ACS Catalysis
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2025
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IF 13.1
Shihao Li,Jiafu Shi,Yu Chen,Xinyu Mao,Shusong Liu,Yang Yang,Hong Wu,Zhongyi Jiang
Amino alcohols are widely used in chemical and pharmaceutical industries, while conventional synthesis methods face drawbacks such as low selectivity and high energy consumption. Multienzyme catalysis combined with light-driven cofactor regeneration affords a platform of light-driven synthesis of chemicals, where the transfer of electrons and protons as well as the route of enzymatic reactions dominates the energy conversion efficiency and atomic economy of carbon utilization. Herein, we construct a light-driven synthesis system comprising an energy-supplying module and a multienzyme catalytic module for 2-aminoethanol synthesis from formaldehyde and ammonia. First, a S-scheme heterojunction photocatalysts with a metal–organic framework core and a bipyridine-based conjugated polymer shell are prepared as an energy-supplying module. Through synergistic intensification of proton transfer and electron transfer, the photocatalysts render cofactor (NADH) regeneration efficiency with a turnover frequency of 30.49 h–1. Second, a multienzyme catalytic module is constructed for 2-aminoethanol synthesis in the presence of NADH. Under optimal conditions, this module produces 2-aminoethanol with an average reaction rate of 76.34 μmol L–1 h–1 within 24 h. Finally, the energy-supplying module is coupled with the multienzyme catalytic module for continuous synthesis of 2-aminoethanol from formaldehyde and ammonia, generating 0.55 mmol L–1 2-aminoethanol after 4 light–dark cycles. In addition, triethanolamine (TEOA) and glucose, a biomass-derived carbon source, are both confirmed as effective electron donors for NADH regeneration and light-driven synthesis system. This work opens a pathway for the synthesis of amino alcohols and demonstrates a paradigm for the intensification of reaction processes.
研究领域:
生物化学
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绿色化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yang Yang,Jiafu Shi,Yu Chen,Shihao Li,Han Wang,Wenping Li,Shusong Liu,Xinyu Mao,Hong Wu,Zhongyi Jiang
Rational design of immobilized enzyme catalysts based on covalent organic framework (COF) with high enzyme loading and superior robustness is highly desired. Herein, we designed an immobilized enzyme catalyst based on bifunctional COF. The quaternary ammonium-functionalized COF nanosheets adsorbed enzymes and subsequently induced the in-situ formation of silica coating without additional reagents. The ultrathin COF nanosheets guaranteed high enzyme loading of 3.4 mg mg −1 . Meanwhile, quaternary ammonium groups on COF induced the formation of silica coating on the surface of COF, where the as-formed silica coating protected the fragile enzyme. The stability of the enzyme in immobilization form increased by 165 %, 113 % and 44 %, respectively, compared to the enzyme directly adsorbed on COF under different conditions (50 °C, pH 11, or after five cycles). Furthermore, given the high enzyme loading of COF nanosheets, an immobilized multi-enzyme catalytic system was constructed to convert methanol to ethylene glycol via a four-enzyme cascade reaction, which exhibited 143 % increase in catalytic activity by contrast with free enzymes system. This study provides a promising approach for enzyme immobilization and extends the application of COF in biocatalysis.
研究领域:
生物化学
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材料科学
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酶工程
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产品关联
DOI
高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 9
·2171
·
IF 5.076
Le Wang,Pengxue Sun,Yiyu Yang,Hanzhen Qiao,Hailong Tian,Dapeng Wu,Shuoye Yang,Qipeng Yuan,Jinshui Wang
The field of enzyme cascades in limited microscale or nanoscale environments has undergone a quick growth and attracted increasing interests in the field of rapid development of systems chemistry. In this study, alcohol dehydrogenase (ADH), lactate dehydrogenase (LDH), and mesoporous silica nanoparticles (MSN) immobilized nicotinamide adenine dinucleotide (NAD+) were successfully immobilized on the zeolitic imidazolate frameworks (ZIFs). This immobilized product was named ZIF@ADH/NAD-MSN/LDH, and the effect of the multi-enzyme cascade was studied by measuring the catalytic synthesis of lactic acid. The loading efficiency of the enzyme in the in-situ co-immobilization method reached 92.65%. The synthesis rate of lactic acid was increased to 70.10%, which was about 2.82 times that of the free enzyme under the optimal conditions (40 °C, pH = 8). Additionally, ZIF@ADH/NAD-MSN/LDH had experimental stability (71.67% relative activity after four experiments) and storage stability (93.45% relative activity after three weeks of storage at 4 °C; 76.89% relative activity after incubation in acetonitrile-aqueous solution for 1 h; 27.42% relative activity after incubation in 15% N, N-Dimethylformamide (DMF) solution for 1 h). In summary, in this paper, the cyclic regeneration of coenzymes was achieved, and the reaction efficiency of the multi-enzyme biocatalytic cascade was improved due to the reduction of substrate diffusion.Keywords:confinement effect;multi-enzyme catalytic cascade;in-situ synthesis;coenzyme recycling;co-immobilization enzyme
研究领域:
生物化学
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纳米生物学
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系统化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Le He,Gang Ding,Sasha You,Si Lu,Xianfeng Huang,Ling Li,Xiaolan Yu
Nanozymes that mimic the catalytic reaction of natural enzymes show great prospects for tumor catalytic therapy because they possess the properties of nanomaterials and natural enzymes. However, the therapeutic effect of nanozymes is restricted by the low catalytic efficiency and specific oxidation–reduction systems in the tumor microenvironment (TME), such as overexpressed glutathione (GSH) level. In order to improve the catalytic efficiency, a multifunctional nanozyme, Cu/zeolitic imidazolate framework-67 (ZIF-67)/Prussian blue (PB), was designed through the modification of Prussian blue (PB) on the surface of the copper-doped zeolitic imidazolate framework, which can be used for imaging-guided synergistic therapy with photothermal-enhanced multienzyme-like catalytic therapy and chemotherapy. The doping of Cu2+ provided better glutathione oxidase-like (GPx-like) activity and peroxidase-like (POD-like) activity to deplete GSH and increase the generation of •OH in TME. The modification of PB provided better catalase-like activity (CAT-like) to promote the production of O2 and enhance the multienzyme-like catalytic therapy. In vivo experiments showed a satisfactory anticancer effect. This work thus provided a strategy for designing a type of multifunctional nanozyme for imaging-guided combination therapy.
研究领域:
生物医学工程
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纳米医学
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肿瘤学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2018
·Vol. 54
·期 3
·2535-2551
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IF 2.993
Shen Hao,Song Jiayi,Yang Ye,Su Ping,Yang Yi
The exploration of new tactics for manufacturing artificial immobilized multi-enzyme systems based on enzyme cascades has recently attracted considerable interest because of the urgent need for multi-enzyme catalysts and the high cost of free enzymes. Because of the inevitable limitations of native enzymes such as instability and storage issues, the development of nanozyme–enzyme cascades is needed. A versatile strategy was developed for fabricating an efficient multi-catalyst system by immobilizing glucose oxidase (GO x ) on ferriferous oxide nanocomposites functionalized with nitrogen-doped graphene quantum dots (Fe 3 O 4 @N-GQDs) through DNA-directed immobilization. The Fe 3 O 4 @N-GQDs acted as a carrier for the natural enzyme and showed high peroxidase activity which enabled an enzyme cascade that included GO x to be set up. This multi-catalyst system showed great catalytic activity, reversibility and operational stability. The surfaces of GO x -targeted magnetic nanoparticles were regenerated by mild dehybridization of DNA. The Michaelis constant ( K m ) and maximum initial velocity ( V max ) of the multi-catalyst system were 1.069 mM and 11.2 × 10 −8 M s −1 , respectively, which are considerably better than the corresponding values for adsorbed and free bienzyme combinations. The increased bioactivity of the multi-catalyst system is ascribed to the satisfactory peroxidase-like activity of Fe 3 O 4 @N-GQDs, the enzyme–promoting effect of the QDs and enhancement by DNA-directed immobilization. Because of the diverse range of possible nanozyme–enzyme combinations and high efficiency of this approach, this work provides a novel pathway for the manufacturing of synthetic enzyme catalyst systems, which have great potential in the field of biotechnology.
研究领域:
生物技术
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酶工程
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纳米生物学
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DOI
高影响因子
Frontiers in Microbiology
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2023
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IF 5.2
Liu Quanzhen,Wei Guoguang,Yang Pengfan,Wang Chengyong,Chen Kequan,Ouyang Pingkai,Zhang Alei
N-acetylneuraminic acid (Neu5Ac) possesses the ability to promote mental health and enhance immunity and is widely used in both medicine and food fields as a supplement. Enzymatic production of Neu5Ac using N-acetyl-D-glucosamine (GlcNAc) as substrate was significant. However, the high-cost GlcNAc limited its development. In this study, an in vitro multi-enzyme catalysis was built to produce Neu5Ac using affordable chitin as substrate. Firstly, exochitinase SmChiA from Serratia proteamaculans and N-acetylglucosaminosidase CmNAGase from Chitinolyticbacter meiyuanensis SYBC-H1 were screened and combined to produce GlcNAc, effectively. Then, the chitinase was cascaded with N-acetylglucosamine-2-epimerase (AGE) and N-neuraminic acid aldolase (NanA) to produce Neu5Ac; the optimal conditions of the multi-enzyme catalysis system were 37°C and pH 8.5, the ratio of AGE to NanA (1:4) and addition of pyruvate (70 mM), respectively. Finally, 9.2 g/L Neu5Ac could be obtained from 20 g/L chitin within 24 h along with two supplementations with pyruvate. This work will lay a good foundation for the production of Neu5Ac from cheap chitin resources.
研究领域:
生物技术
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酶学
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食品科学
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医学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
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IF 16
Tonghui Jin,Sophally Chhong,Mingqin Li,Jiangtao Zhou,Qize Xuan,Jiaqi Su,Ming Dai,Mohammad Peydayesh,Zhou Dong,Qiyao Sun,Mattia Usuelli,Raffaele Mezzenga
Enzyme immobilization is an efficient and cost-effective approach to recovering, stabilizing, and enhancing enzyme catalytic properties. It is a challenge, however, for coimmobilized multiple enzymes to perform consecutive reactions without being inactivated under similar conditions. Here, we present a facile enzyme immobilization platform using β-lactoglobulin amyloid fibril hydrogels. Two different hydrogels, loading either RuBisCO alone (hereby termed AFR*) or seven enzymes related to the Calvin Cycle (hereby termed AF7E hydrogel), show immobilization efficiency of over ∼95% while simultaneously exhibiting excellent activity and stability. The AFR* hydrogel enables the fixation of CO2 into 3-phosphoglycerate (3-PGA), which is then utilized as the initial step in the Calvin Cycle cascade catalytic reactions if the AF7E hydrogel is used, mimicking the light-independent part of the more complex natural photosynthesis full process. The converted substrates of this process contain precursors (α-glycerophosphate dehydrogenase and dihydroxyacetone phosphate), which can be further converted to fructose by additional aldolase. Due to the proteinaceous nature of the amyloid substrate, the AF7E hydrogel is completely biodegradable by pepsin, as confirmed via atomic force microscopy and circular dichroism spectroscopy analysis. This original enzyme-amyloid hybrid is biocompatible, sustainable, and scalable and may serve as a general template for multienzymatic catalytic platforms.
研究领域:
生物化学
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生物技术
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环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
TALANTA
·
2023
·
IF 6.1
Chaonan Jiao,Ying Zhu,Tongkai Ji,Xingwei Cai,Jing Wang
For yolk-shell structured nanoreactors , multiple active components can be precisely positioned on core and/or shell that can afford more exposed accessible active sites, and the internal voids can guarantee sufficient contact of reactants and catalysts. In this work, a unique yolk–shell structured nanoreactor [email protected] 3 O 4 /CeO 2 @mSiO 2 was fabricated and applied as nanozyme for biosensing. The [email protected] 3 O 4 /CeO 2 @mSiO 2 exhibited superior peroxidase-like activity with a lower Michaelis constant ( K m ) and a higher affinity to H 2 O 2 . The enhanced peroxidase-like activity was attributed to the unique structure and the synergistic effects between the multiple active components. Colorimetric essays were developed based on [email protected] 3 O 4 /CeO 2 @mSiO 2 for the ultra-sensitive sensing of glucose in the range of 3.9 nM–1.03 mM with the limit of detection as low as 3.2 nM. In the detection of glucose-6-phosphate dehydrogenase (G6PD), the cooperation between G6PD and [email protected] 3 O 4 /CeO 2 @mSiO 2 triggered the redox cycling between NAD + and NADH, thereby achieving the amplification of the signal and enhancing the sensitivity of the assay. The assay showed superior performance as compared to other methods with linear response of 5.0 × 10 −3 –15 mU mL −1 and lower detection limit of 3.6 × 10 −3 mU mL −1 . The fabricated novel multi-enzyme catalytical cascade reaction system allowed rapid and sensitive biodetection, demonstrating its potential in biosensors and biomedical applications.
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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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）