In this paper, we report chemoselective ligation-assisted self-assembly of DNA walker. Specifically, three kinds of chemoselective ligations including azide-alkyne cycloaddition, oxime ligation, and hydrazone ligation, have been proposed to mediate the self-assembly of DNA walker and to induce the following operation. Then, we present our design that the walking strand of the DNA walker is splitted as action strand and supporting strand, which are separately modified by the pair of the chemoselective linkage groups. Therefore, combined with the supporting strand, the action strand can activate the DNA walker, which can be further developed as a biosensor for the analysis of different kinds of biomolecules such as polysaccharide, protein, and nucleic acid. Taking lipopolysaccharide, thrombin, and Let-7a as examples, the fabricated biosensors based on chemoselective ligation-assisted DNA walkers all exhibit high sensitivity and accuracy in view of the great advantages of chemoselective ligation. This work may provide an insight for covalent bond adjusted molecular self-assembly and the development of biosensor based on the construction of DNA walker.

在本文中，我们报道了DNA Walker的化学选择性连接辅助自组装。具体地，已经提出了三种化学选择性连接，包括叠氮化物-炔烃环加成，肟连接和连接，以介导DNA Walker的自组装并诱导以下操作。然后，我们提出我们的设计，将DNA Walker的行走链拆分为作用链和支撑链，分别通过一对化学选择性连接基团进行修饰。因此，与支撑链结合，作用链可以激活DNA Walker，该DNA Walker可以进一步发展为一种生物传感器，用于分析不同种类的生物分子，例如多糖，蛋白质和核酸。以脂多糖，凝血酶和Let-7a为例，考虑到化学选择性连接的巨大优势，基于化学选择性连接辅助的DNA Walker制成的生物传感器都具有很高的灵敏度和准确性。这项工作可以为共价键调节的分子自组装和基于DNA Walker构建的生物传感器的发展提供见解。