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Harnessing Self-Repairing and Crystallization Processes for Effective Enzyme Encapsulation in Covalent Organic
Yufeng Zhang1, Chunyan Xing1, Zhenjie Mu1
1Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Key Laboratory of Cluster Science, Ministry of Education, Advanced Technology Research Institute (Jinan), Frontiers Science Center for High Energy Material, Advanced Research Institute of Multidisciplinary Science, School of Chemistry and Chemical Engineering, School of Medical Technology, Beijing Institute of Technology, Beijing 100081, P. R. China.
Abstract:
Immobilization of fragile enzymes in crystalline porous materials offers new opportunities to expand the applications of biocatalysts. However, limited by the pore size and/or harsh synthesis conditions of the porous hosts, enzymes often suffer from dimension limitation or denaturation during the immobilization process. Taking advantage of the dynamic covalent chemistry feature of covalent organic frameworks (COFs), herein, we report a preprotection strategy to encapsulate enzymes in COFs during the self-repairing and crystallization process. Enzymes were first loaded in the low-crystalline polymer networks with mesopores formed at the initial growth stage, which could offer effective protection for enzymes from the harsh reaction conditions, and subsequently the encapsulation proceeded during the self-repairing and crystallization of the disordered polymer into the crystalline framework. Impressively, the biological activity of the enzymes can be well-maintained after encapsulation, and the obtained enzyme@COFs also show superior stability. Furthermore, the preprotection strategy circumvents the size limitation for enzymes, and its versatility was verified by enzymes with different sizes and surface charges, as well as a two-enzyme cascade system. This study offers a universal design idea to encapsulate enzymes in robust porous supports and holds promise for developing high-performance immobilized biocatalysts.
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