Confinement-Induced Biocatalytic Activity Enhancement of Light- and Thermoresponsive Polymer@Enzyme@MOF Composites,ACS Applied Materials & Interfaces

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Confinement-Induced Biocatalytic Activity Enhancement of Light- and Thermoresponsive Polymer@Enzyme@MOF Composites
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-07-08 , DOI: 10.1021/acsami.4c05742
Rubina Jabeen _{1,

2} , Muhammad Ali Tajwar _{1,

2} , Changyan Cao _{2,

3} , Yutong Liu _{1,

4} , Shidi Zhang _{1,

5} , Nasir Ali _{1,

2} , Li Qi _{1,

2}

Affiliation

Metal–organic frameworks (MOFs) are favorable hosting materials for fixing enzymes to construct enzyme@MOF composites and to expand the applications of biocatalysts. However, the rigid structure of MOFs without tunable hollow voids and a confinement effect often limits their catalytic activities. Taking advantage of the smart soft polymers to overcome the limitation, herein, a protection protocol to encapsulate the enzyme in zeolitic imidazolate framework-8 (ZIF-8) was developed using a glutathione-sensitive liposome (L) as a soft template. Glucose oxidase (GOx) and horseradish peroxidase (HRP) were first anchored on a light- and thermoresponsive porous poly(styrene-maleic anhydride-N,N-dimethylaminoethyl methacrylate-spiropyran) membrane (PSMDSP) to produce PSMDSP@GOx-HRP, which could provide a confinement effect by switching the UV irradiation or varying the temperature. Afterward, embedding PSMDSP@GOx-HRP in L and encapsulating PSMDSP@GOx-HRP@L into hollow ZIF-8 (HZIF-8) to form PSMDSP@GOx-HRP@HZIF-8 composites were performed, which proceeded during the crystallization of the framework following the removal of L by adding glutathione. Impressively, the biocatalytic activity of the composites was 4.45-fold higher than that of the free enzyme under UV irradiation at 47 °C, which could benefit from the confinement effect of PSMDSP and the conformational freedom of the enzyme in HZIF-8. The proposed composites contributed to the protection of the enzyme against harsh conditions and exhibited superior stability. Furthermore, a colorimetric assay based on the composites for the detection of serum glucose was established with a linearity range of 0.05–5.0 mM, and the calculated LOD value was 0.001 mM in a cascade reaction system. This work provides a universal design idea and a versatile technique to immobilize enzymes on soft polymer membranes that can be encapsulated in porous rigid MOF-hosts. It also holds potential for the development of smart polymer@enzyme@HMOFs biocatalysts with a tunable confinement effect and high catalytic performance.

中文翻译：

光响应和热响应聚合物@Enzyme@MOF复合材料的约束诱导生物催化活性增强

金属有机框架（MOF）是固定酶以构建酶@MOF复合材料并扩大生物催化剂应用的有利宿主材料。然而，MOFs 的刚性结构没有可调的中空空隙和限制效应，通常限制了它们的催化活性。利用智能软聚合物来克服这一限制，本文使用谷胱甘肽敏感脂质体（L）作为软模板，开发了一种将酶封装在沸石咪唑酯骨架-8（ZIF-8）中的保护方案。首先将葡萄糖氧化酶（GOx）和辣根过氧化物酶（HRP）锚定在光和热响应性多孔聚（苯乙烯-马来酸酐-N , N-二甲基氨基乙基甲基丙烯酸酯-螺吡喃）膜（PSMDSP）上以产生PSMDSP@GOx-HRP，可以通过切换紫外线照射或改变温度来提供限制效果。然后，将PSMDSP@GOx-HRP@L嵌入到L中并将PSMDSP@GOx-HRP@L封装到空心ZIF-8（HZIF-8）中形成PSMDSP@GOx-HRP@HZIF-8复合材料，该复合材料在L的结晶过程中进行。通过添加谷胱甘肽去除 L 后的框架。令人印象深刻的是，在 47°C 的紫外线照射下，复合材料的生物催化活性比游离酶高 4.45 倍，这可能得益于 PSMDSP 的限制效应和 HZIF-8 中酶的构象自由度。所提出的复合材料有助于保护酶免受恶劣条件的影响，并表现出优异的稳定性。此外，建立了基于复合物的比色法检测血糖，线性范围为0.05-5.0 mM，在级联反应体系中计算的LOD值为0.001 mM。这项工作提供了一种通用的设计理念和一种通用技术，可以将酶固定在可封装在多孔刚性 MOF 主体中的软聚合物膜上。它还具有开发具有可调限制效应和高催化性能的智能聚合物@酶@HMOFs生物催化剂的潜力。

更新日期：2024-07-08

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