State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, 163 Xianlin Avenue, Nanjing 210023, China.
J Mater Chem B. 2022 Sep 15;10(35):6716-6723. doi: 10.1039/d1tb02325j.
Enzyme mimics are of significant importance due to their facile preparation, low cost and stability to rigorous environments. Molecularly imprinted polymers (MIPs) have been important synthetic mimics of enzymes. However, effective strategies for the rational design of enzyme-mimicking MIPs have still remained limited. Herein, we report a new strategy, termed affinity gathering-enhanced coupling and thermal cycling amplification (AGEC-TCA), for the rational design and engineering of molecularly imprinted mesoporous silica nanoparticles (MSNs) that are capable of ligating short ssDNA fragments. This strategy relied on enhancing the effective collision probability binding substrates into highly favorable orientation by product-imprinted MSNs as well as product release thermal cycling which enabled successive product amplification. Using modified and natural hexadeoxyribonucleotide as templates, the prepared product-imprinted MSNs exhibited a remarkably enhanced reaction speed (by up to 63-fold) as well as excellent sequence specificity towards substrate trideoxyribonucleotides. Thus, this strategy opened up a new avenue to access enzyme mimics molecular imprinting.
由于酶模拟物制备简便、成本低、稳定性强，因此具有重要意义。分子印迹聚合物（MIPs）是酶的重要合成模拟物。然而，用于合理设计酶模拟 MIP 的有效策略仍然有限。在此，我们报告了一种新策略，称为亲和聚集增强偶联和热循环扩增（AGEC-TCA），用于合理设计和工程化能够连接短 ssDNA 片段的分子印迹介孔硅纳米粒子（MSNs）。该策略依赖于通过产物印迹 MSNs 增强有效碰撞概率 将底物结合到有利的取向，以及通过热循环进行产物释放 这使得产物能够连续扩增。使用修饰和天然十六脱氧核苷酸作为模板，制备的产物印迹 MSNs 表现出显著增强的反应速度（高达 63 倍）以及对底物三脱氧核苷酸的优异序列特异性。因此，该策略为获得酶模拟物开辟了一条新途径 分子印迹。
