Preparation of thermoresponsive hydrogels via polymerizable deep eutectic monomer solvents,Polymer Chemistry

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Preparation of thermoresponsive hydrogels via polymerizable deep eutectic monomer solvents
Polymer Chemistry ( IF 4.1 ) Pub Date : 2020-11-24 , DOI: 10.1039/d0py01159b
Yeasmin Nahar _{1,

2,

3,

4} , James Horne _{2,

3,

4,

5} , Vinh Truong _{4,

6,

7,

8} , Alex C. Bissember _{1,

2,

3,

4} , Stuart C. Thickett _{1,

2,

3,

4}

Affiliation

We report the preparation of thermoresponsive poly(N-isopropylacrylamide) (polyNIPAM) hydrogels via the free radical polymerization of deep eutectic monomer solvents (DEMs) for the first time, where NIPAM serves as a polymerizable hydrogen bond donor. DEMs were prepared by a simple heating and stirring protocol using NIPAM and either choline chloride (ChCl) or acetylcholine chloride (AcChCl) (as hydrogen bond acceptor) in various ratios to yield low-melting point liquids (as low as 15 °C). 1D and 2D NMR spectroscopy supported the association of the NIPAM and choline salts present within the DEM structure, in addition to the low self-diffusion coefficients of the species present compared to when dissolved in water. Thermogravimetric analysis demonstrated an enhanced thermal stability of the DEMs compared to NIPAM. Hydrogels prepared by free-radical polymerization of the prepared DEMs in the presence of N,N′-methylenebisacrylamide (BIS) as crosslinker showed a significant increase in reaction rate compared to the equivalent reaction in water, which was attributed in part to the high viscosity of the DEMs. These gels exhibited thermoresponsive swelling behaviour when immersed in water. Specifically, gels prepared via DEMs featured reduced swelling capacity and increased mechanical strength relative to those prepared by aqueous polymerization, attributed to a significant increase in cross-linking density.

中文翻译：

通过可聚合的深共晶单体溶剂制备热敏性水凝胶

我们报告温敏聚（编制ñ -isopropylacrylamide）（polyNIPAM）水凝胶通过深共晶单体溶剂（DEM）的自由基聚合首次出现，其中NIPAM用作可聚合的氢键供体。通过使用NIPAM和氯化胆碱（ChCl）或乙酰胆碱氯化物（AcChCl）（作为氢键受体）以各种比例通过简单的加热和搅拌方案制备DEM，以产生低熔点液体（低至15°C）。1D和2D NMR光谱支持NIPAM和DEM结构内存在的胆碱盐的缔合，此外，与溶解在水中相比，该物种的自扩散系数低。热重分析表明，与NIPAM相比，DEM的热稳定性更高。在N的存在下，通过自由基聚合制备的DEM制备的水凝胶，与在水中的等效反应相比，作为交联剂的N'-亚甲基双丙烯酰胺（BIS）显示出反应速率的显着提高，这部分归因于DEM的高粘度。当浸入水中时，这些凝胶表现出热响应性溶胀行为。具体而言，与通过水聚合制备的那些凝胶相比，通过DEM制备的凝胶的溶胀能力降低，机械强度提高，这归因于交联密度的显着提高。

更新日期：2020-12-16

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