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Silk granular hydrogels self-reinforced with regenerated silk fibroin fibers
Soft Matter ( IF 2.9 ) Pub Date : 2021-07-08 , DOI: 10.1039/d1sm00585e Céline Samira Wyss 1 , Peyman Karami 2 , Adrien Demongeot 1 , Pierre-Etienne Bourban 1 , Dominique P Pioletti 2
Soft Matter ( IF 2.9 ) Pub Date : 2021-07-08 , DOI: 10.1039/d1sm00585e Céline Samira Wyss 1 , Peyman Karami 2 , Adrien Demongeot 1 , Pierre-Etienne Bourban 1 , Dominique P Pioletti 2
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Granular hydrogels with high stability, strength, and toughness are laborious to develop. Post-curing is often employed to bind microgels chemically and enhance mechanical properties. Here a unique strategy was investigated to maintain microgels together with a novel self-reinforced silk granular hydrogel composed of 10 wt% 20 kDa poly(ethylene glycol) dimethacrylate microgels and regenerated silk fibroin fibers. The principle is to use the swelling of microgels to concentrate the surrounding solution and regenerate silk fibroin in situ. Self-reinforcement is subsequently one of the added functions. We showed that silk fibroin in most compositions was homogeneously distributed and had successfully regenerated in situ around microgels, holding them together in a network-like structure. FTIR analysis revealed the presence of amorphous and crystalline silk fibroin, where 50% of the secondary structures could be assigned to strong β-sheets. Swelling ratios, i.e. 10–45 vol%, increased proportionally with the microgel content, suggesting that mainly microgels governed swelling. In contrast, the elastic modulus, i.e. 58–296 kPa, increased almost linearly with silk fibroin content. Moreover, we showed that the precursor could be injected and cast into a given shape. Viscous precursors of various compositions were also placed side by side to create mechanical gradients. Finally, it was demonstrated that silk granular hydrogel could successfully be synthesized with other microgels like gelatin methacryloyl. Silk granular hydrogels represent, therefore, a novel class of self-reinforced hydrogel structures with tunable swelling and elastic properties.
中文翻译：
用再生丝素蛋白纤维自增强的丝粒水凝胶
具有高稳定性、强度和韧性的颗粒状水凝胶很难开发。后固化通常用于化学结合微凝胶并提高机械性能。这里研究了一种独特的策略来维持微凝胶以及由 10 wt% 20 kDa 聚（乙二醇）二甲基丙烯酸酯微凝胶和再生丝素蛋白纤维组成的新型自增强丝颗粒水凝胶。其原理是利用微凝胶的溶胀作用浓缩周围溶液，原位再生丝素蛋白。自我强化随后是附加功能之一。我们发现大多数组合物中的丝素蛋白分布均匀，并已成功原位再生围绕微凝胶，将它们固定在网络状结构中。FTIR 分析显示存在无定形和结晶丝素蛋白，其中 50% 的二级结构可以分配给强β-折叠。溶胀率，即10–45 vol%，随微凝胶含量成比例增加，表明主要是微凝胶控制溶胀。相比之下，弹性模量，即58-296 kPa，几乎随丝素蛋白含量线性增加。此外，我们表明可以将前体注入并浇铸成给定的形状。各种组成的粘性前体也并排放置以产生机械梯度。最后，证明了丝粒水凝胶可以与其他微凝胶如明胶甲基丙烯酰成功合成。因此，丝粒水凝胶代表了一类具有可调膨胀和弹性特性的新型自增强水凝胶结构。
更新日期：2021-07-12
中文翻译：
用再生丝素蛋白纤维自增强的丝粒水凝胶
具有高稳定性、强度和韧性的颗粒状水凝胶很难开发。后固化通常用于化学结合微凝胶并提高机械性能。这里研究了一种独特的策略来维持微凝胶以及由 10 wt% 20 kDa 聚（乙二醇）二甲基丙烯酸酯微凝胶和再生丝素蛋白纤维组成的新型自增强丝颗粒水凝胶。其原理是利用微凝胶的溶胀作用浓缩周围溶液，原位再生丝素蛋白。自我强化随后是附加功能之一。我们发现大多数组合物中的丝素蛋白分布均匀，并已成功原位再生围绕微凝胶，将它们固定在网络状结构中。FTIR 分析显示存在无定形和结晶丝素蛋白，其中 50% 的二级结构可以分配给强β-折叠。溶胀率，即10–45 vol%，随微凝胶含量成比例增加，表明主要是微凝胶控制溶胀。相比之下，弹性模量，即58-296 kPa，几乎随丝素蛋白含量线性增加。此外，我们表明可以将前体注入并浇铸成给定的形状。各种组成的粘性前体也并排放置以产生机械梯度。最后，证明了丝粒水凝胶可以与其他微凝胶如明胶甲基丙烯酰成功合成。因此，丝粒水凝胶代表了一类具有可调膨胀和弹性特性的新型自增强水凝胶结构。
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