Tunable mechanical behavior of collagen-based films: A comparison of celluloses in different geometries

Collagen (Col) films were reinforced by celluloses in different geometries: microcrystalline cellulose (MCC), cellulosic fines (CF), cellulose nanofiber (CNF) and cellulose nanocrystals (CNC). The reinforcement mechanisms were investigated by the elastoplasticity and fracture appearance. Compared with the fracture stress of collagen film (67.5 MPa), the Col-CNF films effectively borne the stress (95.8 MPa) by intercrystalline fracture, ascribing the abundant hydrogen bonding and mechanical locking between cellulose and collagen. The toughness of Col-CF films was increased by the interfibrillar slippage of CF and pull-off of CF within the matrix, improving the strain-to-break from 8.37% to 12.13%. The films added with MCC and CNC weaken the mechanical behavior, due to the defects and lack of mechanical locking. Besides, the effects of celluloses' geometries on the thickness, density, water-tightness, thermal stability, crystallinity and FTIR of films were also investigated. These provide the evidence that the geometries of fillers diversely improve the behaviors of collagen film offering strategies for the film with adjustable mechanical properties.