DNA Nanostructures as Catalysts: Double Crossover Tile-Assisted 5′ to 5′ and 3′ to 3′ Chemical Ligation of Oligonucleotides
DNA Nanostructures as Catalysts: Double Crossover Tile-Assisted 5′ to 5′ and 3′ to 3′ Chemical Ligation of Oligonucleotides
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DOI：
10.1021/acs.bioconjchem.3c00502
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发表时间：
2023-12-22
影响因子：
4.7
通讯作者：
Kolpashchikov，Dmitry M.
中科院分区：
文献类型：
--
作者：
Bardales，Andrea C.;Mills，Joseph R.;Kolpashchikov，Dmitry M.
合成寡核苷酸的可及性和 DNA 纳米技术的成功为使用 DNA 纳米结构构建复杂的酶样催化中心提供了可能性。在这里，我们使用双 DNA 交叉 (DX) 平铺纳米结构来提高任意序列的两个寡核苷酸 5'–5' 连接的速率、产量和特异性。通过简单的程序分离连接产物。同样的策略也适用于 3'–3' 连接寡核苷酸的合成，从而引入了一种低资源实验室可以负担得起的方向转换的 DNA 和 RNA 合成路线。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性形成的圆形结构，我们将其命名为“不可能的 DNA 轮”，因为它不能通过酶促反应从常规 DNA 链构建。因此，DX-tile 纳米结构可以开辟一条生产通过酶合成无法获得的有用化学产品的途径。这是使用 DNA 纳米结构作为催化剂的第一个例子。这项研究提倡进一步探索 DNA 纳米技术来构建类酶反应系统。
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.