A general strategy for synthesizing biomacromolecular ionogel membranes via solvent-induced self-assembly

Two-dimensional (2D) ionogel membranes have emerged as a promising class of materials for broad applications in flexible electronics, smart robotics and artificial intelligence. However, the rapid, reliable and reproducible fabrication of ionogel membranes remains challenging due to difficult-to-control molecular behaviour. To overcome this challenge, we propose a ‘dip and peel’ strategy to exfoliate 2D ionogel membranes from a biomacromolecular gelatum (for example, a cellulose ionogel colloid) by controlling the solvent-induced supramolecular self-assembly. This strategy enables the simple and rapid fabrication of ionogel membranes with tunable shapes, controllable thicknesses, high ionic conductivity up to 14.1 mS cm −1 , good stretchability exceeding 130% and excellent tandem duplication over 700 times. We further extend this strategy to fabricate different ionogel membranes from various biomacromolecules, including silk fibroin, chitosan and guar gum. Our results shed light on exploration of fundamental macromolecular interactions and provide an effective approach to prepare 2D biomacromolecular ionogel membranes with advanced functionalities.