZIF-8 is predominantly induced by ROS, whereas both ROS and glutathione contribute to the oxidative stress in ZIF@Ce6 and pristine ZIF-67. When bacteria are preincubated with the antioxidant N-acetyl cysteine, the bactericidal activity of ZIF@Ce6 increases while the activity of pristine ZIF-8 is reduced and that of ZIF-67 remains unchanged. This study deepens our understanding of the antibacterial properties of ZIFs and their oxidative stress paths, paving way for the fabrication of ZIF-based materials with enriched and targeted antibacterial properties.
研究领域:
微生物学
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材料科学
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药理学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
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IF 8.328
Xia Chen,Wangyang Lu,Tiefeng Xu,Nan Li,Dandan Qin,Zhexin Zhu,Gangqiang Wang,Wenxing Chen
In nature, metalloporphyrins, such as chlorophyll, cytochrome P450 and so forth, are key materials in maintaining the ecological cycles, especially the carbon cycle, and play an important role in both photosynthesis and the catalytic oxidation of organisms. Inspired by these factors, we skillfully combined photocatalysis and biomimetic catalysis using imidazole (IMD)-functionalized modification of g-C 3 N 4 and axial coordination with hemin. Compared with pure hemin, g-C 3 N 4 and a mixture of the two, our novel catalytic system (g-C 3 N 4 -IMD-hemin/H 2 O 2 ) showed high photocatalytic oxidation activity for the degradation of 4-chlorophenol (4-CP), and the stability of hemin was enhanced under solar irradiation. Furthermore, the effect of pH and the sustained photocatalytic oxidation stability of g-C 3 N 4 -IMD-hemin for degrading 4-CP were investigated. The results indicated that g-C 3 N 4 -IMD-hemin presents a high photocatalytic oxidation activity over a wide pH range and exhibits good recyclability. A series of designed experiments showed that superoxide radicals ( O 2 − ), high-valent iron (Fe(IV) = O) species, peroxy radicals ( OOH) and few hydroxyl radicals ( OH) were generated in the g-C 3 N 4 -IMD-hemin/H 2 O 2 system. This synergistic photocatalytic and biomimetic process offers new insight for the utilization of solar energy and offers a new perspective for the exploration of catalysts for environmental remediation.
研究领域:
环境科学
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生物化学
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材料科学
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DOI
高影响因子
Catalysts
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2022
·Vol. 13
·期 1
·81
·
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
TOXICOLOGY AND APPLIED PHARMACOLOGY
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2025
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IF 3.4
Xuemin Xian,Xin Zhao,Xingchen Zhou,Hanfang Liu,Changxi Li,Xinquan Wu,Yuhang Chen,Keyue Ye,Hongwei Yang,Mingxi Li,Jianyun Yan,Xiuli Zhang
Vascular calcification (VC) is a common complication of chronic kidney disease (CKD), with oxidative stress identified as a key contributor to VC progression. Honokiol (HKL), a biphenolic compound derived from plants, has been found to be effective in treating various models of cardiovascular disease through the mitigation of oxidative stress. However, its effects on VC remain unexplored. To elucidate the effects of HKL on VC, a CKD rat model, a vitamin D 3 -overload-induced mouse model of vascular calcification, and a high-phosphate-induced human vascular smooth muscle cell (VSMC) calcification model were established. Calcification levels were assessed using Alizarin Red staining, calcium quantification, and Western blotting of osteogenic markers. Oxidative stress was assessed by measuring reactive oxygen species. Furthermore, transcriptome sequencing was employed to identify molecules and pathways affected by HKL. HKL was found to significantly reduce calcification in both in vivo and in vitro models. It also mitigated oxidative stress induced by high phosphate in human VSMCs. Mechanistically, HKL upregulated heme oxygenase-1 (HMOX-1), thereby inhibiting oxidative stress and reducing calcification. Pharmacological inhibition of HMOX-1 counteracted the protective effect of HKL on vascular calcification. In summary, the findings suggest that HKL ameliorates VC by upregulating HMOX-1 and decreasing oxidative stress.
研究领域:
医学
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药理学
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产品关联
DOI
PubMed
高影响因子
Food Bioscience
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2024
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IF 4.8
Ying Wu,Feiran Xu,Lingjie Kong,Xiaomin Li,Liangmin Wei,Baocai Xu
In this study, we investigated cooked hams to understand the relationship between display life and quality changes, as well as the microbiological characteristics of refrigerated storage for up to 90 days. Initially, the L* and a* values exhibited an initial decline with a gradual restitution to levels insignificantly disparate from those Day 15 hams. In contrast, the b* and h° values demonstrated an ascending pattern, indicating an augmentation in yellow intensity during the storage. Furthermore, there was an observable escalation in the C* value following 45 days of storage, implying an amplified luminosity and vividness of color during the latter phase of the storage period. Analyses of TBARS , TVB-N, and other physicochemical indexes indicated that the hams underwent deterioration during storage. Whereas, UV–vis and fluorescence spectroscopy illustrated that the pigment in cooked hams changed from nitrosylheme (NO-heme) to Zn-protoporphyrin IX (ZnPP) during storage. The NO-heme content decreased from 41.08 ± 0.44 to 12.76 ± 0.29 mg/kg, while the ZnPP content increased from 12.19 ± 0.41 to 89.44 ± 1.57 mg/kg. The structure of the bacterial community in the ham samples changed over the storage period. Towards the end of the shelf life, the microbial population was dominated by Lactic acid bacteria (LAB), particularly Latilactobacillus (34.91%) and Leuconostoc (19.73%). Redundancy analysis and Pearson correlation revealed a positive correlation between Latilactobacillus and Leuconostoc with TBARS , TVB-N, ZnPP content, and negative correlations with Aw and NO-heme.
研究领域:
食品科学
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微生物学
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产品关联
DOI
高影响因子