氢键对丙烯酰胺类共聚物溶液流变行为与DNA分离性能的影响

Influence of Hydrogen Bonding on Rheological Behavior and DNA Separation Performance of Acrylamide-Based Copolymer Solutions

摘要

通过溶液聚合法制备了一系列不同结构单元比例的N,N-二甲基丙烯酰胺（DMA）与羟乙基丙烯酰胺（HEA）的共聚物（P(DMA-co-HEA)，简称PDH），并系统研究了聚合物溶液的氢键相互作用、质量浓度、温度及剪切速率对聚合物溶液流变学性能的影响，同时将其应用于毛细管电泳以评估HEA含量对脱氧核糖核酸（DNA）片段分离性能的影响。流变学研究结果表明，在不同质量浓度和温度下，当n(DMA)/n(HEA)为30时，P(DMA-co-HEA)的增黏性能达到最优，说明适量的HEA结构单元能够通过氢键相互作用提高聚合物溶液的抗剪切稳定性和高温流变稳定性。黏弹行为结果表明，当n(DMA)/n(HEA)为20～40时，体系能够形成稳定的弱氢键物理网络。DNA片段分析结果进一步表明，适当引入HEA有助于提高对DNA片段的分离能力，其中当n(DMA)/n(HEA)为30时，PDH表现出最优的分离性能、较小的峰衰程度以及良好的分析重现性。

Abstract

Using N,N-dimethylacrylamide (DMA) and hydroxyethyl acrylamide (HEA) as comonomers, a series of P(DMA-co-HEA) copolymers with varying structural unit ratios were synthesized via solution polymerization. The hydrogen-bonding interactions in the polymer solutions and the effects of mass concentration, temperature, and shear rate on the rheological properties of the polymer solutions were systematically investigated. Concurrently, the copolymers were employed as sieving matrices in capillary electrophoresis applications to assess the impact of HEA content on the separation performance of deoxyribonucleic acid (DNA) fragments. Rheological results revealed that, across different mass concentrations and temperatures, the thickening ability of P(DMA-co-HEA) reached its maximum at a structural unit molar ratio (n(DMA)/n(HEA)) of 30, indicating that appropriate HEA structural units can improve the shear stability and high-temperature rheological stability of polymer solutions via hydrogen-bonding interactions. Furthermore, the evaluation of viscoelastic behavior demonstrated that a stable, weak hydrogen-bonded physical network is formed within the system when n(DMA)/n(HEA) ranges from 20 to 40. DNA fragment analysis further confirmed that the proper incorporation of HEA facilitates the enhancement of DNA separation capability. Notably, when n(DMA)/n(HEA) was 30, the sieving matrix exhibited optimal separation performance, minimized peak attenuation, and excellent analytical reproducibility.

关键词

N,N-二甲基丙烯酰胺 / 羟乙基丙烯酰胺 / 流变学 / 氢键 / DNA片段分离

Key words

N,N-dimethylacrylamide / hydroxyethyl acrylamide / rheology / hydrogen bond / DNA fragment separation

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