Decoding silkworm spinning programmed by pH and metal ions

丝素 丝绸 纺纱 材料科学 纳米技术 化学工程 水溶液中的金属离子 化学 高分子化学 离子 生物物理学 复合材料 有机化学 生物 工程类
作者
Kai Song,Yejing Wang,Wenjie Dong,Zhenzhen Li,Qingyou Xia,Ping Zhu,Huawei He
出处
期刊:Science Bulletin [Elsevier BV]
卷期号:69 (6): 792-802 被引量:12
标识
DOI:10.1016/j.scib.2023.12.050
摘要

Silk is one of the toughest fibrous materials known despite spun at ambient temperature and pressure with water as a solvent. It is a great challenge to reproduce high-performance artificial fibers comparable to natural silk by bionic for the incomplete understanding of silkworm spinning in vivo. Here, we found that amphipol and digitonin stabilized the structure of natural silk fibroin (NSF) by a large-scale screening in vitro, and then studied the close-to-native ultrastructure and hierarchical assembly of NSF in the silk gland lumen. Our study showed that NSF formed reversible flexible nanofibrils mainly composed of random coils with a sedimentation coefficient of 5.8 S and a diameter of about 4 nm, rather than a micellar or rod-like structure assembled by the aggregation of globular NSF molecules. Metal ions were required for NSF nanofibril formation. The successive pH decrease from posterior silk gland (PSG) to anterior silk gland (ASG) resulted in a gradual increase in NSF hydrophobicity, thus inducing the sol-gelation transition of NSF nanofibrils. NSF nanofibrils were randomly dispersed from PSG to ASG-1, and self-assembled into anisotropic herringbone patterns at ASG-2 near the spinneret ready for silkworm spinning. Our findings reveal the controlled self-assembly mechanism of the multi-scale hierarchical architecture of NSF from nanofibrils to herringbone patterns programmed by metal ions and pH gradient, which provides novel insights into the spinning mechanism of silk-secreting insects and bioinspired design of high-performance fibers.
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