Toughening Effect of Rodlike Cellulose Nanocrystals in Epoxy Adhesive

Epoxy structural adhesives have been used extensively in the automotive and aerospace industries to bond assembly parts. Much effort has been devoted to enhancing the mechanical properties of epoxy resin by incorporating fillers. Among a variety of fillers investigated for this purpose, nanocelluloses are regarded as a promising type of emerging green filler material because of their excellent mechanical and physicochemical properties. Indeed, nanocelluloses have been used as a filler for polymer nanocomposites. However, the toughening and reinforcing effects of nanocelluloses on rigid epoxy adhesives have not yet been fully revealed, particularly from the perspective of adhesive bonded joints. Here we report that epoxy adhesive containing cellulose nanocrystal (CNC) aggregates produced using a solvent-free ball milling method achieves drastically improved adhesive strength and fracture toughness compared with that of the reference adhesive without CNCs. The epoxy adhesive containing CNC aggregates exhibited an excellent adhesive strength of 29 MPa and a fracture toughness of 389 J/m2, which were 125% and 378% greater than those of epoxy adhesive without CNCs, respectively.