An in-situ dissolving-co-crosslinking strategy for fabricating high-strength, wet-stable, and biocompatible...

Developing degradable plastics with excellent mechanical strength and wet stability from renewable and biodegradable biomass resources remains challenging. Here, we propose a simple one-step strategy for the in-situ multiscale dissolution of cellulose and crosslinking with 1,4-butanediol diglycidyl ether (BDDE) within a mixture of BDDE and AlCl₃/ZnCl₂ aqueous solution at room temperature. This strategy enables the synthesis of cellulosic paper-based bioplastics with high mechanical strength and wet stability from cellulose paper. In this process, conventional cellulose paper is partially dissolved, and simultaneously, BDDE forms chemical crosslinking with undissolved micro-level, nano-level cellulose fibers and dissolved cellulose macromolecules through an autocatalytic effect from AlCl₃/ZnCl₂ aqueous solution, resulting in multiscale physicochemical entanglements and multiple hydrogen bonds. Hence, the prepared bioplastic's dry and wet strength reached 58.2 MPa and 24.2 MPa, respectively, about 6.9 times and 71.2 times higher than untreated paper-based materials. The prepared bioplastic showed excellent wet stability, biosafety, and biodegradability. The density functional theory (DFT) simulation data indicates that Al³⁺, Zn²⁺ ions, and freely hydrated hydrogen protons are crucial to the dissolving-co-crosslinking system. This strategy involves only green and recyclable chemicals, offering a promising pathway for producing strong and biodegradable cellulosic paper-based bioplastics as an alternative to nondegradable plastics.