ACS Applied Materials & Interfaces
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2020
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IF 8.758
Hang Jiang,Liangdong Liu,Yunxing Li,Shouwei Yin,To Ngai
Water-in-oil (w/o) Pickering emulsions have received considerable attention in biphasic enzymatic catalysis for their advantages of good stability, large interfacial area, and ease of product separation. However, enzymes are commonly encapsulated in the interior of aqueous droplets, which inevitably increases the diffusional resistance to catalysis. Alternatively, enzymes are immobilized or trapped into Pickering stabilizers. Often, however, these approaches suffer from leaching and a decrease of enzyme activity during the chemical treatments. We report here a new Pickering interfacial biocatalysis platform with efficient enzyme encapsulation, binary particle composition, and high catalytic performance. Our approach is based on w/o Pickering emulsions stabilized by binary particles consisting of hard silica and soft, pH-responsive microgel particles. We demonstrate that pH-responsive microgels can simultaneously stabilize a w/o Pickering emulsion, encapsulate enzymes, and catalyze reactions at the water/oil interface. In addition, we show that the coordination with rigid silica nanoparticles as additional stabilizers markedly improves the emulsion structure and will provide a new avenue for the preparation of w/o Pickering emulsion and concept of biphasic catalysis.
研究领域:
化学工程
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生物催化
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材料科学
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产品关联
DOI
PubMed
高影响因子
Advanced Materials Technologies
·
2024
·Vol. 9
·期 4
·2301678
·
IF 6.4
Muxue Wang,Han Wang,Jing Cheng
Diabetes mellitus has become a serious public health problem worldwide. Current home-based glucose testing, including fingerstick blood testing and continuous glucose monitoring, suffers from low compliance and potential infection. Non-invasive glucose detection, with the advantages of pain-free, easy-to-operate, and low-cost, is expected to significantly improve the experience of glucose testing at home for diabetic patients. Here, an enzymatic biosensing platform with high sensitivity and high stability is developed based on a conductive nanomesh composed of interconnected metal-organic frameworks (MOF). The as-prepared enzyme-encapsulated MOF nanomesh exhibits uniform morphology, regular structure, superior catalytic performance, and outstanding electrical conductivity. The glucose sensor modified by enzyme-encapsulated MOF nanomesh demonstrates a considerably high sensitivity of 86.86 µA m m −1 cm −2 with a limit of detection of 16.57 µ m , and remains stable for 16 days of usage. Detection of real saliva samples matches well with the commercial salivary glucose assay kit with an accuracy >93%, and a high correlation with blood glucose with Pearson's r > 0.7. Therefore, the presented enzyme-encapsulated MOF nanomesh biosensor holds great potential in salivary glucose testing and provides a novel strategy for noan-invasive glucose detection.
研究领域:
生物传感器技术
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医学诊断
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材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Hao Chao,Zixin Zhou,Wenting He,Meng Li,Xiaoyu Yuan,Ping Su,Jiayi Song,Yi Yang
Although capsule-like materials as host carriers for enzyme encapsulation have been a hot topic in recent years, creating an ideal microenvironment for enhanced enzymatic performance is still a formidable challenge. Herein, we created a template-free method to in situ encapsulate natural enzymes in hollow covalent organic framework (COF) capsules at room temperature. The COF crystallites migrated from the inner core and self-assembled at the outside walls during the inside-out Ostwald ripening process, retaining the enzymes in the cavity. The adjustable hollow structure of the enzyme@COF capsule allowed the basic vibration of the enzyme to maintain a certain degree of freedom, thus significantly enhancing the enzymatic bioactivity. The hollow enzyme@COF capsule has large mesoporous tunnels allowing the efficient transport. In addition, the enzyme encapsulated in the capsule showed superior activity and ultrahigh stability under various extreme conditions that may lead to enzyme inactivation, such as high temperature, organic solvents, chelates, and the denaturing agent. Finally, the prepared hollow GOx@COF capsule was used for electrochemical sensing of glucose in human serum, and the electrochemical sensor exhibited high selectivity and satisfactory test results. This research not only provides a new way for COFs to encapsulate enzymes but also has potential applications in biocatalysis and biosensing, making artificial organelles possible.
研究领域:
生物化学
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材料科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2025
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IF 3.8
Linsong Luo,Xiao Han,Xiaoyan Dong,Qinghong Shi,Yan Sun
The growth of biodiesel and oleochemical industries results in substantial surpluses of glycerol and consistently low prices. To absorb this surplus, we report a polymer-assisted in situ enzymes encapsulation strategy in which glycerol dehydrogenase (GDH) is encapsulated with polyvinylpyrrolidone (PVP) and cysteine (Cys) within ZIF-8 for glycerol conversion. The results showed that the encapsulated GDH/ZIF-8 composites presented stronger substrate affinities and higher catalytic efficiencies than free GDH as well as good stability. Among the free GDH and GDH/ZIF-8 composites, GDH/Cys/PVP@ZIF-8 presented the highest relative activity of 300.7 %. This could be attributed to the structural evolution of the encapsulated GDH and the formation of a more hydrophilic microenvironment around GDH during complexation with PVP. To increase cofactor utilization, a cofactor self-sufficient cascade system was constructed by encapsulating GDH and forming H 2 O NADH oxidase (Nox) with PVP and Cys within ZIF-8 for the conversion of glycerol to 1,3-dihydroxyacetone (DHA). At the optimal GDH:Nox molar ratio (4:1) and a substrate concentration of 100 mM, the DHA yield reached approximately 4.2 mM in GDH-Nox/Cys/PVP@ZIF-8, and the total turnover number of GDH-Nox/Cys/PVP@ZIF-8 reached 2787 at 0.05 µM NAD + , indicating its feasibility for large-scale DHA production. This work has thus provided a promising procedure of co-immobilizing enzymes via Cys/PVP-assisted in situ encapsulation within ZIF-8 for the development of economically viable multienzyme biocatalysts for glycerol conversion.
研究领域:
生物化学
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工业生物技术
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产品关联
DOI
高影响因子
Nano Energy
·
2019
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IF 15.548
Xin Li,Dawei Li,Yanan Zhang,Pengfei Lv,Quan Feng,Qufu Wei
Self-powered biosensor, as a new sensing platform, utilizes biofuel cells as synchronous power source and biosensor system, with the advantages of no external power source , simple instrumentation and easy miniaturization. Meanwhile, inspired by biomimics for the encapsulation of soft tissue within protective exteriors in nature, encapsulation of biological macromolecules by metal organic-frameworks (MOFs) have been proved to be an effective strategy for enhancing the biocatalytic activity in maintaining biological functions. Herein, we successfully encapsulated laccase (LAC) in zeolitic imidazolate framework-8 (ZIF-8) and combined it with bacterial cellulose (BC)/carboxylated multi-walled carbon nanotubes (c-MWCNTs) skeleton to prepare highly flexible BC/c-MWCNTs/ZIF-8@LAC electrode. Subsequently, we ingeniously designed an highly flexible self-powered sensing platform based on biofuel-cell driven by single-enzyme, harvesting bisphenol A (BPA) as a model analyte. The maximum power density (P max ) of single-enzymatic biofuel cell (EBFC) exhibited an excellent linear dynamic range from 0.01 to 0.4 mM with a lower detection limit of 1.95 × 10 −3 mM for BPA concentrations. Therefore, the designed single-EBFC-based self-powered sensor is feasible in BPA detection and has a broad application prospect in the field of water pollutants detection.
研究领域:
生物化学
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材料科学
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环境科学
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DOI
高影响因子
MICROCHIMICA ACTA
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2021
·Vol. 188
·期 10
·1-10
·
IF 5.833
Qiu Peipei,Yuan Ping,Deng Zhichen,Su Zhengquan,Bai Yan,He Jincan
A rapid method for colorimetric monitoring of bacterial viability is described. The colorimetric method was carried out based on glucose oxidase-encapsulated Zn/Co-infinite coordination polymer (Zn/Co-ICP@GOx), which was prepared in aqueous solution free of toxic organic solvents at room temperature. The Zn/Co-ICP@GOx was confirmed to be a robust sphere structure with an average diameter of 147.53 ± 20.40 nm. It integrated the catalytic activity of natural enzyme (GOx) and mimetic peroxidase (Co (П)) all in one, efficiently acting as a biocatalytic cascade platform for glucose catalytic reaction. Exhibiting good multi-enzyme catalytic activity, stability, and selectivity, Zn/Co-ICP@GOx can be used for colorimetric glucose detection. The linear range was 0.01–1.0 mmol/L, and the limit of detection (LOD) was 0.005 mmol/L. As the glucose metabolism is a common expression of bacteria, the remaining glucose can indirectly represent the bacterial viability. Hence, a Zn/Co-ICP@GOx-based colorimetric method was developed for monitoring of bacterial viability. The color was intuitively observed with the naked eye, and the bacterial viability was accurately quantified by measurement of the absorbance at 510 nm. The method was applied to determination of bacterial viability in water and milk samples with recoveries of 99.0–103% and RSD of 0.43–7.5%. The method was rapid (less than 40 min) and applicable to different bacterial species irrespective of Gram-positive and Gram-negative bacteria, providing a universal and promising strategy for real-time monitoring of bacterial viability. Graphical abstract
研究领域:
生物化学
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分析化学
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微生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2023
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IF 6.1
Fu-Zhen Zhou,Li-Hua Xie,Xin-Hao Yu,Xiao-Quan Yang,Shou-Wei Yin
Double emulsions hold great potential for various applications due to their compartmentalized internal structures. However, achieving their long-term physical stability remains a challenging task. Here, we present a simple one-step method for producing stable oil-in-water-in-oil (O/W/O) double emulsions using biocompatible gliadin/ethyl cellulose complex particles as the sole stabilizer. The resulting O/W/O systems serve as effective platforms for encapsulating enzymes and as templates for synthesizing porous microspheres. We investigated the impact of particle concentration and water fraction on the properties of Pickering O/W/O emulsions. Our results demonstrate that the number and volume of inner oil droplets increased proportionally with both the water fraction and particle concentration after a 60-day storage period. Moreover, the catalytic reaction rate of the encapsulated lipase within the double emulsion exhibited a significant acceleration, achieving a substrate conversion of 80.9% within 15 min. Remarkably, the encapsulated enzyme showed excellent recyclability, enabling up to 10 cycles of reuse. Additionally, by utilizing the O/W/O systems as templates, we successfully obtained porous microspheres whose size can be controlled by the outer water droplet. These findings have significant implications for the future design of Pickering complex emulsion-based systems, opening avenues for extensive applications in pharmaceuticals, food, cosmetics, material synthesis, and (bio)catalysis.
研究领域:
食品科学
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材料科学
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生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Man Tiantian,Xu Caixia,Liu Xiao-Yuan,Li Dan,Tsung Chia-Kuang,Pei Hao,Wan Ying,Li Li
Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonstrate that multi-shelled metal-organic frameworks (MOFs) can be used as a hierarchical scaffold to spatially organize enzymes on nanoscale to enhance cascade catalytic efficiency. Encapsulating multi-enzymes with multi-shelled MOFs by epitaxial shell-by-shell overgrowth leads to 5.8~13.5-fold enhancements in catalytic efficiencies compared with free enzymes in solution. Importantly, multi-shelled MOFs can act as a multi-spatial-compartmental nanoreactor that allows physically compartmentalize multiple enzymes in a single MOF nanoparticle for operating incompatible tandem biocatalytic reaction in one pot. Additionally, we use nanoscale Fourier transform infrared (nano-FTIR) spectroscopy to resolve nanoscale heterogeneity of vibrational activity associated to enzymes encapsulated in multi-shelled MOFs. Furthermore, multi-shelled MOFs enable facile control of multi-enzyme positions according to specific tandem reaction routes, in which close positioning of enzyme-1-loaded and enzyme-2-loaded shells along the inner-to-outer shells could effectively facilitate mass transportation to promote efficient tandem biocatalytic reaction. This work is anticipated to shed new light on designing efficient multi-enzyme catalytic cascades to encourage applications in many chemical and pharmaceutical industrial processes.
研究领域:
生物化学
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材料科学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
Nanomaterials
·
2018
·Vol. 8
·期 2
·127
·
IF 3.504
Sen Lin,Shiyong Sun,Ke Wang,Kexuan Shen,Biaobiao Ma,Yuquan Ren,Xiaoyu Fan
The bioinspired design and construction of enzyme@capsule microreactors with specific cell-like functionality has generated tremendous interest in recent years. Inspired by their fascinating complexity, scientists have endeavored to understand the essential aspects of a natural cell and create biomimicking microreactors so as to immobilize enzymes within the hierarchical structure of a microcapsule. In this study, simultaneous encapsulation of alcohol dehydrogenase (ADH) was achieved during the preparation of microcapsules by the Pickering emulsion method using amphiphilic modified TiO2nanoparticles (NPs) as building blocks for assembling the photocatalytic microcapsule membrane. The ADH@TiO2NP microreactors exhibited dual catalytic functions, i.e., spatially confined enzymatic catalysis and the membrane-associated photocatalytic oxidation under visible light. The sustainable cycling of nicotinamide adenine dinucleotide (NAD) coenzyme between NADH and NAD+was realized by enzymatic regeneration of NADH from NAD+reduction, and was provided in a form that enabled further photocatalytic oxidation to NAD+under visible light. This bioinspired ADH@TiO2NP microreactor allowed the linking of a semiconductor mineral-based inorganic photosystem to enzymatic reactions. This is a first step toward the realization of sustainable biological cycling of NAD+/NADH coenzyme in synthetic functional microsystems operating under visible light irradiation.Keywords:enzyme encapsulation;bioinspired microreactors;nicotinamide coenzymes cycling;alcohol dehydrogenase;TiO2nanoparticles
研究领域:
生物化学
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材料科学
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光催化
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DOI
PubMed
高影响因子
ACS Sensors
·
2019
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IF 6.944
Hao-Hua Deng,Hua-Ping Peng,Kai-Yuan Huang,Shao-Bin He,Qiao-Feng Yuan,Zhen Lin,Rui-Ting Chen,Xing-Hua Xia,Wei Chen
In this study, on the basis of the biomineralization capability of urease, a facile, one-step, and green synthetic method has been proposed for the fabrication of gold nanoclusters (AuNCs). The prepared urease-encapsulated AuNCs (U-AuNCs) exhibited strong red fluorescence emission (λem = 630 nm) with a quantum yield as high as 17%. Interestingly, at a low concentration, the U-AuNC solution was found to be a dual-emissive system with the blue emission of the dityrosine (diTyr) residues of urease and the red emission of the embedded AuNCs. Further experiments demonstrated that p-nitrophenol (PNP) can selectively suppress the 410 nm emission of the diTyr residues of U-AuNCs without affecting the red emission of the U-AuNCs. The fluorescence quenching mechanism between U-AuNCs and PNP was systematically studied, and the leading role of the inner filter effect (IFE) was identified. Additionally, based on the sulfatase-catalyzed hydrolysis of p-nitrophenyl sulfate (PNPS) to release PNP, a self-referenced ratiometric detection method for sulfatase, which plays a crucial role in sulfur cycling, degradation of sulfated glycosaminoglycans and glycolipids, and extracellular remodeling of sulfated glycosaminoglycans, was developed by using dual-emissive U-AuNCs as the signal readout, in which the diTyr residues served as the probe and the AuNCs functioned as the internal reference. This IFE-based ratiometric sensing strategy showed a good linear relationship over the range of 0.01–1 U/mL (R2 = 0.997). The detection limit for sulfatase activity was 0.01 U/mL. The developed protocol was successfully used to detect sulfatase activity in human serum samples. The simplicity, rapidity, low cost, high credibility, good reproducibility, and excellent selectivity of the detection platform serve as an inspiration for further applications of fluorescent AuNCs in chemo/biosensing.
研究领域:
生物化学
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医学检测
·
纳米材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2018
·
IF 6.042
Jiqing Yang,Xiaotong Hu,Jia Xu,Xin Liu,Li Yang
A novel capillary electrophoresis-integrated immobilized enzyme reactor (CE-integrated IMER) is developed using single-step in situ acetylcholinesterase (AChE)-mediated alginate hydrogelation and enzyme encapsulation. Alginate hydrogelation with “egg-box” structure is triggered inside a capillary with releasing of Ca2+ by changing the pH of the sol solution, which is accomplished in situ by AChE-catalyzed hydrolysis reaction of acetylthiocholine to produce acetic acid. AChE and any other enzyme initially contained in the sol solution [e.g., xanthine oxidase (XO)] are efficiently encapsulated as the hydrogel network grows, forming CE-integrated IMERs without any additional manipulation process. The proposed method facilitates the analysis of different kinds of enzymes using the same IMER depending on the substrate injected for CE analysis. Approximately 68% of the original enzyme in the sol mixture can be encapsulated, indicating high loading capacity for the CE-integrated IMERs. The IMERs exhibit excellent intraday and interday stability and batch-to-batch reproducibility, and these characteristics imply the reliability of the proposed IMERs for accurate online enzyme assays. Enzymatic activities and inhibition of immobilized AChE and XO are analyzed, and the results are compared with those using free enzymes. The feasibility of the proposed method for potential application in real sample analysis is demonstrated by the successful application of the IMERs in detecting organophosphorus pesticides in apple juice samples using AChE-catalyzed reactions. The proposed method is a simple, efficient, and universal approach for online CE assays with immobilized enzymes, which can be widely applied in bioanalysis.
研究领域:
生物化学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 4
·1-8
·
IF 4.3
Chu Ziyi,Zhang Boyu,Wu Zhenhua,Zhang Jiaxu,Cheng Yiran,Wang Xueying,Shi Jiafu,Jiang Zhongyi
Organic matter-induced mineralization is a green and versatile method for synthesizing hybrid nanostructured materials, where the material properties are mainly influenced by the species of natural biomolecules, linear synthetic polymer, or small molecules, limiting their diversity. Herein, we adopted dendrimer poly(amidoamine) (PAMAM) as the inducer to synthesize organosilica-PAMAM network (OSPN) capsules for mannose isomerase (MIase) encapsulation based on a hard-templating method. The structure of OSPN capsules can be precisely regulated by adjusting the molecular weight and concentration of PAMAM, thereby demonstrating a substantial impact on the kinetic behavior of the MIase@OSPN system. The MIase@OSPN system was used for catalytic production of mannose from D-fructose. A mannose yield of 22.24% was obtained, which is higher than that of MIase in organosilica network capsules and similar to that of the free enzyme. The overall catalytic efficiency ( k cat / K m ) of the MIase@OSPN system for the substrate D-fructose was up to 0.556 s −1 ·mmol −1 ·L. Meanwhile, the MIase@OSPN system showed excellent stability and recyclability, maintaining more than 50% of the yield even after 12 cycles.
研究领域:
材料科学
·
生物化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）