Understanding the variability of properties in Antheraea pernyi silk fibres

Variability is a common feature of natural silk fibres, caused by a range of natural processing conditions. Better understanding of variability will not only be favourable for explaining the enviable mechanical properties of animal silks but will provide valuable information for the design of advanced artificial and biomimetic silk-like materials. In this work, we have investigated the origin of variability in forcibly reeled Antheraea pernyi silks from different individuals using dynamic mechanical thermal analysis (DMTA) combined with the effect of polar solvent penetration. Quasi-static tensile curves in different media have been tested to show the considerable variability of tensile properties between samples from different silkworms. The DMTA profiles (as a function of temperature or humidity) through the glass transition region of different silks as well as dynamic mechanical properties after high temperature and water annealing are analysed in detail to identify the origin of silk variability in terms of molecular structures and interactions, which indicate that different hydrogen bonded structures exist in the amorphous regions and they are notably different for silks from different individuals. Solubility parameter effects of solvents are quantitatively correlated with the different glass transitions values. Furthermore, the overall ordered fraction is shown to be a key parameter to quantify the variability in the different silk fibres, which is consistent with DMTA and FTIR observations.