Self-Assembled DNA/Peptide-Based Nanoparticle Exhibiting Synergistic Enzymatic Activity
Self-Assembled DNA/Peptide-Based Nanoparticle Exhibiting Synergistic Enzymatic Activity
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DOI：
10.1021/acsnano.7b03195
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发表时间：
2017-07-01
期刊：
影响因子：
17.1
通讯作者：
Ding, Baoquan
中科院分区：
文献类型：
--
作者：
Liu, Qing;Wang, Hui;Ding, Baoquan
在人工系统中设计酶模拟活性位点是实现与天然酶相媲美的催化效率的关键，并且可以为理解酶的自然进化提供有价值的见解。在这里，我们报告了一个催化含氯化血红素的纳米粒子的设计与自组装的富含鸟嘌呤的核酸/富含组氨酸的肽成分，模仿血红素蛋白的活性位点和过氧化活性。折叠的核酸和肽之间的化学互补性使得活性位点中的必需元件的空间排列和氯化血红素的有效活化成为可能。结果表明，核酸和肽对催化剂的催化性能有显著的协同效应。过氧化物的周转数达到天然过氧化物酶的数量级，催化效率与肌红蛋白相当。这些结果在精确设计的超分子酶模拟物，特别是那些与分级活性位点的影响。我们在这里描述的组件也可能类似于现代酶从原始细胞的催化RNA进化的中间体。
Designing enzyme-mimicking active sites in artificial systems is key to achieving catalytic efficiencies rivaling those of natural enzymes and can provide valuable insight in the understanding of the natural evolution of enzymes. Here, we report the design of a catalytic hemin-containing nanoparticle with self-assembled guanine-rich nucleic acid/histidine-rich peptide components that mimics the active site and peroxidative activity of hemoproteins. The chemical complementarities between the folded nucleic acid and peptide enable the spatial arrangement of essential elements in the active site and effective activation of hemin. As a result, remarkable synergistic effects of nucleic acid and peptide on the catalytic performances were observed. The turnover number of peroxide reached the order of that of natural peroxidase, and the catalytic efficiency is comparable to that of myoglobin. These results have implications in the precise design of supramolecular enzyme mimetics, particularly those with hierarchical active sites. The assemblies we describe here may also resemble an intermediate in the evolution of contemporary enzymes from the catalytic RNA of primitive cells.