Size-Tunable Metal-Organic Framework-Coated Magnetic Nanoparticles for Enzyme Encapsulation and Large-Substrate Biocatalysis
| Autor: | Zhongyu Yang, Yanxiong Pan, Lina Alhalhooly, Qiaobin Li, Bingcan Chen, Yue Li, Yongki Choi, Hui Li |
|---|---|
| Rok vydání: | 2020 |
| Předmět: |
Materials science
Immobilized enzyme Surface Properties Phthalic Acids Nanoparticle 02 engineering and technology 010402 general chemistry 01 natural sciences Article General Materials Science Particle Size Magnetite Nanoparticles health care economics and organizations Metal-Organic Frameworks chemistry.chemical_classification fungi Substrate (chemistry) 021001 nanoscience & nanotechnology Enzymes Immobilized Enzyme encapsulation 0104 chemical sciences Enzyme Chemical engineering chemistry Biocatalysis Magnetic nanoparticles Metal-organic framework Calcium Muramidase 0210 nano-technology |
| Zdroj: | ACS Appl Mater Interfaces |
| ISSN: | 1944-8252 |
| Popis: | Immobilizing enzymes on nanoparticles (NPs) enhances the cost-efficiency of biocatalysis; however, when the substrates are large, it becomes difficult to separate the enzyme@NP from the products while avoiding leaching or damage of enzymes in the reaction medium. Metal-Organic Framework (MOF) coated magnetic nanoparticles (MNPs) offers efficient magnetic separation and enhanced enzyme protection; however, the involved enzymes/substrates have to be smaller than MOF apertures. A potential solution to these challenges is co-precipitating metal/ligand with enzymes on MNP surface, which can partially bury (protect) the enzyme below the composite surface while exposing the rest of the enzyme to the reaction medium for catalysis of larger substrates. Here, to prove this concept, we show that using Ca(2+) and terephthalic acid (BDC), large-substrate enzymes can be encapsulated in the CaBDC-MOF layers coated on MNPs via enzyme-friendly, aqueous phase one-pot synthesis. Interestingly, we found that using MNP as the nuclei of crystallization, the composite size can be tuned so that nanoscale composites were formed under low Ca(2+)/BDC concentrations while microscale composites under high Ca(2+)/BDC concentrations. While the microscale composites showed significantly enhanced reusability against a non-structured large substrate, the nanoscale composites displayed enhanced catalytic efficiency against a rigid, crystalline-like large substrate, starch, likely due to the improved diffusivity of the nanoscale composites. To our best knowledge, this is the first report on aqueous phase one-pot synthesis of size-tunable enzyme@MOF/MNP composites for large substrate biocatalysis. Our platform can be applied to immobilize other large substrate enzymes with enhanced reusability and tunable sizes. |
| Databáze: | OpenAIRE |
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