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hols are 1.17 × 10−6 and 2.9 × 10−6 cm2s−1, respectively, and are in good agreement with the philic domains constrains indirectly the segmental motion of the hydrophobic blocks, and Materials 2021, 14, 1617 literature values. Except for the A50G4S-10 membrane, the cross-linked diblock membranes generally showed much greater alcohol resistance than the Nafion 117 membrane. The relatively poor showing of the A50G4S-10 membrane could be attributed to excessive swell- ing caused by a higher proportion of sulfonic acid groups in this ionomer. In these Figures, 12 of 20 alcohol permeability of Nafion 117 presents an obvious increasing trend compared to the other membranes in question with the increase in alcohol concentration. Materials 2021, 14, x FOR PEER REVIEW 13 of 20 Figure 9. Effect of methanol concentration on the methanol permeability of cross-linked diblock Figure 9. Effect of methanol concentration on the methanol permeability of cross-linked diblock ionomer membranes. A Nafion 117 membrane is included for comparison. ionomer membranes. A Nafion 117 membrane is included for comparison. Figure 10. Effect of ethanol concentration on the ethanol permeability of cross-linked diblock ionomer Figure 10. Effect of ethanol concentration on the ethanol permeability of cross-linked diblock iono- mermbermanbersa.nAesN. AafiNonaf1io1n7 m11e7mbermanberaisnienicsluindceldudfoerdcfomr cpoamrispoanri.son. This trend may be attributed to the ease of swelling of Nafion in alcohols, thereby This trend may be attributed to the ease of swelling of Nafion in alcohols, thereby allowing alcohol molecules to be able to transport through hydrophilic domains in the allowing alcohol molecules to be able to transport through hydrophilic domains in the membrane. However, the extent of swelling is lower in the cross-linked diblock ionomer membrane. However, the extent of swelling is lower in the cross-linked diblock ionomer membranes. Furthermore, the swelling characteristics in methanol and ethanol are com- membranes. Furthermore, the swelling characteristics in methanol and ethanol are com- pletely different. While methanol concentration does not apparently affect methanol pletely different. While methanol concentration does not apparently affect methanol per- permeability, ethanol permeability is significantly lowered in higher ethanol concentra- meability, ethanol permeability is significantly lowered in higher ethanol concentrations. tions. These opposite trends could be understood in terms of solvent solvation effects. These opposite trends could be understood in terms of solvent solvation effects. The hy- The hydrophobic (AN-co-GMA) block can be partially solvated by ethanol while the hy- drophobic (AN-co-GMA) block can be partially solvated by ethanol while the hydrophilic drophilic SPM block is completely solvated by water. Increase in ethanol concentration SPM block is completely solvated by water. Increase in ethanol concentration could there- could therefore promote the segmental motion of the hydrophobic blocks through the fore promote the segmental motion of the hydrophobic blocks through the ethanol solva- ethanol solvation effect. On the other hand, the decrease in the water content at the same tion effect. On the other hand, the decrease in the water content at the same time would time would reduce hydration of the hydrophilic domains and hence the segmental mo- reduce hydration of the hydrophilic domains and hence the segmental motion of the hy- drophilic blocks. It is noteworthy to point out that the decreased mobility of the hydro- philic blocks could also impede the segmental motion of the hydrophobic blocks; con- travening the increase in hydrophobic mobility due to the ethanol solvation effect. For example, at high ethanol concentrations (8 M) the reduced water content in the hydro-PDF Image | Hydrophilic Cross-Linked Aliphatic Hydrocarbon Diblock Copolymer
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