Cellulose‐Based Crosslinker Tailored Smart Hydrogel: Unlocking Excellent Mechanical Properties and Adaptive Dye Removal Control

ABSTRACT Smart adsorption material toward both anionic and cationic dyes have been reported rarely, despite bright prospects in dye adsorption. Polyampholyte is a potential ideal candidate. PAAD (copolymer of acrylamide, acrylic acid and [2‐(Methacryloyloxy) ethyl] dimethyl‐(3‐sulfopropyl) ammonium hydroxide) is a novel thermo‐responsive hydrogel based on polyampholyte, whereas inferior mechanical properties induce fracture during the adsorption process. Herein, we designed a novel cellulose‐based crosslinker, which constructs both a robust backbone and reconfigurable physical entanglements in the PAAD‐matrix hydrogel to improve the fracture strength and elongation by nearly 195.70% and 360.65%. Meanwhile, the physical entangle is disentangled during deformation and could be re‐entangled after deformation, endowing the hydrogel with efficient energy dissipation, fatigue resistance and self‐recovery ability, while the highly rigid chemically crosslinked backbone could maintain the shape of the hydrogel under stress. Moreover, the hydrogel can be used as a controllable adsorption material toward both cationic and anionic dyes, which could greatly increase adsorption capacity after reaching UCST due to its temperature‐sensitive characteristics.