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Modulating the biofunctionality of enzyme-MOF nanobiocatalyst through structure-switching aptamer for continuous degradation of BPA
Colloids and Surfaces B: Biointerfaces ( IF 5.8 ) Pub Date : 2021-09-08 , DOI: 10.1016/j.colsurfb.2021.112099
Yuanyuan Liu 1 , Yihan Liu 1 , Linyan Gu 1 , Juan Han 2 , Wenjing Zhi 1 , Yun Wang 1 , Lei Wang 1
Affiliation  

Encapsulating enzyme within MOF (enzyme-MOF) gives rise to new opportunity to improve the fragility of enzyme, but practical application of enzyme-MOF composite is far from being realized. The development of a novel enzyme-MOF composite system should simultaneously guarantee the enhanced activity and controllably complete recycling, and only in this way can we efficiently and economically utilize the enzyme-MOF composite. Herein, we addressed all these fundamental limitations of current enzyme-MOF composite by establishing aptamer-functionalized enzyme-MOF composite (HRP-ZIF-8@P1). HRP-ZIF-8@P1 relied on automatic structure switch of aptamer-target binding and aptamer-cDNA (complementary DNA) hybridization, achieving effectiveness in self-enriching substrate around HRP-ZIF-8@P1 to boost enzymatic activity first, subsequently hybridizing spontaneously with magnetically controllable cDNA sequence (Fe3O4@P3) to completely recover the HRP-ZIF-8@P1, where preferentially capturing substrate could further induce the release of the hybridized HRP-ZIF-8@P1 for automatically starting the cyclic enzyme catalysis. A 5.6-fold enhancement in the catalytic efficiency for BPA degradation was endowed, and 94.7% catalytic activity was retained for 8 consecutive degradations of BPA, both of which were even more significant than HRP-ZIF-8. Additionally, remarkable stability of HRP-ZIF-8@P1 was afforded by dual-layer protection of ZIF-8 and P1 in denaturing conditions. Taking the possibility of discovering an aptamer for any target into account, the aptamer-functionalized enzyme-MOF composites provide a generic and simple guide for simultaneously boosting enzymatic activity and controllably full recycling the enzyme-MOF systems, accelerating their commercial utilizations.



中文翻译:

通过结构转换适体调节酶-MOF纳米生物催化剂的生物功能性以连续降解BPA

将酶包裹在 MOF(酶-MOF)中为提高酶的脆性提供了新的机会,但酶-MOF 复合材料的实际应用远未实现。新型酶-MOF复合体系的开发应同时保证活性的增强和可控的完全回收,只有这样才能高效、经济地利用酶-MOF复合材料。在此,我们通过建立适体功能化酶-MOF 复合材料(HRP-ZIF-8@P1)解决了当前酶-MOF 复合材料的所有这些基本局限性。HRP-ZIF-8@P1依靠适体-靶标结合和适体-cDNA(互补DNA)杂交的自动结构转换,首先在HRP-ZIF-8@P1周围实现自富集底物以提高酶活性,3 O 4@P3) 以完全恢复 HRP-ZIF-8@P1,其中优先捕获底物可以进一步诱导杂交 HRP-ZIF-8@P1 的释放,以自动启动循环酶催化。BPA降解催化效率提高了5.6倍,连续8次降解BPA仍保持94.7%的催化活性,均比HRP-ZIF-8更显着。此外,ZIF-8 和 P1 在变性条件下的双层保护提供了 HRP-ZIF-8@P1 的显着稳定性。考虑到为任何目标发现适体的可能性,适体功能化的酶-MOF 复合材料为同时提高酶活性和可控地完全回收酶-MOF 系统提供了通用和简单的指导,

更新日期:2021-09-15
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