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Research Article

Preparation of hollow spherical covalent organic frameworks via Oswald ripening under ambient conditions for immobilizing enzymes with improved catalytic performance

Hao Zhao1, Guanhua Liu1( ), Yunting Liu1, Liya Zhou1, Li Ma1, Ying He1, Xiaobing Zheng1, Jing Gao1, Yanjun Jiang1,2( )
School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
State Key Laboratory of Biocatalysis and Enzyme Engineering, School of Life Sciences, Hubei University, Wuhan 430062, China
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Graphical Abstract

A hollow spherical covalent organic framework with high specific surface area, high crystallinity, high chemical/mechanical/thermal stability, and uniform particle size is prepared by Oswald ripening mechanism at ambient temperature and pressure. The unique hollow structure, clear through holes, and hydrophobic pore environment improve the catalytic performance of the immobilized lipase in the kinetic resolution of secondary alcohols.

Abstract

The hollow spherical covalent organic frameworks (COFs) have a wide application prospect thanks to their special structures. However, the controllable synthesis of uniform and stable hollow COFs is still a challenge. We herein propose a self-templated method for the preparation of hollow COFs through the Ostwald ripening mechanism under ambient conditions, which avoids most disadvantages of the commonly used hard-templating and soft-templating methods. A detailed time-dependent study reveals that the COFs are transformed from initial spheres to hollow spheres because of the inside-out Ostwald ripening process. The obtained hollow spherical COFs have high crystallinity, specific surface area (2,036 m2·g−1), stability, and single-batch yield. Thanks to unique hollow structure, clear through holes, and hydrophobic pore environment of the hollow spherical COFs, the obtained immobilized lipase (BCL@H-COF-OMe) exhibits higher thermostability, polar organic solvent tolerance, and reusability. The BCL@H-COF-OMe also shows higher catalytic performance than the lipase immobilized on non-hollow COF and free lipase in the kinetic resolution of secondary alcohols. This study provides a simple approach for the preparation of hollow spherical COFs, and will promote the valuable research of COFs in the field of biocatalysis.

Keywords

hollow spherical structurecovalent organic frameworkOswald ripening mechanismlipasekinetic resolution

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Nano Research
Volume 16 Issue 1,
January 2023
Pages 281-289
DOI: 10.1007/s12274-022-4769-5
Cite this article:
Zhao H, Liu G, Liu Y, et al. Preparation of hollow spherical covalent organic frameworks via Oswald ripening under ambient conditions for immobilizing enzymes with improved catalytic performance. Nano Research, 2023, 16(1): 281-289. https://doi.org/10.1007/s12274-022-4769-5
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Received: 31 May 2022
Revised: 09 July 2022
Accepted: 13 July 2022
Published: 27 August 2022
© Tsinghua University Press 2022
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