One-Pot Assembly of Microfibrillated Cellulose Reinforced PVA–Borax Hydrogels with Self-Healing and pH-Responsive Properties

A facile, environmentally benign approach has been developed for the preparation of dynamic, multiresponsive, and self-healing hydrogels from inexpensive bamboo pulp, poly(vinyl alcohol) (PVA), and borax. The microfibrillated cellulose (MFC) reinforced PVA–borax hydrogels were produced through a one-pot route in conjunction with ball milling and physical blending in tandem in aqueous medium. In this way, MFC particles could be efficiently generated and well-dispersed in a polymer matrix, and they have been verified by scanning electron microscopy. The rheology analysis indicated a close relationship between the mechanical strength and the MFC loading and ball milling time. Due to the dynamic equilibrium of the didiol–borax linkages and the reinforcement of MFC fibers, the hydrogels showed enhanced self-healing behavior and mechanical stiffness, which was also supported by rheology analyses. In addition, the hydrogels were found to be sensitive to the pH value. The hydrogels present a solvent or gel state with the change of pH value, and this sol–gel transfer can be repeated while maintaining the shape, further demonstrating the dynamic reversible behavior of the hydrogels.