Reversible Surface Engineering of Cellulose Elementary Fibrils: From Ultralong Nanocelluloses to Advanced Cellulosic Materials

). In particular, on the CNF surface, the surface hydroxyl groups are restored by removal of the carboxyl moieties via saponification, which offers a significant opportunity for reconstitution of stronger hydrogen bonding interfaces. Therefore, the resultant CNFs can be used as sustainable building blocks for construction of multidimensional advanced cellulosic materials, e.g., 1D filaments, 2D films, and 3D aerogels. The proposed surface engineering strategy provides a new platform for fully utilizing the characteristics of the cellulose elementary fibrils in the development of high-performance cellulosic materials.