Complexation of Poly(ethylene glycol)-(ds)OligoDNA Conjugates with Ionic Liquids

IF 5.1 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2024-04-17 DOI:10.1021/acsmacrolett.4c00028

Young Hun Kim, Nayeong Jeon, Sujin Park, Siyoung Q. Choi, Eunji Lee* and Sheng Li*,

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Abstract

We report the complexation of poly(ethylene glycol) conjugated double-stranded oligoDNA (PEG-(ds)oligoDNA) with imidazolium-based ionic liquids (ILs) to form polyelectrolyte complex aggregates (PCAs). The PEG-(ds)oligoDNA conjugates are prepared following a solution-phase coupling reaction. The binding of PEG-(ds)oligoDNA with either 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF₄]) or 1-hexyl-3-methylimidazolium tetrafluoroborate ([HMIM][BF₄]) is confirmed by a fluorescence displacement assay. Both ILs show stronger binding affinity to PEG-(ds)oligoDNA than bare (ds)oligoDNA due to the PEG-assisted increase in IL cation concentration in the vicinity of (ds)oligoDNA. The complex morphology formed at various amine (N) to phosphate (P) ratios is also examined. At high N/P ratios above 4, nanosized PCAs are formed, driven by a counterion-mediated attraction among the IL-bound (ds)oligoDNA segments and stabilized by the conjugated PEG segments. The PCAs exhibit near-neutral surface charges and resistance to DNase degradation, suggesting their potential use in gene delivery applications.

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聚乙二醇-(ds)寡核苷酸共轭物与离子液体的络合反应

我们报告了聚乙二醇共轭双链寡 DNA（PEG-(ds)oligoDNA）与咪唑基离子液体（ILs）络合形成聚电解质复合物聚集体（PCAs）的过程。PEG-(ds)oligoDNA 共轭物是通过溶液相偶联反应制备的。PEG-(ds)oligoDNA 与 1-丁基-3-甲基咪唑四氟硼酸盐（[BMIM][BF4]）或 1-己基-3-甲基咪唑四氟硼酸盐（[HMIM][BF4]）的结合通过荧光置换试验得到了证实。与裸(ds)寡核苷酸相比，这两种 IL 与 PEG-(ds)寡核苷酸的结合亲和力都更强，这是因为 PEG 辅助增加了(ds)寡核苷酸附近的 IL 阳离子浓度。我们还研究了在不同胺（N）与磷酸盐（P）比率下形成的复合物形态。当 N/P 比率高于 4 时，在反离子介导的 IL 结合 (ds)oligoDNA 片段之间的吸引力驱动下，并在共轭 PEG 片段的稳定下，形成了纳米级的 PCAs。PCAs 显示出接近中性的表面电荷和抗 DNase 降解性，这表明它们有可能用于基因递送应用。

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来源期刊

ACS Macro Letters 化学-

CiteScore

10.40

自引率

3.40%

发文量

209

审稿时长

1 months

期刊介绍： ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.