Andrea C. Bardales, Joseph R. Mills and Dmitry M. Kolpashchikov*,
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引用次数: 0
摘要
合成寡核苷酸的可获得性和 DNA 纳米技术的成功为利用 DNA 纳米结构构建复杂的酶催化中心提供了可能。在这里,我们使用双 DNA 交叉(DX)瓦片纳米结构来提高任意序列的两个寡核苷酸的 5'-5' 连接速率、产量和特异性。通过简单的程序就能分离出连接产物。同样的策略也应用于 3'-3' 连接的寡核苷酸的合成,从而为 DNA 和 RNA 的合成引入了一条方向可调的途径,而且资源匮乏的实验室也能负担得起。为了强调连接产物的实用性,我们合成了一种由分子内互补形成的环状结构,并将其命名为 "不可能的 DNA 轮",因为它无法通过酶促反应从常规 DNA 链构建而成。因此,DX-tile 纳米结构可以为生产酶合成无法实现的有用化学产品开辟一条途径。这是利用 DNA 纳米结构作为催化剂的首个实例。这项研究提倡进一步探索 DNA 纳米技术,以构建类似酶的反应系统。
DNA Nanostructures as Catalysts: Double Crossover Tile-Assisted 5′ to 5′ and 3′ to 3′ Chemical Ligation of Oligonucleotides
Accessibility of synthetic oligonucleotides and the success of DNA nanotechnology open a possibility to use DNA nanostructures for building sophisticated enzyme-like catalytic centers. Here we used a double DNA crossover (DX) tile nanostructure to enhance the rate, the yield, and the specificity of 5′–5′ ligation of two oligonucleotides with arbitrary sequences. The ligation product was isolated via a simple procedure. The same strategy was applied for the synthesis of 3′–3′ linked oligonucleotides, thus introducing a synthetic route to DNA and RNA with a switched orientation that is affordable by a low-resource laboratory. To emphasize the utility of the ligation products, we synthesized a circular structure formed from intramolecular complementarity that we named “an impossible DNA wheel” since it cannot be built from regular DNA strands by enzymatic reactions. Therefore, DX-tile nanostructures can open a route to producing useful chemical products that are unattainable via enzymatic synthesis. This is the first example of the use of DNA nanostructures as a catalyst. This study advocates for further exploration of DNA nanotechnology for building enzyme-like reactive systems.
期刊介绍:
Bioconjugate Chemistry invites original contributions on all research at the interface between man-made and biological materials. The mission of the journal is to communicate to advances in fields including therapeutic delivery, imaging, bionanotechnology, and synthetic biology. Bioconjugate Chemistry is intended to provide a forum for presentation of research relevant to all aspects of bioconjugates, including the preparation, properties and applications of biomolecular conjugates.