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Investigation of the state and dynamics of water in hydrogels of cellulose ethers by1H NMR spectroscopy

机译:1H NMR光谱研究纤维素醚水凝胶中水的状态和动力学

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摘要

The aim of this work was to study the effect of the type of substituent of the cellulose ethers and the molecular mass on the state and dynamics of water in the respective hydrogels to specify the quantity of adsorbed water on the polymers or, more explicitly, to calculate the average number of water molecules bound to a polymer repeating unit (PRU).1H NMR relaxation experiments were performed on equilibrated systems of cellulose ether polymers (HEC, HPC, HPMC K4M, and HPMC K100M) with water. In particular, the water proton spinlattice (T1) and spin-spin (T2) relaxation times were measured in these systems at room temperature. The observed proton NMRT1 andT2 of water in hydrogels at different cellulose ether concentrations at room temperature were shown to decrease with increasing polymer concentration. The relaxation rate 1/T1 is sensitive to the type of polymer substituent but insensitive to the polymer molecular mass. The rate 1/T2 appears much less influenced by the polymer substitution. The procedure developed for calculating the amount of water bound per PRU, based on the analysis of theT1 andT2 data, shows that this amount is the largest for HPC followed by HEC, HP MC K4M, and HPMC K100M. The results correlate well with the degree of hydrophilic substitution of the polymer chains. This NMR analysis deals with a single molecular layer of adsorbed water for the investigated cellulose ether polymers at all concentrations, while the rest of the water in the hydrogel is bulk-like. Therefore, the mesh size of polymer network in the view of a single molecular layer is not effectively changed.
机译:这项工作的目的是研究纤维素醚的取代基类型和分子质量对各自水凝胶中水的状态和动力学的影响,从而确定聚合物上水的吸附量,或者更明确地讲,计算与聚合物重复单元(PRU)结合的水分子的平均数。 1 H NMR弛豫实验是在平衡的纤维素醚聚合物体系(HEC,HPC,HPMC K4M和HPMC K100M)上进行的与水。特别是,在室温下,在这些系统中测量了水质子自旋晶格(T1)和自旋自旋(T2)弛豫时间。在室温下,在不同纤维素醚浓度下,水凝胶中水的质子NMRT1和T2随聚合物浓度的增加而降低。弛豫速率1 / T1对聚合物取代基的类型敏感,但对聚合物分子量不敏感。速率1 / T2似乎受聚合物取代的影响小得多。基于对T1和T2数据的分析而开发的用于计算每个PRU结合水的数量的程序表明,对于HPC,此数量最大,其次是HEC,HP MC K4M和HPMC K100M。结果与聚合物链的亲水取代度很好地相关。这项NMR分析处理了所有浓度下所研究的纤维素醚聚合物的吸附水的单分子层,而水凝胶中的其余水则呈块状。因此,从单分子层的观点来看,聚合物网络的网眼尺寸不能有效地改变。

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