Ali Tajwar Muhammad, Liu Yutong, Qi Li
Beijing National Laboratory of Molecular Sciences, Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, No. 2 Zhongguancun, Beiyijie, Beijing, 100190, P. R. China.
School of Chemical Sciences, University of Chinese Academy of Sciences, 19A Yuquanlu, Beijing, 100049, P. R. China.
Chem Asian J. 2025 Jan 2;20(1):e202400990. doi: 10.1002/asia.202400990. Epub 2024 Nov 14.
Metal-organic frameworks (MOFs) are considered as an ideal enzyme support because of their porous structural superiority. However, MOFs@enzyme composites have usually compromised their hydrolysis efficiency due to the narrow space inducing unfavourable enzyme conformations. Herein, a thermo-responsive poly(N,N-dimethylacrylamide) (PD) was fixed onto the surface of UiO-66-NH (UiO) through a post-synthetic modification protocol. Using poly(2-vinyl-4,4 dimethylazlactone) (V) as a linker, PVD-UiO@cellulase composites were fabricated after cellulase was immobilized onto the UiO surface through covalent bonding. The composites conferred favorable cellulase conformations, boosting hydrolysis efficiency and stability, which relied on the soft PVD shell and confinement effect yielded by the curled PVD chains at high temperatures. Compared with free cellulase, the proposed composites exhibited a 33.1-fold enhancement of the K values at 50 °C. The PVD-UiO@cellulase composites were applied to the hydrolysis of cellulose in the stalks and leaves of Epipremnum aureum. The results highlight the potential of smart PVD-UiO@cellulase composites in the hydrolysis of cellulose, affording a valuable platform for the preparation of unique MOFs@enzyme composites and their industrial applications.
金属有机框架材料（MOFs）因其多孔结构优势而被视为理想的酶载体。然而，MOFs@酶复合材料通常会因其狭窄空间导致酶构象不利而降低其水解效率。在此，通过后合成修饰方案将热响应性聚（N，N-二甲基丙烯酰胺）（PD）固定在UiO-66-NH（UiO）表面。以聚（2-乙烯基-4,4-二甲基氮杂环丁烷酮）（V）作为连接体，在通过共价键将纤维素酶固定在UiO表面后制备了PVD-UiO@纤维素酶复合材料。该复合材料赋予纤维素酶良好的构象，提高了水解效率和稳定性，这依赖于柔软的PVD壳层以及高温下卷曲的PVD链产生的限域效应。与游离纤维素酶相比，所制备的复合材料在50°C时的K值提高了33.1倍。PVD-UiO@纤维素酶复合材料被应用于绿萝茎和叶中纤维素的水解。结果突出了智能PVD-UiO@纤维素酶复合材料在纤维素水解方面的潜力，为制备独特的MOFs@酶复合材料及其工业应用提供了一个有价值的平台。
