Cyclic Macroscopic Assembly and Disassembly Driven by Ionic Strength Fuel: A Waste-Free Approach

Nonequilibrium assembling systems developed so far have relied on chemical fuels to drive the programmable pH cycles, redox reactions, and metastable bond formations. However, these methods often result in the unwanted accumulation of chemical waste. Herein, we present a novel strategy for achieving cyclic and waste-free nonequilibrium assembly and disassembly of macroscopic hydrogels, utilizing an ionic strength-mediated approach. Our strategy involves using ammonium carbonate as a chemical fuel to temporally regulate the attractions between oppositely charged hydrogels via ionic strength-controlled charge screening and hydrogel elasticity changes. This chemical fuel effectively mediates the assembly/disassembly processes and prevents waste accumulation, as ammonium carbonate can completely decompose into volatile chemical waste. The cyclic and reversible assembly process can be achieved without significant damping due to the self-clearance mechanism, as long as the chemical fuel is repeatedly supplied. This concept holds promise for creating macroscopic and microscopic nonequilibrium systems and self-adaptive materials.