Sustainable design of carboxymethyl cellulose-integrated cationic hybrids: Multicomponent polymerization towards poly(tertiary amine) polymers in one-pot fashion

Carboxymethyl cellulose (CMC)-integrated cationic hybrids were successfully fabricated via a one-pot multi-component polymerization strategy to design poly(2-(dimethylamino)ethyl methacrylate-co-N-(3-(dimethylamino)propyl methacrylamide), P(DAEM-co-DAPMA) network. The methacrylate/methacrylamide ratio is a critical parameter for modifying the elasticity and overall performance of hybrids to the desired extent. The investigation clarified how CMC integration optimizes the balance between DAEM-induced functionality and DAPMA-induced stability. Reducing the polymerization temperature to cryoconditions resulted in higher compressive modulus in hybrid cryogels, while increasing methacrylate/methacrylamide ratio increased flexibility. The overall swelling of hybrid cryogels improved significantly with higher DAPMA content, despite causing a 5.4-fold decline in modulus from 27.2 to 4.97 kPa. The hybrids exhibited a pH-dependent U-shaped swelling, where changing the electrostatic repulsions among DAEM, DAPMA, and CMC directly controlled the expansion. For adsorption of anionic azorubine dye, hybrid compositions were optimized across pH, initial concentrations, and contact times. Using a minimum adsorbent dosage of 10 mg at pH 3.0, the hybrids effectively removed higher dye concentrations up to 250 mg/L. In particular, 30 mol% DAPMA-containing hybrid achieved exceptional adsorption capacities ranging from 94.15 to 450.59 mg/g as initial concentration increased. Adsorption process followed pseudo second-order kinetics, conforming to Langmuir monolayer isotherm. The ability to precisely customize swelling profile and mechanical integrity of poly(tertiary amine)-based hybrids by adjusting feed methacrylate/methacrylamide ratio provides a level of structural control for targeted applications. Adsorption results highlight that CMC-integrated hybrid cryogels are not only an alternative but also a pioneering, high-capacity, and economically viable platform for next-generation industrial wastewater treatment.