One-Pot Synthesis of UPy-Functionalized Nanocellulose under Mechanochemical Synergy for High-Performance Epoxy Nanocomposites

The high strength, high specific surface area, excellent biocompatibility, and degradability of nanocellulose (NCC) make it a potential reinforcing phase for composite materials. However, the polyhydroxyl property of NCC renders it prone to self-aggregation and it has weak interfacial compatibility with non-polar substrates, limiting its enhancement performance for composite materials. Therefore, based on the high reactivity of NCC, the chemical modification of NCC to introduce functional groups is the basis for effectively reducing its self-aggregation, improving its interfacial compatibility with the polymer matrix, and creating nanocellulose-based functional materials. The existing functional modifications of NCC have limitations; they require cumbersome steps, generate low yields, and are environmentally unfriendly. Herein, ureido-pyrimidinone (UPy) was introduced to NCC through a sustainable and high-efficiency avenue formed by the mechanochemical synergy of microwaves and ultrasonication. The obtained UPy-modified nanocellulose (NCC-UPy) exhibited a rod-like shape, with a length of 200–300 nm and a width of 20–30 nm, which presented oriented and stable dispersion in an aqueous medium, and the zeta potential reached −40 mV. Moreover, NCC-UPy had good thermostability (>350 °C) and high crystallinity (82.5%) within the crystal type of cellulose I. Using the as-prepared NCC-UPy as a molecular bridge, it was organically combined with epoxy resin through multiple hydrogen bonds to construct a nanocomposite membrane with superior mechanical strength and thermal stability. The results revealed that NCC-UPy dispersed uniformly in the epoxy matrix without aggregating and that the interfacial compatibility was good, leading to an 87% increase in the tensile strength of the formed nanocomposite membrane when 0.5 wt.% NCC-UPy was loaded. It was proved that NCC-UPy had remarkable reinforcing potential and effective stress transfer capacity for composites. Consequently, this study may open the door to the development of a one-pot green approach for undertaking the functional modification of NCC, and it is of great significance for the development of NCC-based nanocomposites.