Direct 4D printing of functionally graded hydrogel networks for biodegradable, untethered, and multimorphic soft robots

Abstract

<jats:title>Abstract</jats:title> <jats:p>Recent advances in functionally graded additive manufacturing (FGAM) technology have enabled the seamless hybridization of multiple functionalities in a single structure. Soft robotics can become one of the largest beneficiaries of these advances, through the design of a facile four-dimensional (4D) FGAM process that can grant an intelligent stimuli-responsive mechanical functionality to the printed objects. Herein, we present a simple binder jetting approach for the 4D printing of functionally graded porous multi-materials (FGMM) by introducing rationally designed graded multiphase feeder beds. Compositionally graded cross-linking agents gradually form stable porous network structures within aqueous polymer particles, enabling programmable hygroscopic deformation without complex mechanical designs. Furthermore, a systematic bed design incorporating additional functional agents enables a multi-stimuli-responsive and untethered soft robot with stark stimulus selectivity. The biodegradability of the proposed 4D-printed soft robot further ensures the sustainability of our approach, with immediate degradation rates of 96.6% within 72 h. The proposed 4D printing concept for FGMMs can create new opportunities for intelligent and sustainable additive manufacturing in soft robotics.</jats:p>