Scientific Reports
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2025
·Vol. 15
·期 1
·1-6
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IF 3.9
Li Wenfang,Lu Yuze,Wang Jiajun,Li Chuanbi
In this study, a novel artificial enzyme Zn(II)-SMM with simple organic structure for PNPA-directed hydrolysis is proposed. The introduction of hydrophobic quinoline and dipyridinium in Zn(II)-SMM system demonstrates high activity for the complexation of Zn 2+ and hydrolysis of PNPA, and the catalytic rate (k cat /k uncat ) exceeds 5239 times that of non-catalytic systems. The newly designed small molecule organic complex effectively binds to and catalyzes the hydrolysis of substrate PNPA in accordance with Michaelis-Menten kinetics. The mechanism with activation by single Lewis acid provides fundamental insights for the development of small molecule hydrolases.
研究领域:
生物化学
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分子生物学
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PubMed
高影响因子
RSC Advances
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2021
·Vol. 11
·期 26
·16090-16095
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IF 3.361
Heng-Fang Xiang,Jia-Kun Xu,Jiao Liu,Xin-Zhi Yang,Shu-Qin Gao,Ge-Bo Wen,Ying-Wu Lin
Synthetic dyes such as malachite green (MG) have a wide range of applications. Meanwhile, they bring great challenges for environmental security and cause potential damages to human health. Compared with traditional approaches, enzymatic catalysis is an emerging technique for wastewater treatment. As alternatives to natural enzymes, artificial enzymes have received much attention for potential applications. In previous studies, we have rationally designed artificial enzymes based on myoglobin (Mb), such as by introducing a distal histidine (F43H mutation) and creating a channel to the heme pocket (H64A mutation). We herein show that the artificial enzyme of F43H/H64A Mb can be successfully applied for efficient biodegradation of MG under weak acid conditions. The degradation efficiency is much higher than those of natural enzymes, such as dye-decolorizing peroxidase and laccase (13–18-fold). The interaction of MG and F43H/H64A Mb was investigated by using both experimental and molecular docking studies, and the biodegradation products of MG were also revealed by UPLC-ESI-MS analysis. Based on these results, we proposed a plausible biodegradation mechanism of MG. With the high-yield of overexpression in E. coli cells, this study suggests that the artificial enzyme has potential applications in the biodegradation of MG in fisheries and textile industries.
研究领域:
环境科学
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生物化学
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DOI
PubMed
高影响因子
Frontiers in Bioengineering and Biotechnology
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2021
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IF 5.89
Guo Wen-Jie,Xu Jia-Kun,Liu Jing-Jing,Lang Jia-Jia,Gao Shu-Qin,Wen Ge-Bo,Lin Ying-Wu
The conversion of Kraft lignin in plant biomass into renewable chemicals, aiming at harvesting aromatic compounds, is a challenge process in biorefinery. Comparing to the traditional chemical methods, enzymatic catalysis provides a gentle way for the degradation of lignin. Alternative to natural enzymes, artificial enzymes have been received much attention for potential applications. We herein achieved the biodegradation of Kraft lignin using an artificial peroxidase rationally designed in myoglobin (Mb), F43Y/T67R Mb, with a covalently linked heme cofactor. The artificial enzyme of F43Y/T67R Mb has improved catalytic efficiencies at mild acidic pH for phenolic and aromatic amine substrates, including Kraft lignin and the model lignin dimer guaiacylglycerol-β-guaiacyl ether (GGE). We proposed a possible catalytic mechanism for the biotransformation of lignin catalyzed by the enzyme, based on the results of kinetic UV-Vis studies and UPLC-ESI-MS analysis, as well as molecular modeling studies. With the advantages of F43Y/T67R Mb, such as the high-yield by overexpression in E. coli cells and the enhanced protein stability, this study suggests that the artificial enzyme has potential applications in the biodegradation of lignin to provide sustainable bioresource.
研究领域:
生物化学
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酶工程
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可再生资源
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lijun Yang,Jiaxing Zhang,Mengfan Wang,Yutong Wang,Wei Qi,Zhimin He
As bridging species between short peptides and macromolecular proteins, peptide assemblies not only provide a supramolecular approach for the fabrication of controllable molecular machines with enzyme-like functions, but also a simplified model for understanding the catalytic mechanism of natural enzymes. In this study, we focused on probing the effect of microenvironment on the catalytic behavior of peptide assemblies. Upon simply replacing the X residue in Fmoc-FFXAH-CONH 2 , we realized the modulation of the microenvironment of the amyloid assemblies, which thus appeared esterase-like function with different catalytic abilities. The chemistry , structure and activity were analyzed to explore the principles that how the hydrophobic, charged, polar and chiral microenvironment deciding the catalytic behavior of the esterase mimic. In addition, we also presented the potential of the catalytic assemblies in the encapsulation, delivery and enzymatic metabolization of a mutual prodrug . This work sheds new insights for understanding the structure–function relationship of catalytic peptide assemblies and natural enzymes, and also provides a new avenue for the designing of artificial enzymes with better functions.
研究领域:
生物化学
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分子生物学
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催化科学
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DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2017
·Vol. 23
·期 38
·9156-9161
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IF 5.317
Yanyan Huang,Fang Pu,Jinsong Ren,Xiaogang Qu
Graphical Of mimes and men : Based on the biocatalytic properties of artificial enzymes and the redox characteristic of glutathione, we designed a colorimetric and resettable biological operation to mimic intracellular enzyme-participated redox balance system. By using four artificial enzymes, three simple biological logic gates were fabricated. With the assistance of glutathione, the system could be easily reset without needing a complicated procedure. Owing to the biocatalytic properties of artificial enzymes and the redox characteristic of glutathione, a colorimetric and resettable biological operation was successfully designed to mimic enzyme-participated redox balance in living systems. As one promising candidate of a natural enzyme, artificial enzyme possesses many advantages and has been used in numerous fields. Similar to natural enzymes, communications are also present between different artificial enzymes. With the assistance of four artificial enzymes, three simple biological logic gates were fabricated to help us deepen the understanding of communications between artificial enzymes. In the presence of glutathione, the system could be easily reset without any complicated procedures. We prospect that this work may push forward the exploration of communications between different artificial enzymes and the design of novel artificial enzyme-based biological gates or nanodevices. We hope that our mimic system may help us further understand the functioning of complex biological pathways in biological systems.
研究领域:
生物化学
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合成生物学
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纳米技术
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DOI
PubMed
高影响因子
JOURNAL OF INORGANIC BIOCHEMISTRY
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2017
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IF 3.348
Xin Li,Zihui Liu,Ying Xu,Dongfeng Wang
A novel heterobinuclear complex [CoNa(C 15 H 10 NO 4 F) 2 (CH 3 OH)] 2 with Schiff base (C 15 H 10 NO 4 F: 2-amino-4-fluorobenzoic acid-3-methoxysalicylaldehyde) was synthesized and characterized by IR and 1 H NMR spectroscopy, elemental analysis and single crystal X-ray diffraction. X-ray crystallography reveals that the cobalt atom is six-coordinated by two nitrogen atoms from –C N–, two carboxylate oxygen atoms and two hydroxyl oxygen atoms in different ligands, while the sodium atom is seven-coordinated by two methoxy oxygen atoms, two hydroxyl oxygen atoms in different ligands, two oxygen atoms in the same carboxylate and one oxygen atom of solvent methanol. The reaction results of the complex with the p -nitrophenylphosphate (pNPP) and the adenosine monophosphate (AMP) reveal that the complex can hydrolyze phosphoester bonds. Then the DNA-hydrolysis activity is studied experimentally and theoretically, indicating that the complex can effectively hydrolyze the pBR322 supercoiled plasmid DNA . The molecular docking technology predicts the best binding site and binding affinity between the complex and DNA, and then the catalytic mechanism of hydrolysis is supposed. The study results suggest that the Schiff base metal complex, as a potent artificial enzyme , may find its applications in catalytic hydrolysis and biotechnological areas.
研究领域:
配位化学
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生物无机化学
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催化化学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2018
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IF 8.097
Ruibo Zhong,Mingshu Xiao,Changfeng Zhu,Xizhong Shen,Qian Tang,Weijia Zhang,Lihua Wang,Shiping Song,Xiangmeng Qu,Hao Pei,Cheng Wang,Li Li
By incorporating hemin into G-quadruplex (G4) during cation-templated self-assembly between guanosine and KB(OH)4, we have constructed an artificial enzyme hydrogel (AEH)-based system for the highly sensitive and selective detection of Pb2+. The sensing strategy is based on a Pb2+-induced decrease in AEH activity. Because of the higher efficiency of Pb2+ for stabilizing G4 compared with K+, the Pb2+ ions substitute K+ and trigger hemin release from G4, thus giving rise to a conformational interconversion accompanied by the loss of enzyme activity. The Pb2+-induced catalytic interconversion endows the AEH-based system with high sensitivity and selectivity for detecting Pb2+. As a result, the AEH-based system shows an excellent response for Pb2+ in the range from 1 pM to 50 nM with a limit of detection of ∼0.32 pM, which is much lower than that of the previously reported G4-DNAzyme. We also demonstrate that this AEH-based system exhibits high selectivity toward Pb2+ over other metal ions. Furthermore, two two-input INHIBIT logic gates have been constructed via switching of the catalytic interconversion induced by K+ and Pb2+ or K+ and pH. Given its versatility, this AEH-based system provides a novel platform for sensing and biomolecular computation.
研究领域:
生物化学
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分析化学
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分子生物学
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DOI
PubMed
高影响因子
BIOTECHNOLOGY AND APPLIED BIOCHEMISTRY
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2023
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IF 2.8
Jiayi Jiang,Bin Wang,Linghuan Luo,Na Ying,Gaofan Shi,Mengmeng Zhang,Haoyuan Su,Dongdong Zeng
In this study, an electrochemical biosensor was constructed for the detection of fibrin, specifically by a simple two-step approach, with a novel artificial enzyme (Tetrazyme) based on the DNA tetrahedral framework as signal probe. The multichannel screen-printed electrode with the activated surface cannot only remove some biological impurities, but also serve as a carrier to immobilize a large number of antigen proteins. The DNA tetrahedral nanostructure was employed to ensure the high sensitivity of the probe for biological analysis. The hemin was chimeric into the G-quadruplex to constitute the complex with peroxidase catalytic activity (hemin/G4-DNAzyme), subsequently, Tetrazyme was formed through combining of this complex and DNA tetrahedral nucleic acid framework. The artificial enzyme signal probe formed by the covalent combination of the homing peptide (Cys-Arg-Glu-Lys-Ala, CREKA), which is the aptamer of fibrin and the new artificial enzyme is fixed on the surface of the multichannel carbon electrode by CREKA-specific recognition, so as to realize the sensitive detection of fibrin. The feasibility of sensing platform was validated by cyclic voltammetry (CV) and amperometric i – t curve (IT) methods. Effects of Tetrazyme concentration, CREKA concentrations and hybridization time on the sensor were explored. Under the best optimal conditions of 0.6 μmol/L Tetrazyme, 80 μmol/L CREKA, and 2.5 h reaction time, the immunosensor had two linear detection ranges, 10–40 nmol/L, with linear regression equation Y = 0.01487 X − 0.011 ( R 2 = 0.992), and 50–100 nmol/L, with linear regression equation Y = 0.00137 X + 0.6405 ( R 2 = 0.998), the detection limit was 9.4 nmol/L, S / N ≥ 3. The biosensor could provide a new method with great potential for the detection of fibrin with good selectivity, stability, and reproducibility.
研究领域:
生物技术
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医学检测
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纳米生物学
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DOI
PubMed
高影响因子
DYES AND PIGMENTS
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2018
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IF 3.767
Chao Yang,Wenjun Feng,Yong Li,Xike Tian,Zhaoxin Zhou,Liqiang Lu,Yulun Nie
To develop a highly sensitive colorimetric detection method for the diabetes early diagnosis by determining the glucose in urine instead of blood can avoid the painful blood collection and risks of cross infection. In this paper, novel artificial enzyme mimics were formed by loading bimetallic nanoparticle Fe Pd on the surface of reduced graphene (rGO). Also, we proposed a Fe Pd/rGO coupled with portable paper sensor for the detection of glucose in urine. The results indicated that urine glucose can be sensitively detected in a wide range of 1–200 μM with a limit of detection (LOD) of 1.76 μM. Most important, the color difference along with the increase of urine glucose concentration can be easily distinguished by naked eyes, which is important to its practical usage in screening and diagnosis of diabetes. Furthermore, the reason of the high sensitivity of Fe Pd/rGO towards glucose was investigated in detail via various probing experiments. Fe Pd/rGO has an artificial enzyme mimic activity, which can catalyze O 2 and generate H 2 O 2 from glucose oxidation . The electron transfer between Fe Pd and H 2 O 2 will produce • OH that can oxidize terephthalic acid (TMB) by emitting a blue color. The findings in this study provide a promising alternative for the early screening and diagnosis of diabetes.
研究领域:
生物化学
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医学诊断
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纳米材料科学
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2020
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IF 5.977
Meng Li,Jie Lv,Shuangling Wang,Jing Wang,Yulong Lin
Design of synthetic structures that possess the similar functions to natural enzymes held great promise in environmental detection and biomedical application. Herein, a new concept for the fabrication of solid-supported catalysts as peroxidase mimic have been proposed to realize high-catalytic activity and stability by utilizing expanded mesoporous silica (EMSN)-encapsulated Pt nanoclusters . Compared with PtNCs, the introduction of amino group modified EMSN would enrich H 2 O 2 on the surface of PtNCs and increase the catalytic sites for H 2 O 2 decomposition, which gave rise to the higher catalytic activity of EMSN-PtNCs over a broad pH range, especially in weakly acidic and neural solutions. This would facilitate their applications for real-time monitoring the secretion of H 2 O 2 from living cancer cells stimulated by various anticancer drugs . Our findings not only pave the way to use porous matrix as the structural component for the design of the biomimetic catalysts , but also provide a simple and reliable platform to monitor H 2 O 2 released from living cells in real time, which holds great potential for elucidating the biological roles of H 2 O 2 and underlying molecular mechanisms of drug cytotoxicity as well as drug therapeutic effects.
研究领域:
生物医学
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材料科学
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催化化学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Lei Jiang,Miguel Tinoco,Susana Fernández-García,Yujiao Sun,Mariia Traviankina,Pengli Nan,Qi Xue,Huiyan Pan,Almudena Aguinaco,Juan M. González-Leal,Ginesa Blanco,Eduardo Blanco,Ana B. Hungría,Jose J. Calvino,Xiaowei Chen
In this work, a simple one-step thermal oxidation process was established to achieve a significant surface increase in {110} and {111} nanofacets on well-defined, pure and Pr-doped, ceria nanocubes. More importantly, without changing most of the bulk properties, this treatment leads to a remarkable boost of their enzymatic activities: from the oxidant (oxidase-like) to antioxidant (hydroxyl radical scavenging) as well as the paraoxon degradation (phosphatase-like) activities. Such performance improvement might be due to the thermally generated sawtoothlike {111} nanofacets and defects, which facilitate the oxygen mobility and the formation of oxygen vacancies on the surface. Finally, possible mechanisms of nanoceria as artificial enzymes have been proposed in this manuscript. Considering the potential application of ceria as artificial enzymes, this thermal treatment may enable the future design of highly efficient nanozymes without changing the bulk composition.
研究领域:
材料科学
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生物化学
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纳米医学
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PubMed
高影响因子
Advanced Science
·
2021
·Vol. 9
·期 3
·2104205
·
IF 16.806
Suya Zhou,Shuo Yang,Dong Cai,Ce Liang,Shuang Yu,Yue Hu,Huagui Nie,Zhi Yang
Lithium–sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor-assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin on carboxylated carbon nanotubes (CNTs) (i.e., [CNTs–MM–hemin]), is presented to efficiently convert polysulfides. The MM cofactors bind with the hemin artificial enzymes and CNT conductive substrates through FeN 5 coordination and/or covalent amide bonds to provide high and durable catalytic activity for polysulfide conversions, while π – π conjugations between hemin and CNTs and multiple Li-bond networks offered by MM endow the cathode with good electronic/Li + transmission ability. This synergistic mechanism enables rapid sulfur reaction kinetics, alleviated polysulfide shuttling, and an ultralow (<1.3%) loss of hemin active sites in electrolyte, which is ≈60 times lower than those of noncovalent crosslinked samples. As a result, the Li–S battery using [CNTs–MM–hemin] cathode retains a capacity of 571 mAh g −1 after 900 cycles at 1C with an ultralow capacity decay rate of 0.046% per cycle. Even under raising sulfur loadings up to 7.5 mg cm −2 , the cathode still can steadily run 110 cycles with a capacity retention of 83%.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）