Spontaneous Bio‐Derived Porous Hydrogels for Sustainable Pollutant Removal from Contaminated Water

ABSTRACT Spontaneous gelation, which involves in situ polymerization followed by network crosslinking of monomers under ambient or moderately elevated temperatures, occurring without the incorporation of external initiators or catalysts, is a major challenge in polymer chemistry and environmental science. In this work, we report the design and synthesis of amino acid‐derived porous hydrogels prepared via a spontaneous gelation without any external trigger, utilizing a glutamic acid‐derived monomer N‐methacryloyl‐(L)‐glutamic acid (MAGA) without the need for any additional crosslinking agents. Copolymers of MAGA with DMAEMA or DMA are synthesized through free‐radical polymerization and used to initiate gelation with acrylamide via persulfate activation, enabled by the N,N‐dimethyl functionalities in the copolymers. The resulting poly(DMAEMA‐ r ‐MAGA)/PAAm and poly(DMA‐ r ‐MAGA)/PAAm composite hydrogels demonstrated rapid gelation at ambient temperature, significant structural integrity, and tunable porous structures, as confirmed by rheological studies and electron microscopic imaging. These hydrogels exhibited excellent dye adsorption efficiency toward both anionic (Eosin B, Methyl Orange) and cationic (Rhodamine B) organic dyes. The system's ability to form defined shapes via mould printing, along with its bio‐derived fabrication, scalability, and performance, presents a promising route for future use in 3D‐printed devices and sustainable wastewater treatment. This catalyst‐free, crosslinker‐free, and ambient‐condition gelation approach marks a significant step toward environmental friendly hydrogel technologies.