writer：Anh Tuan Nguyen, Qiao‐Ling Huang, Zhen Yang, Naibo Lin, Gangqin Xu, Xiang Yang Liu*
keywords：silk
source：期刊
specific source：Small, 2015, 11 (9-10): 1039-54
Issue time：2015年

This review provides a comprehensive survey of the structural characteristics of crystal networks of silk soft fibrous materials in correlation with the macroscopic properties/performance and the network formation mechanisms. The correlation between the hierarchical mesoscopic structures and the mechanical properties of silk soft fi brous materials including silk fibroin hydrogels and naturally spun silk fi bers are addressed based on the hierarchical crystal network models. Namely, two types of hierarchical networks are identifi ed: the weak nanofi brilnanofi bril interaction case (i.e., silk fi broin hydrogels), and the strong nanofi bril–nanofi bril interaction case (i.e., silk fi bers). The macroscopic properties, i.e., the rheological/mechanical properties, can be controlled in terms of tuning different levels of hierarchical network structures by ultrasonication-induced gelation, introducing the initial nucleation centers, etc. Such controls take effect by different mesoscale assembly pathways, which are found to occur via different routes of the nucleation and growth processes. Furthermore, the hierarchical network model of soft fi brous materials can be applied to explain the superior mechanical properties and the unique strainhardening behaviors of spider silk fi bers within the framework of hierarchical breaking mechanism. Obviously, a knowledge of crystal networks will allow the prediction of the performance and engineering strategy of silk fi brous materials in generals.