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Origin of the variability of the mechanical properties of silk fibres: 1. The relationship between disorder, hydration and stress/strain behaviour

Abstract : The causes of the variability in mechanical behaviour of various silks obtained from silkworms (Bombyx mori, Antheraea/Tussah) and spiders (Nephila madagascarensis) have been studied by tensile uniaxial tests, differential scanning calorimetry and Raman microspectrometry. Analyses of tensile stress–strain curves recorded for different silkworm and spider baves and single fibres, undergoing different histories (age, degumming, thermal/chemical treatments), allow the behaviour to be classified into five groups and correlated with the fibroin/spidroin structural status: (1) Type I exhibits linear elastic behaviour and then a quasi plateau, (2) Type II has a two-step linear elastic behaviour with kinks then a quasi plateau, (3) Type III exhibits a smooth transition from a linear behaviour to a plateau, (4) Type IV has a behaviour rather similar to that of Type I but above ~8–12% hardening occurs, and (5) Type V results in the breakage of fibres during the first elastic stage. Unambiguously, Type IV is more frequent for degummed, very dried fibres and Type III for water-saturated fibres. The most striking Raman signature differences are observed in the Raman intensity of the amorphous/‘ordered’ νN–H and H2O band components and correlated to the water content and disorder degree according to the calorimetry study. Types I and II are frequently observed for fresh (largely amorphous) spun fibres/baves. Type V is characteristic of degraded fibres. Type IV represents the most ordered state. The similar stress–strain types for dried silkworm and spider fibres show that the general difference in amino acid contents is not the most pertinent parameter for the mechanical behaviour.
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Philippe Colomban, Hung Manh Dinh, Anthony R. Bunsell, Bernard Mauchamp. Origin of the variability of the mechanical properties of silk fibres: 1. The relationship between disorder, hydration and stress/strain behaviour. Journal of Raman Spectroscopy, Wiley, 2012, 43 (3), pp.425-432. ⟨10.1002/jrs.3044⟩. ⟨hal-01109327⟩

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