Flexible Assembly of an Enzyme Cascade on a DNA Triangle Prism Nanostructure for the Controlled Biomimetic Generation of Nitric Oxide
Flexible Assembly of an Enzyme Cascade on a DNA Triangle Prism Nanostructure for the Controlled Biomimetic Generation of Nitric Oxide
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DNA 三角棱柱纳米结构上酶级联的灵活组装，用于受控仿生一氧化氮的产生
DOI：
10.1002/cbic.201800337
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发表时间：
2018
期刊：
影响因子：
3.2
通讯作者：
Wang Kemin
中科院分区：
文献类型：
--
作者：
Zhou Li;Liu Yu;Shi Hui;Yang Xiaohai;Huang Jin;Liu Songyang;Chen Qiaoshu;Liu Jianbo;Wang Kemin
近年来，多个酶在特定位置的空间组织以实现受控级联反应引起了广泛的关注。在这里，我们报告了一个仿生酶级联DNA三角棱柱（TP）纳米结构上组织的建设，使一氧化氮（NO）的有效催化生产的一个单一的微珠。两种酶，葡萄糖氧化酶（GOx）和辣根过氧化物酶（HRP），通过使用具有小酶间距离的DNA结合蛋白衔接子在DNA TP纳米结构上的相邻位置组装。在级联反应中，第一种酶GOx在氧气存在下将葡萄糖转化为葡萄糖酸。所产生的H2 O2中间体被迅速转运到第二种酶HRP，HRP将羟基脲氧化成NO和其他硝酰基物质。带负电荷的DNA纳米结构的表面附近的pH被认为低于本体溶液中的pH;这为锚定的酶创造了最佳pH环境，这导致NO产物的产率更高。此外，多酶系统被固定在由DNA适配器介导的微珠上，这使得能够在微反应器中有效地催化产生气体分子。因此，这项工作提供了一个替代途径，通过酶级联仿生生成NO。特别是，DNA序列的动态结合能力使蛋白酶和DNA纳米结构的位置能够逆转，这使得级联催化能够被调节。
Spatial organization of multiple enzymes at specific positions for a controlled reaction cascade has attracted wide attention in recent years. Here, we report the construction of a biomimetic enzyme cascade organized on DNA triangle prism (TP) nanostructures to enable the efficient catalytic production of nitric oxide (NO) on a single microbead. Two enzymes, glucose oxidase (GOx) and horseradish peroxidase (HRP), were assembled at adjacent locations on a DNA TP nanostructure by using DNA‐binding protein adaptors with small interenzyme distances. In the cascade, the first enzyme, GOx, converts glucose into gluconic acid in the presence of oxygen. The produced H2O2 intermediate is rapidly transported to the second enzyme, HRP, which oxides hydroxyurea into NO and other nitroxyl species. The pH near the surface of the negatively charged DNA nanostructures is believed to be lower than that in the bulk solution; this creates an optimal pH environment for the anchored enzymes, which results in higher yields of the NO product. Furthermore, the multienzyme system was immobilized on a microbead mediated by a DNA adaptor, and this enabled the efficient catalytic generation of gas molecules in the microreactor. Therefore, this work provides an alternative route for the biomimetic generation of NO through enzyme cascades. In particular, the dynamic binding capability of the DNA sequence enabled the positions of the protein enzyme and the DNA nanostructure to be reversed, which allowed the cascade catalysis to be modulated.