Hata Yuuki, Kojima Tomoya, Koizumi Taro, Okura Hiromichi, Sakai Takamasa, Sawada Toshiki, Serizawa Takeshi
Department of Bioengineering, Graduate School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
Precursory Research for Embryonic Science and Technology, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi-shi, Saitama 332-0012, Japan.
ACS Macro Lett. 2017 Feb 21;6(2):165-170. doi: 10.1021/acsmacrolett.6b00848. Epub 2017 Feb 3.
Macromolecular crowding, a solution state with high macromolecular concentrations, was used to promote the crystallization-driven self-assembly of enzymatically synthesized cellulose oligomers. Cellulose oligomers were synthesized via cellodextrin phosphorylase-catalyzed enzymatic reactions in the concentrated solutions of water-soluble polymers, such as dextran, poly(ethylene glycol), and poly(-vinylpyrrolidone). The reaction mixtures were transformed into cellulose oligomer hydrogels composed of well-grown crystalline nanoribbon networks irrespective of the polymer species. This method was successfully applied in the one-pot preparation of double network hydrogels composed of the nanoribbons and physically cross-linked gelatin molecules through the simple control of reaction temperatures, demonstrating the superior mechanical properties of the composite hydrogels. Our concept that promotes the growth of self-assembled architectures under macromolecular crowding conditions demonstrates a new avenue into developing novel hydrogel materials.
大分子拥挤效应，即一种具有高分子浓度的溶液状态，被用于促进酶促合成的纤维素低聚物的结晶驱动自组装。纤维素低聚物是通过纤维糊精磷酸化酶催化的酶促反应在水溶性聚合物（如葡聚糖、聚乙二醇和聚（乙烯基吡咯烷酮））的浓溶液中合成的。无论聚合物种类如何，反应混合物都能转化为由生长良好的结晶纳米带网络组成的纤维素低聚物水凝胶。通过简单控制反应温度，该方法成功应用于由纳米带和物理交联的明胶分子组成的双网络水凝胶的一锅法制备，证明了复合水凝胶具有优异的力学性能。我们在大分子拥挤条件下促进自组装结构生长的概念为开发新型水凝胶材料开辟了一条新途径。
