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Molecularly imprinted peptide-based enzyme mimics with enhanced activity and specificity.
Soft Matter ( IF 2.9 ) Pub Date : 2020-07-02 , DOI: 10.1039/d0sm00635a Jingyi Li 1 , Mingjie Zhu 1 , Mengfan Wang 2 , Wei Qi 3 , Rongxin Su 3 , Zhimin He 1
Soft Matter ( IF 2.9 ) Pub Date : 2020-07-02 , DOI: 10.1039/d0sm00635a Jingyi Li 1 , Mingjie Zhu 1 , Mengfan Wang 2 , Wei Qi 3 , Rongxin Su 3 , Zhimin He 1
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We herein report the construction of peroxidase (POD)-mimicking catalysts based on the strategy of peptide assembly and molecular imprinting. Upon co-assembly of Fmoc-FFH and Hemin, we firstly fabricated CA-H/Hemin which displayed POD-like catalytic activity and showed a 21-fold rate acceleration in the oxidation of 2,2′-azinobis-(3-ethylbenzthiazoline-6-sulphonate) (ABTS) compared to the uncatalyzed reaction. Then, upon combining CA-H/Hemin with the ABTS-imprinted polymer, the obtained imprinted catalyst (MIP-H/Hemin) showed 52-fold acceleration due to the enhanced re-binding toward ABTS. Moreover, by introducing cationic monomers, a 137-fold rate enhancement was further achieved for the positively charged imprinted catalyst (MIP+-H/Hemin), from the synergistic effect of molecular imprinting and electrostatic attraction. Remarkably, by comparing the catalytic activity of these POD mimics towards ABTS and 3,3′,5,5′-tetramethylbenzidine (TMB), we also highlighted the substrate specificity of MIP-H/Hemin and MIP+-H/Hemin toward ABTS. This study provides a promising approach to improve the catalytic activity and specificity of peptide-based enzyme mimics.
中文翻译：
分子印迹的基于肽的酶模拟物具有增强的活性和特异性。
我们在此报告了基于肽组装和分子印迹策略的过氧化物酶（POD）模拟催化剂的构建。在Fmoc-FFH和Hemin共组装后，我们首先制备了CA-H / Hemin，它显示出类似于POD的催化活性，并且在2,2'-叠氮基双-（3-乙基苯并噻唑啉-与未催化反应相比，6-磺酸盐（ABTS）。然后，当将CA-H / Hemin与ABTS印迹聚合物结合时，由于增强的对ABTS的重新结合，所得的印迹催化剂（MIP-H / Hemin）显示出52倍的加速度。此外，通过引入阳离子单体，带正电荷的印迹催化剂（MIP +-H / Hemin），来自分子印迹和静电吸引的协同效应。值得注意的是，通过比较这些POD模拟物对ABTS和3,3'，5,5'-四甲基联苯胺（TMB）的催化活性，我们还强调了MIP-H / Hemin和MIP + -H / Hemin对ABTS的底物特异性。这项研究提供了一种有前途的方法来提高基于肽的酶模拟物的催化活性和特异性。
更新日期：2020-08-05
中文翻译：
分子印迹的基于肽的酶模拟物具有增强的活性和特异性。
我们在此报告了基于肽组装和分子印迹策略的过氧化物酶（POD）模拟催化剂的构建。在Fmoc-FFH和Hemin共组装后，我们首先制备了CA-H / Hemin，它显示出类似于POD的催化活性，并且在2,2'-叠氮基双-（3-乙基苯并噻唑啉-与未催化反应相比，6-磺酸盐（ABTS）。然后，当将CA-H / Hemin与ABTS印迹聚合物结合时，由于增强的对ABTS的重新结合，所得的印迹催化剂（MIP-H / Hemin）显示出52倍的加速度。此外，通过引入阳离子单体，带正电荷的印迹催化剂（MIP +-H / Hemin），来自分子印迹和静电吸引的协同效应。值得注意的是，通过比较这些POD模拟物对ABTS和3,3'，5,5'-四甲基联苯胺（TMB）的催化活性，我们还强调了MIP-H / Hemin和MIP + -H / Hemin对ABTS的底物特异性。这项研究提供了一种有前途的方法来提高基于肽的酶模拟物的催化活性和特异性。
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