Crystallinity of low molar ratio urea-formaldehyde resins modified with cellulose nanomaterials

Inherent crystalline domains present in low formaldehyde to urea (F/U) molar ratio urea-formaldehyde (UF) resins are responsible for their poor adhesion in wood-based composite panels. To modify the crystallinity of low molar ratio (LMR) UF resins, this study investigates the additional effect of cellulose nanomaterials (CNMs), such as cellulose microfibrils (CMFs), cellulose nanofibrils (CNFs), and TEMPO-oxidized CNFs (TEMPO-CNFs) on the crystallinity of modified LMR UF resins. First, two modification methods (post-mixing and in situ) were compared for modified LMR UF resins with TEMPO-CNFs. The modified UF resins with TEMPO-CNFs decreased the nonvolatile solid contents, while increasing the viscosity and gel time. However, the in situ modification of UF resins with TEMPO-CNFs showed lower crystallinity than that of post-mixing. Then, the in situ method was compared for all CNMs to modify LMR UF resins. The modified UF resins with CMFs using the in situ method increased nonvolatile solid contents and viscosity but decreased the gel time. The crystallinity of UF resins modified with TEMPO-CNFs was the lowest even though the crystalline domains were not significantly changed for all modified UF resins. These results suggest that these CNMs should be modified to prevent the formation of crystalline domains in LMR UF resins.