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超稳定的分级多孔核苷酸基金属有机框架及其在酶固定化和催化中的应用。

Ultrastable hierarchically porous nucleotide-based MOFs and their use for enzyme immobilization and catalysis.

作者信息

Chen Wenyi, Lin Shuping, Zheng Jiawei, Ling Jie, Zhong Nanjing

机构信息

School of Food Science, Guangdong Pharmaceutical University, Zhongshan 528458, China.

School of Food Science, Guangdong Pharmaceutical University, Zhongshan 528458, China.

出版信息

Colloids Surf B Biointerfaces. 2025 Jan;245:114294. doi: 10.1016/j.colsurfb.2024.114294. Epub 2024 Oct 4.

Abstract

Immobilization of free enzymes facilitates their recovery and reuse, while also enhances their enzymatic characteristics. Hierarchically porous metal-organic frameworks (HP-MOFs) are promising candidates for enzyme immobilization. However, fabrication of HP-MOFs with more kinds of components as ligands is still a challenge. Herein, ultrastable crystalline MOFs with micro-, meso- and macroporous structure were constructed using guanosine 5'-monophosphate (GMP) as organic ligand through templated emulsification method. HP-MOFs crystals with the near rhomb-like, rod-like and slab-like morphology were interestingly obtained from Zn, Cu and Cd respectively. The HP-MOFs immobilized enzymes exhibited an enhanced enzymatic activity and stability. In addition, the immobilized CALB (Candida antarctica lipase B) showed great glycerolysis and esterification performances for glycerides preparation, with diacylglycerols (DAG) content over 60 wt% and triacylglycerols (TAG) content over 90 wt% obtained respectively from glycerolysis and esterification. Moreover, it retained 82.32 % of its initial glycerolysis activity after six cycles of reuse in glycerolysis. The present study will provide clues and show new horizons to explore new organic ligands for HP-MOFs fabrication, as well as to expand the applications of HP-MOFs and their supported enzymes.

摘要

固定游离酶有助于其回收和再利用,同时还能增强其酶学特性。分级多孔金属有机框架材料(HP-MOFs)是酶固定化的有前途的候选材料。然而,制备具有更多种类配体成分的HP-MOFs仍然是一个挑战。在此,通过模板乳化法使用5'-单磷酸鸟苷(GMP)作为有机配体构建了具有微孔、介孔和大孔结构的超稳定晶体MOFs。有趣的是,分别从锌、铜和镉中获得了具有近似菱形、棒状和平板状形态的HP-MOFs晶体。固定化酶的HP-MOFs表现出增强的酶活性和稳定性。此外,固定化的南极假丝酵母脂肪酶B(CALB)在甘油酯制备中表现出优异的甘油解和酯化性能,分别从甘油解和酯化中获得的甘油二酯(DAG)含量超过60 wt%和甘油三酯(TAG)含量超过90 wt%。此外,在甘油解中重复使用六个循环后,它保留了其初始甘油解活性的82.32%。本研究将为探索用于HP-MOFs制备的新有机配体提供线索,并展示新的前景,同时也为扩大HP-MOFs及其负载酶的应用提供帮助。

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