Hao Li, Bizhu Sun, Meiai Huang, Yipeng Liu, Qian Zhang, Zhuolin Luo, Quan Zeng, Wenjing Zhu, Xuan Li, Juan Chen, Xin Yuan, Panliang Zhang, Kewen Tang
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引用次数: 0
摘要
开发有效的固定化支架以提高酶活性和可回收性是一个非常理想的目标。单晶有序大微孔ZIF-8 (SOM-ZIF-8)已成为一种高效的酶固定化基质,但其固有的疏水性限制了其进一步发展。在此,我们通过使用聚乙二醇(PEG) (LP@SOM-ZIF-8-PEG)对somf - zif -8的内表面特性进行功能化,定制了cepacia假单胞菌脂肪酶(LP)在SOM-ZIF-8修饰通道中的固定化,并实现了活性和(热、溶剂和循环)稳定性的显著提高。PEG掺入到SOM-ZIF-8中调节其内表面电荷和疏水性,从而增强酶的负载,促进酶的构象调整,并实现LP在SOM-ZIF-8-PEG中的均匀分散。LP@SOM-ZIF-8-PEG不仅在酶的负荷和活性上明显高于LP@SOM-ZIF-8,而且酶的活性也比LP@ZIF-8高了三倍。它能在60 min内完全溶解1-苯乙醇外消旋物,转化率接近50% %,对映选择性为99.8 %。在9个重用周期之后,LP@SOM-ZIF-8-PEG仍然保持其初始活动的95% %。LP@SOM-ZIF-8-PEG优异的催化性能和稳定性,以及PEG修饰策略对其他酶的通用性,使这项工作在工业应用中具有广阔的前景。
Decorating channel walls in ordered macroporous ZIF-8 with hydrophilic PEG to immobilize lipase for efficient chiral resolution.
The development of efficient immobilization support for the enhancement of enzyme activity and recyclability is a highly desirable objective. Single-crystalline ordered macro-microporous ZIF-8 (SOM-ZIF-8), has emerged as a highly effective matrix for enzyme immobilization, however, the inherent hydrophobic nature limits its further advancement. Herein, we have customized the immobilization of the Pseudomonas cepacia lipase (LP) in the modification-channels of SOM-ZIF-8 by functionalizing the inner surface-properties with polyethylene glycol (PEG) (LP@SOM-ZIF-8-PEG), and significant enhancement of the activity and (thermal, solvent and cyclic) stability can be realized. The incorporation of PEG into SOM-ZIF-8 regulates its inner surface charge and hydrophobic properties, thereby enhancing enzyme loading, facilitating enzyme conformational adjustments, and achieving a uniform dispersion of LP in SOM-ZIF-8-PEG. LP@SOM-ZIF-8-PEG not only demonstrates a pronounced elevation in enzyme loading and activity over LP@SOM-ZIF-8 but also shows an enzyme activity that is impressively three times greater than LP@ZIF-8. It can completely resolve the 1-phenylethanol racemate in 60 min, with a conversion close to 50 % and an enantioselectivity of 99.8 %. After nine cycles of reuse, the LP@SOM-ZIF-8-PEG still holds onto 95 % of its initial activity. The excellent catalytic performance and stability of LP@SOM-ZIF-8-PEG, along with the universality of the PEG modification strategy for other enzymes, make this work promising in industrial applications.
期刊介绍:
The International Journal of Biological Macromolecules is a well-established international journal dedicated to research on the chemical and biological aspects of natural macromolecules. Focusing on proteins, macromolecular carbohydrates, glycoproteins, proteoglycans, lignins, biological poly-acids, and nucleic acids, the journal presents the latest findings in molecular structure, properties, biological activities, interactions, modifications, and functional properties. Papers must offer new and novel insights, encompassing related model systems, structural conformational studies, theoretical developments, and analytical techniques. Each paper is required to primarily focus on at least one named biological macromolecule, reflected in the title, abstract, and text.