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Neutron diffraction study of hydrogels

中性子回折法によるハイドロゲル研究

関根 由莉奈   ; 深澤 倫子*; 小林 理気*; Chi, S.*; Fernandez, J.*; 深澤 裕

Sekine, Yurina; Fukazawa, Tomoko*; Kobayashi, Riki*; Chi, S.*; Fernandez, J.*; Fukazawa, Hiroshi

ハイドロゲルとは、3次元のポリマーネットワークに多量の水を安定に含む物質である。本研究では、ゲル中における水の性質や構造を明らかにすることを目的として、オークリッジ国立研究所の中性子回折装置(WAND)を用いて含水率の異なるポリ$$N$$,$$N$$-ジメチルアクリルアミドゲルの中性子散乱を測定した。結果、低含水率のゲルにおいて、230K以下でアモルファス氷の回折パターンを観察した。昇温過程に伴いアモルファス氷の回折パターンはcubic氷の回折パターンへと変化した。これらの結果より、ハイドロゲル中には通常と異なる水が存在することが明らかとなった。これらの性質は、ゲル材料の開発において重要な知見となると考えている。

Hydrogels are unique materials that can contain a large amount of water in their three-dimensional polymer chain networks. We used neutron diffraction to probe the structure of D$$_{2}$$O in poly-$$N$$,$$N$$,-dimethylacrylamide (PDMAA) hydrogel. Two PDMAA hydrogels with high and low D$$_{2}$$O-content W (W = 0.9 and 0.5) were prepared. The neutron diffraction measurements were performed using the Wide Angle Neutron Diffractometer (WAND) at the High Flux Isotope Reactor in Oak Ridge, U.S.A. The samples were rapidly cooled using liquid nitrogen, and then heated from 10 to 300 K. The neutron diffraction profiles of the high D$$_{2}$$O-content PDMAA gel (W = 0.9) have strong sharp peaks below 270 K that are similar to diffraction patterns of hexagonal ice Ih. At 300 K, the profile has a broad liquid-like diffraction feature. The profile of the gel at W = 0.5 has a broad band in the 2$$theta$$ range from 20$$^{circ}$$ - 28$$^{circ}$$ below 230 K that are similar to diffraction pattern of glassy water. Sharp peaks are observed in the profile at 230 K. The feature of the profile is similar to that of cubic ice. The profile at 260 K has ice Ih-like strong peaks. Our neutron diffraction results show the existence of ice in hydrogels and that the structure of ice depends on the water content of the hydrogel. The structural changes of ice in hydrogels might have important implications in the interpretation of hydrogel properties, for both biological tissues and synthetic gel materials.

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