ACS Applied Materials & Interfaces
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2018
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IF 8.097
Zhenning Liu,Bingdi Wang,Shenghui Jin,Zhida Wang,Lei Wang,Song Liang
In this paper, a novel method for the construction of colloidosomes as a microreactor for dual-enzyme cascade biphasic reaction has been reported. A lipase–glucose oxidase (GOx) enzyme pair is employed in this system. A water-soluble enzyme GOx is compartmentalized inside the colloidosomes. A hydrophobic environment-favored enzyme Candida Antarctica lipase B (CalB) is adsorbed on the outer surfaces of the colloidosomes. The catalysis system is set up by introducing these dual-enzyme-immobilized microcapsules into acetic ether. H2O2 is produced in the aqueous phase by the doped GOx, and then H2O2 diffused out of the microcapsules is utilized by CalB to catalyze the oxidation of ethyl acetate. Finally, the formed peracids oxidized N-heteroaromatic in situ. Furthermore, no obvious yield decline is observed in four reaction cycles. Thus, our work provides a new strategy for the design of high-performance biomimicking reactors for multiple enzyme cascade reactions and further expands the potential application area of colloidosomes.
研究领域:
生物化学
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材料科学
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PubMed
高影响因子
Catalysts
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2023
·Vol. 13
·期 2
·267
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IF 3.9
Jia Wu,Bao-Di Ma,Yi Xu
A novel and efficient one-pot three-enzyme cascade method for the synthesis of β-alanine from maleic acid was developed. Two recombinantE. colistrains were constructed. TheE. coli(MaiA-AspA) co-expressing maleiccis-trans isomerase (MaiA) and L-aspartase (AspA) catalyzed the biotransformation of maleic acid to L-aspartate via fumaric acid, andE. coli(ADC) expressing L-aspartate-α-decarboxylase (ADC) catalyzed the bioconversion of L-aspartate to β-alanine. After systematic optimization of reaction conditions for each strain, the whole cells of two strains were combined for one-pot synthesis of β-alanine. It was found that the ratio of the two kinds of cells as well as the cell amount play critical roles in the reaction rate and yield of β-alanine. Adding two kinds of cells in one-pot at the beginning of the reaction was better than adding step by step. Under optimal conditions, the concentration of β-alanine reached 751 mM after a 9 h reaction, corresponding to a 93.9% yield and 178 g/L/d space-time yield. The developed new route showed application potential for green and efficient biosynthesis of β-alanine from a cheap substrate by tandem biocatalysts.Keywords:β-alanine;cascade reaction;biotransformation;one-pot
研究领域:
生物化学
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合成生物学
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2024
·Vol. 171
·期 8
·085501
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IF 3.1
Yinghong Zhu,Minling Zhou,Zhanbang Ge,Yufeng Jiao,Menghui Wang,Wujin Peng
An efficient and transition-metal-free synthesis strategy of aromatic nitriles from corresponding aldehydes with H2SO4(NH2OH)2 as the nitrogen source and Cl−/ClO− as the redox mediator was developed. The redox Cl−/ClO− showed electrochemical reversibility in acidic condition. The possible mechanism involving the transformation of Cl−, the generation and electrochemical reduction of nitrile oxides based on the results of cyclic voltammetry and constant current electrolysis was proposed.
研究领域:
有机化学
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电化学
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高影响因子
Molecular Catalysis
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2023
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IF 4.6
Bin Wu,Xiangyun Wang,Bo Yang,Yunjian Ma,Frank Hollmann,Yonghua Wang
In the present work we propose a bienzymatic cascade for the oxyfunctionalisation of cycloalkanes to cyclic alcohols/cyclic ketones. By combining a H 2 O 2 -dependent peroxygenase with a O 2 -consuming and H 2 O 2 -producing alcohol oxidase an overall aerobic oxidation system was established. A convincing proof-of-concept is presented and some current limitations are outlined.
研究领域:
生物化学
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酶工程
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2017
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IF 5.951
Xueyan Zhang,Yue Li,Lifang Xue,Shengtian Wang,Xiaohong Wang,Zijiang Jiang
A series of Lewis acid metals monosubstituted phosphotungstic acids HnPW11MO39 (HPWM, M = CuII, ZnII, CrIII, FeIII, SnIV, TiIV, and ZrIV; for Ti and Zr, the number of oxygen is 40) was evaluated in direct production of methyl levulinate (ML) from cellulosic biomass in a cascade reaction. One of the solid catalysts, H5PW11TiO40 (HPWTi), was found to be highly efficient for generation of ML from mono- or polysaccharides, reaching 51.3% ML yield directly from cellulose. And under microwave-assistance, the efficiency could be improved to a 62.6% ML yield within 2 h, which was almost the best result so far among reported solid catalysts. Identification of the reaction intermediates and the products provided some insight into the reaction mechanism and showed the requirement of certain Brønsted/Lewis acid ratio as 2.84/1 for HPWM. Moreover, the different metals in catalysts profoundly affected the Lewis or total acidity, and therefore, the catalytic activity and selectivity to ML or methyl glucosides (MG). HPWTi acted as a heterogeneous catalyst after being calcinated at 200 °C and showed high recyclability with minor loss of performance.
研究领域:
化学工程
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生物质能
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高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Ran Wang,Wei Song,Hangyuan Xu,Jian Wen,Wanqing Wei,Zhaoyang Chen,Guipeng Hu,Cong Gao,Xiaomin Li,Jia Liu,Jing Wu
l-Asparagine (l-Asn) is an important amino acid with broad applications in food, medicine, fine chemicals, and environmental protection. However, its industrial production is limited by the high cost of raw materials and the low catalytic efficiency of enzymes. In this study, a three-enzyme cascade pathway (FDN) was designed to produce l-Asn, using fumaric acid as the raw material. Within this pathway, EcAsnA was identified as the rate-limiting enzyme and was subsequently engineered using a product rescue strategy to reduce product inhibition by opening the closed gate. The optimal mutant, L109 K/K58R, exhibited a 6.61-fold reduction in product inhibition and a 4.24-fold improvement in catalytic efficiency. This mutant was then integrated into Escherichia coli along with the other two enzymes to construct the optimal recombinant strain E. coli 17. Using diatomite-glutaraldehyde cross-linking immobilized E. coli 17 as a biocatalyst, 267.74 g of l-Asn (with 5.35 g·L–1·h–1 STY, > 99% ee) was produced across 50 batch feedings in 1 L reaction volume. The purity of l-Asn exceeded 99% after isolation and purification. This study demonstrates the effective integration of cascade reaction design, enzyme engineering, and cell immobilization, providing a promising approach for synthesizing high-value products from cost-effective substrates.
研究领域:
生物化学
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酶学
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合成生物学
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高影响因子
Jove-Journal of Visualized Experiments
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2019
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IF 1.108
Zhiping Zhang,Shuhang Fan,Zhiqiang Chen,Yanzhi He,Mengfei Huang,Li Ding,Yanyan Zhang,Lin Chen,Xinyue Zhang
Flavonols are a major subclass of flavonoids with a variety of biological and pharmacological activities. Here, we provide a method for the in vitro enzymatic synthesis of a flavonol. In this method, Atf3h and Atfls1, two key genes in the biosynthetic pathway of the flavonols, are cloned and overexpressed in Escherichia coli. The recombinant enzymes are purified via an affinity column and then a bienzymatic cascade is established in a specific synthetic buffer. Two flavonols are synthesized in this system as examples and determined by TLC and HPLC/LC/MS analyses. The method displays obvious advantages in the derivation of flavonols over other approaches. It is time- and labor-saving and highly cost-effective. The reaction is easy to be accurately controlled and thus scaled up for mass production. The target product can be purified easily due to the simple components in the system. However, this system is usually restricted to the production of a flavonol from a flavanone.
研究领域:
生物化学
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分子生物学
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DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2020
·Vol. 95
·期 5
·1421-1430
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IF 2.75
Yuanyuan Zhang,Yangjian Sun,Wenjie Ren,Qiuxiang Zhao,Kuiying Lv,Hui Tang,Xin Gao,Fengke Yang,Fanye Wang,Junhong Liu
BACKGROUND Mitomycin C (MMC) is one of the most important members of the mitomycin family that have been widely used as a strong antineoplastic antibiotic for treating various tumors. In this study, enzymatic oxidation/amination reaction of 2-methyl-1,4-hydroquinone with n -butylamine was carried out to synthesize 2-methyl-3- n -butylaminoyl-1,4-benzoquinone mitomycin analogs. RESULTS A kinetic model was developed based on an ordered sequential mechanism for this cascade reaction system catalyzed by two enzymes, which revealed that the limiting step of the system was the laccase-mediated oxidation of 2-methyl-3- n -butylaminoyl-4-hydro-1-quinone and removing the limiting step resulted in a yield increase from 88.3% to 96.7%. CONCLUSION The developed kinetic model fitted the test data very well, indicating that the reactions catalyzed by coupling of laccase with lipase might follow the ordered sequential mechanism with product inhibition. Synthesis of mitomycin analogs catalyzed by coupling of laccase with lipase has great potential for practical application. © 2020 Society of Chemical Industry
研究领域:
生物化学
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药物化学
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酶工程
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高影响因子
LIFE SCIENCES
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2023
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IF 6.1
Qingbo Yang,Chuangqi Mo,Pengfei Cui,Shuwen Zhou,Lin Qiu,Pengju Jiang,Yang Xuan,Hai Huang,Cheng Wang,Jianhao Wang
Aims Bacterial infection is a significant factor contributing to the deterioration of wounds, and the misuse of antibiotics has exacerbated bacterial resistance. Therefore, there is an urgent need to develop a novel antibacterial strategy to replace conventional therapies. This study aims to construct a self-activated cascade reaction nanozyme, f-FeNC@GOx, which triggers a cascade reaction in the presence of glucose. This cascade reaction generates highly toxic hydroxyl radicals ( OH), thereby achieving the goal of eliminating bacteria and promoting wound healing. Material and methods In vitro antibacterial experiments, bacterial spread plate method, Live/Dead staining, and crystal violet staining were conducted to analyze the antibacterial ability and mechanism of f-FeNC@GOx. In vivo experiments, a mouse wound model was established, and H&E and Masson staining of wound tissues were performed to assess the antibacterial activity of the f-FeNC@GOx in vivo . Key findings The in vivo and in vitro experiments confirmed that f-FeNC@GOx exhibited significant antibacterial effect against both Staphylococcus aureus and Escherichia coli in the presence of glucose. Furthermore, it showed optimal wound healing performance in the wound models. Significance These findings suggested that f-FeNC@GOx was a novel and effective antibacterial nanomaterial, which provided a promising antibacterial strategy using nanoenzyme based cascade reaction.
研究领域:
生物医学工程
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纳米医学
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微生物学
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DOI
PubMed
高影响因子
GREEN CHEMISTRY
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2021
·Vol. 23
·期 6
·2427-2436
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IF 10.182
Jifeng Pang,Bo Zhang,Yu Jiang,Yu Zhao,Changzhi Li,Mingyuan Zheng,Tao Zhang
The complete conversion of hemicellulose, cellulose and lignin in lignocellulosic biomass into value-added chemicals is of great significance in biorefinery processes. Herein, a cascade-step strategy was developed for the conversion of hemicellulose and lignin into mixed organic acids, and cellulose into ethylene glycol. Typical biomass of Miscanthus was first treated with formic acid in the presence of H2O2, giving a formic acid solution and cellulosic biomass. Lignin in Miscanthus was oxidized to low polymerized organic acids through linkage cleavages and aromatic ring ruptures during the treatment process, forming a homogeneous formic acid solution with a weight yield of 95%. Hemicellulose was transformed into maleic acid at 56.2% selectivity via a hydrolysis–dehydration–oxidation process. Both hemicellulose and lignin were degraded into organic acids with an overall weight yield of 92.4%. The cellulose in the solid residue had a hydrophilic surface and is highly accessible to catalysts in the aqueous solution, and it was totally converted into ethylene glycol with a yield of up to 65.7% over a binary catalyst of H2WO4–Ru/C. Relying on such a cascade reaction strategy, the three major components of Miscanthus were transformed into mixed organic acids and ethylene glycol, which provides a potential strategy for complete valorisation of biomass into value-added chemicals.
研究领域:
生物化学
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可再生资源与环境科学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
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2022
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IF 5.304
Jin-Hong Sui,Yun-Yun Wei,Jin Li,Zhang-Run Xu
Mucin 1 (MUC1) is an important tumor biomarker, and the determination of MUC1 is of great significance in clinical diagnostics, prognosis assessment and therapy monitoring. Developing point-of-care testing method of MUC1 is necessary in resource-limited settings. Herein, a visual multicolor aptasensor for MUC1 detection was designed based on an alkaline phosphatase (ALP)-triggered cascade reaction. In the presence of MUC1, ALP-decorated complementary DNA and MUC1 aptamer on magnetic beads were dissociated due to the recognition between MUC1 and aptamer. With the assistance of a magnet, ALP-decorated complementary DNA was separated and collected to catalyze the hydrolysis of l -ascorbic acid-2-phosphate generating l -ascorbic acid, which etched the manganese dioxide nanosheets to mediate the oxidation reaction of 3,3′,5,5′-tetramethylbenzidine sulfate, resulting in different products with distinct visible multicolor. The naked eye detection of MUC1 was realized and the detection limit was estimated to be 0.18 U mL −1 by using the colorimetric method. This proposed aptasensor possesses the merit of vivid multicolor change, and provides a new way for MUC1 detection by naked eyes.
研究领域:
生物医学工程
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临床诊断学
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分子生物学
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DOI
高影响因子
GREEN CHEMISTRY
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2024
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IF 9.3
Daocheng Liao,Shiming Tang,Ying Lin,Suiping Zheng
1,3-Propanediamine is a diamine widely used in microelectronics and porous materials. It can also be used as a curing agent for epoxy resin, forming valuable three-dimensional structures, or as a raw material for synthesizing the radiation-resistant drug amifostine. However, traditional chemical synthesis methods for producing 1,3-propanediamine often contradict the 12 principles of green chemistry. In this study, we designed a new pathway for producing 1,3-diaminopropane through a retrosynthetic-designed multi-enzyme cascade from crude glycerol in vitro. Compared with traditional chemical methods, this multienzyme cascade is simpler in process, less energy-consuming, cleaner in substrate usage, and more environmentally friendly. In the cascade reaction, we selected glycerol dehydratase (KpGDHT) to dehydrate the intermediate product 3-amino-1,2-propanediol based on substrate promiscuity. We then modified the substrate preference of KpGDHT to obtain the optimized mutant KpGDHT/Q337A/S302D, which exhibited a 4.4-fold increase in activity toward 3-amino-1,2-propanediol compared with the wild-type KpGDHT. Using KpGDHT/Q337A/S302D as the catalyst, 3.8 mM 1,3-diaminopropane was produced from 5 mM glycerol within 8h under optimal conditions, achieving 76% conversion efficiency. Finally, we evaluated the performance of 1,3-diaminopropane synthesized from crude glycerol and obtained 1,3-diaminopropane with a concentration of 3.95 mM, which is comparable to that from pure glycerol. Given its robustness and environmental benefits, this proposed cascade reaction pathway has great potential to produce 1,3-diaminopropane on an industrial scale.
研究领域:
生物化学
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合成生物学
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环境科学
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高影响因子
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