Fracture behaviour and toughening mechanisms of dry and wet collagen

The growing interest to the use of collagen films for biomedical applications motivates the analysis of their fracture behaviour in different environments. Studies revealed the decreased mechanical strength and stiffness as well as increased plasticity in water compared to collagen specimens tested in air. However, the fracture behaviour of pure collagen films in both air and water has not been reported so far. In this paper, the entire process of mode-I loading of single-edge notched tension (SENT) specimens was recorded and analysed. In case of in-air (dry) specimens, cracks propagated rapidly in a brittle fashion while large plastic deformations were observed in aqua prior to failure due to crack opening and a blunting mechanism in wet specimens. The fracture-toughness parameters for pure collagen in air and in aqua were estimated using linear-elastic (K_I and G_I) and elasto-plastic (J_I) fracture-mechanics approaches, respectively, following the force-displacement response and deformational behaviour. G_IC and J_I were 1365 ± 112 J/m² and 2500 ± 440 J/m², respectively. Scanning electron microscopy was used to observe the structural changes linked to collagen fibrils in the crack-tip area and the fracture surface. For in-air specimens, the former mostly exhibited extrinsic toughening (usually at micro scale) acting behind the crack-tip, while in-aqua intrinsic toughening acting ahead of a crack tip was found. Fractography of in-air specimens showed no occurrence of voids while multiple micro-voids were found for in-aqua specimens. STATEMENT OF SIGNIFICANCE: The fracture toughness and crack propagation of both mineralised (bone, dentine) and non-mineralised (skin) tissues has been extensively investigated over the past decades. Though these tissues are rich in collagen, the fracture properties of pure collagen have not been quantified yet at macroscale. Considering the applications of collagen films in tissue regeneration, it is essential to perform investigations of their fracture behaviour in both dry and wet conditions. Determining the effect of environment on the fracture behaviour of collagen and understanding its toughening mechanism are essential for prevention of failures during application. Moreover, this would give an insight for fabrication of tougher collagen-based biomaterials for biomedical uses.