Zipper-inspired molecular polarity strategy enabling robust adhesive hydroplastics as sustainable plastic substitutes

Hydroplastics with water-plasticizing effects and programmability are highly desired yet challenges arise from assembling renewable cellulose into hydroplastics with reversible adhesion and enhanced mechanical performance through water-enhancement effects. Here, inspired by zippers, the issue that water molecules are difficult to enhance the comprehensive performances of hydroplastics is addressed by regulating molecular-scale polarity using thioctic acid (TA), combined with reconfigured molecular network under imbalanced polarity environment created by water. This approach enables the fabrication of transparent cellulose hydroplastics (91%) with mechanical performance that can be enhanced to 203 MPa under hydration-dehydration cycles, surpass most cellulose hydroplastics. Moreover, unlike conventional cellulose hydroplastics, the hydroplastic exhibits excellent water-induced reversible adhesion (up to 37 MPa) and rapid programmability (5 minutes). These unique performance advantages open a unique avenue for cellulose to prepare high-performance multifunctional hydroplastics from top-down, dedicated to replacing traditional plastics and reducing the consumption of petrochemical resources. Assembling cellulose into hydroplastics through water-enhanced effects remains challenging. Here the authors demonstrate that modulating the polarity by using thioctic acid leads to a reconfigured network with enhanced mechanical properties and reversible adhesion.