The Cellulose Loading and Silylation Effects on the Mechanical Properties of Epoxy Composites: Insights from Classical and Reactive Molecular Dynamics Simulations

This study investigates the effect of silylation and cellulose loading on the mechanical properties of epoxy composites. We use the hydrolyzed 3-Aminopropyltriethoxysilane (KH550) as a crosslinker for epoxy and as a coupling agent for cellulose. The mechanical properties of the epoxy composites are evaluated using molecular dynamics simulations. The improvement in the interfacial adhesion between epoxy and cellulose, achieved by using KH550, is demonstrated through the pulling out of cellulose from the epoxy composites. The results indicate that the nanocovalent bonds formed by KH550 at the epoxy/cellulose interface have a higher enhancement effect on the pulling force compared to increasing the cellulose content. For instance, the force needed for pulling 44.1 wt.% of raw cellulose is 93 ± 5 (kcal/mol)/Å, while the one required to pull the 28.1 wt.% of silylated cellulose is 97 ± 4 (kcal/mol)/Å. The silylated cellulose at 28.1 wt.% enhances the tensile modulus, shear modulus, and strength of the epoxy-KH550 composite by 14.55%, 15.65%, and 15.64%, respectively, compared to its counterpart reinforced with raw cellulose. Using the silylation treatment on cellulose that reinforces epoxy-KH550 at 43.9 wt.% improves the elastic modulus, shear modulus, and tensile strength of the epoxy composite by 4.23%, 4.64%, and 18.07%, respectively.