A General DNA-Gated Hydrogel Strategy for Selective Transport of Chemical and Biological Cargos
A General DNA-Gated Hydrogel Strategy for Selective Transport of Chemical and Biological Cargos
复制标题
DOI：
10.1021/jacs.1c08114
复制
发表时间：
2021-10-06
影响因子：
15
通讯作者：
Mirkin, Chad A.
中科院分区：
文献类型：
--
作者：
Gu, Yuwei;Distler, Max E.;Mirkin, Chad A.
分子货物的选择性运输在许多生物和化学/材料工艺和应用中是至关重要的。尽管自然界已经进化出高效的体内生物运输系统，但合成运输系统往往受到货物与合成或自然运输屏障之间微调相互作用的挑战的限制。在这里，精心设计的DNA-DNA相互作用被探索为通过DNA接枝的水凝胶载体选择性地传输DNA修饰的货物的一种新方式。货物和水凝胶屏障的化学和物理特性，包括货物上的核酸链数(即货价)和DNA-DNA结合强度，可用于调节货物运输的效率。存在这样一些制度，其中货物-屏障相互作用足够吸引人，以产生高选择性和高机动性，而在其他制度中，吸引人的相互作用太强，不能允许流动性。这些观察结果导致了DNA-树状分子运输标签的设计，该标签可用于普遍修饰大分子货物，以便屏障可以区分要运输的特定物种。这些利用DNA-DNA相互作用的新型运输系统为控制水凝胶中选择性货物流动性的因素提供了新的化学见解，并为设计各种药物/探针输送系统打开了大门。
The selective transport of molecular cargo is critical in many biological and chemical/materials processes and applications. Although nature has evolved highly efficient in vivo biological transport systems, synthetic transport systems are often limited by the challenges associated with fine-tuning interactions between cargo and synthetic or natural transport barriers. Herein, deliberately designed DNA-DNA interactions are explored as a new modality for selective DNA-modified cargo transport through DNA-grafted hydrogel supports. The chemical and physical characteristics of the cargo and hydrogel barrier, including the number of nucleic acid strands on the cargo (i.e., the cargo valency) and DNA-DNA binding strength, can be used to regulate the efficiency of cargo transport. Regimes exist where a cargo-barrier interaction is attractive enough to yield high selectivity yet high mobility, while there are others where the attractive interactions are too strong to allow mobility. These observations led to the design of a DNA-dendron transport tag, which can be used to universally modify macromolecular cargo so that the barrier can differentiate specific species to be transported. These novel transport systems that leverage DNA-DNA interactions provide new chemical insights into the factors that control selective cargo mobility in hydrogels and open the door to designing a wide variety of drug/probe-delivery systems.