TY - JOUR

T1 - Covalent organic networks for in situ entrapment of enzymes with superior robustness and durability

AU - Wu, Zhenhua

AU - Shan, Huiting

AU - Jiao, Yushuai

AU - Huang, Shouying

AU - Wang, Xiaodong

AU - Liang, Kang

AU - Shi, Jiafu

N1 - This is the author’s version of a work that was accepted for publication in Chemical Engineering Journal. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Chemical Engineering Journal, 450, 4, 2022 DOI: 10.1016/j.cej.2022.138446

PY - 2022/12/15

Y1 - 2022/12/15

N2 - Enzyme-based nanobiohybrids (EnNBHs) are an emerging biocatalyst family that can manufacture industrial products such as fuels and chemicals in a green and low- carbon manner. Designing high-performance EnNBHs could confer enzymes with superior robustness and durability, while current strategies confront grand challenges. Indeed, the reticular chemistry materials, especially metal-organic frameworks (MOFs), covalent organic frameworks (COFs), hydrogen-bond organic frameworks (HOFs), are several good candidates for constructing EnNBHs. While, MOFs and HOFs are constructed by coordination bond and hydrogen bond, respectively, which may be destroyed by acid or organic solvents, thus causing structural degradation and loss of protection to enzymes. The use of acetic acid (6 mol L-1) and organic solvents is conventional conditions for the synthesis of COFs, which may be inapplicable for de novo constructing EnNBHs. Herein, a facile and versatile in situ entrapment strategy is developed to entrap a series of enzymes in crystalline imine-based covalent organic networks (CONs) under mild conditions. Notably, the growth rate of CONs induced by glucose oxidase (GOx) is increased by 2 folds than that of CONs in the absence of GOx. Moreover, the crystalline CONs could create confinement environment and safeguard the hosted enzymes from being denatured under unfavorable conditions. Given moderate crystallinity of CONs, short-range ordered micro/meso-porous structures are generated. Compared with GOx@ZIFs, the larger transport channels for reactants/products in GOx@CONs result in 1.73-fold enhancement in the catalytic efficiency. The crystalline CONs could also serve as a cell-mimic nanoreactor for multienzyme catalysis, demonstrating the potential applications in biomanufacturing, bioimaging, biosensing and so on.

AB - Enzyme-based nanobiohybrids (EnNBHs) are an emerging biocatalyst family that can manufacture industrial products such as fuels and chemicals in a green and low- carbon manner. Designing high-performance EnNBHs could confer enzymes with superior robustness and durability, while current strategies confront grand challenges. Indeed, the reticular chemistry materials, especially metal-organic frameworks (MOFs), covalent organic frameworks (COFs), hydrogen-bond organic frameworks (HOFs), are several good candidates for constructing EnNBHs. While, MOFs and HOFs are constructed by coordination bond and hydrogen bond, respectively, which may be destroyed by acid or organic solvents, thus causing structural degradation and loss of protection to enzymes. The use of acetic acid (6 mol L-1) and organic solvents is conventional conditions for the synthesis of COFs, which may be inapplicable for de novo constructing EnNBHs. Herein, a facile and versatile in situ entrapment strategy is developed to entrap a series of enzymes in crystalline imine-based covalent organic networks (CONs) under mild conditions. Notably, the growth rate of CONs induced by glucose oxidase (GOx) is increased by 2 folds than that of CONs in the absence of GOx. Moreover, the crystalline CONs could create confinement environment and safeguard the hosted enzymes from being denatured under unfavorable conditions. Given moderate crystallinity of CONs, short-range ordered micro/meso-porous structures are generated. Compared with GOx@ZIFs, the larger transport channels for reactants/products in GOx@CONs result in 1.73-fold enhancement in the catalytic efficiency. The crystalline CONs could also serve as a cell-mimic nanoreactor for multienzyme catalysis, demonstrating the potential applications in biomanufacturing, bioimaging, biosensing and so on.

KW - Enzyme-based nanobiohybrids

KW - Enzymes

KW - Entrapment

KW - Covalent organic networks

KW - Enzyme catalysis

U2 - 10.1016/j.cej.2022.138446

DO - 10.1016/j.cej.2022.138446

M3 - Journal article

VL - 450

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

SN - 1385-8947

IS - 4

M1 - 138446

ER -