离子型磁性COFs负载GOx实现纳米酶与天然酶的级联反应

Ionic Magnetic COFs Loaded with GOx for Cascade Reaction of Nanoenzymes and Natural Enzyme

【目的】一锅反应中将天然酶的高选择性与纳米酶的高稳定性相结合,已成为一种提高生物催化级联多样性/复杂性和多酶系统稳定性的理想解决方案。【方法】设计合成了一种离子型磁性Fe_(3)O_(4)@EB-COFs材料,在静电作用诱导下制备了葡萄糖氧化酶(GOx)-磁性共价有机框架材料(GOx/Fe_(3)O_(4)@EB-COFs)。【结果】Fe_(3)O_(4)@EB-COFs扮演了纳米酶与载体材料的角色,且所得复合材料可用于葡萄糖浓度的比色测定。酸性条件下,GOx/Fe_(3)O_(4)@EB-COFs展现出极好的催化葡萄糖氧化与2,2′-联氮-双-3-乙基苯并噻唑啉-6-磺酸(ABTS)氧化的级联反应。动力学研究表明,反应遵循Lineweaver-Burk方程,说明构建纳米酶与天然酶的级联反应时仍呈现了生物催化的特点。在磁性Fe_(3)O_(4)的加持下,GOx/Fe_(3)O_(4)@EB-COFs表现出良好的可回收性。【结论】构建纳米酶与天然酶的多酶催化系统对于实现仿生催化具有重要意义。

【Purposes】Combining the high selectivity of natural enzymes with the high stability of nanoenzymes in a one-pot reaction has emerged as an ideal solution to improving the diversity/complexity of biocatalytic cascades and the stability of multi-enzyme systems.【Methods】In this paper,we designed and synthesized an ionic magnetic Fe_(3)O_(4)@EB-COFs material to prepare glucose oxidase(GOx)-magnetic covalent organic framework material(GOx/Fe_(3)O_(4)@EB-COFs)through electrostatic interaction induction.【Findings】Fe_(3)O_(4)@EB-COFs played the role of nanoparticle enzyme and carrier material,and the obtained composite could be used for glucose concentration for colorimetric determination.Under acidic conditions,GOx/Fe_(3)O_(4)@EB-COFs exhibited a good cascade of catalytic glucose oxidation and 2,2'-biazo-bis-3-ethylbenzothiazoline-6-sulfonic acid oxidation.The kinetic study showed that the reaction followed the Lineweaver-Burk equation,indicating that the cascade reaction of the constructed nanoenzyme with natural enzyme still exhibited biocatalytic characteristics.GOx/Fe_(3)O_(4)@EB-COFs exhibited good recoverability with the addition of magnetic Fe_(3)O_(4).【Conclusions】Therefore,the construction of a multi-enzyme catalytic system of nanoenzymes and natural enzymes is important for the realization of biomimetic catalysis.