School of Engineering, Westlake University, Hangzhou, Zhejiang 310030, China.
School of Medicine, Ningbo University, Ningbo, Zhejiang 315211, China; Department of Otolaryngology Head and Neck Surgery, Ningbo Medical Center of Lihuili Hospital, The Affiliated Hospital of Ningbo University, Ningbo, Zhejiang 315040, China.
Acta Biomater. 2022 Nov;153:149-158. doi: 10.1016/j.actbio.2022.09.010. Epub 2022 Sep 12.
Naturally derived protein-based biopolymers are considered potential biomaterials in biomedical applications and eco-friendly materials for replacing current petroleum-based polymers due to their good biocompatibility, low environmental impact, and tunable degradability. However, current strategies for fabricating protein-based materials with superior properties and tailored functionality in a scalable manner are still lacking. Here, we demonstrate an aqueous-based scalable approach for fabricating silk protein-based films through controlled molecular self-assembly (CMS) of silk proteins with plasticizers and salt ions. The films fabricated using this method can achieve a toughness of up to 64±5 MJ/m with a stretchability of up to 574±31%. We also demonstrate the tunable enzymatic degradability, low in vitro cytotoxicity, and good in vivo biocompatibility of the films. Furthermore, the films can be patterned with predesigned complex structures through laser cutting and functionalized with bioactive components. The functional silk protein-based films show great potential in various applications, including flexible electronics, bioelectronics, tissue engineering, and bioplastic packaging. STATEMENT OF SIGNIFICANCE: Inspired by the naturally optimized multi-scale self-assembly of silk proteins in natural silks, we develop an aqueous-based approach for scalable production of superior protein-based films through controlled molecular self-assembly (CMS) of silk proteins with glycerol and calcium ions. The prepared silk films present outstanding mechanical properties, controlled enzymatic biodegradability, low in vitro cytotoxicity, and good in vivo biocompatibility. Notably, the films fabricated using this method can achieve a high toughness of 64±5 MJ/m with a stretchability of 594±31%. The approach introduced in this work provides a facile route toward making silk-based materials with superior properties. It also paves new avenues for developing functional protein-based materials with precisely controlled structures and properties for various applications.
天然衍生的蛋白质基生物聚合物由于其良好的生物相容性、低环境影响和可调节的降解性，被认为是生物医学应用中的潜在生物材料和环保材料，可替代当前的石油基聚合物。然而，目前仍然缺乏以可扩展的方式制造具有优异性能和定制功能的蛋白质基材料的策略。在这里，我们展示了一种基于水的可扩展方法，通过丝蛋白与增塑剂和盐离子的受控分子自组装（CMS）来制造丝蛋白基薄膜。使用这种方法制造的薄膜可以达到高达 64±5 MJ/m 的韧性和高达 574±31%的拉伸性。我们还证明了薄膜具有可调的酶降解性、低体外细胞毒性和良好的体内生物相容性。此外，薄膜可以通过激光切割进行图案化，并与生物活性成分进行功能化。功能化的丝蛋白基薄膜在各种应用中具有很大的潜力，包括柔性电子、生物电子、组织工程和生物塑料包装。
受天然丝中丝蛋白的自然优化多尺度自组装的启发，我们开发了一种基于水的方法，通过丝蛋白与甘油和钙离子的受控分子自组装（CMS）来可扩展地生产优异的蛋白质基薄膜。所制备的丝膜具有出色的机械性能、可控的酶降解性、低体外细胞毒性和良好的体内生物相容性。值得注意的是，使用这种方法制造的薄膜可以达到 64±5 MJ/m 的高韧性和 594±31%的拉伸性。本工作中介绍的方法为制造具有优异性能的基于丝的材料提供了一种简便的途径。它还为开发具有精确控制结构和性能的功能性蛋白质基材料开辟了新途径，可用于各种应用。
