Swollen hydrogels with strong mechanical characteristics: A superior adsorbent for the sustainable removal of diclofenac sodium

Hydrogel adsorbents that possess both good mechanical strength and adsorption capabilities are crucial for practical wastewater treatment. However, achieving this balance has been demanding due to the trade-off between swelling properties and adsorption capacities in hydrogels. Although swelling increases the availability of functional groups and facilitates the diffusion of pollutants, it compromises the mechanical integrity. In this study, we address this challenge by developing double-network hydrogels based on poly(vinyl) alcohol and poly[2-(acryloyloxy)ethyl]trimethyl ammonium chloride, prepared via free-radical polymerization, and subsequent freeze–thaw treatment. These hydrogels were investigated for their efficacy in removing diclofenac sodium, a prevalent drug pollutant in pharmaceutical wastewater. By leveraging the synergistic effect of the physical and chemical networks, the prepared hydrogels exhibit intrinsic toughness and compressibility even in a fully swollen state. Most importantly, the maximum adsorption capacity yielded by the Langmuir model fitting was 1012 mg/g under natural conditions, they surpass all other hydrogel adsorbents proposed so far. Thermodynamic analysis implied the spontaneous and exothermic nature of diclofenac sodium adsorption process, while infrared and photoemission spectroscopy revealed that diclofenac sodium uptake is predominantly governed by ion exchange. Overall, double-network hydrogels offer considerable promise for eco-friendly and sustainable wastewater purification due to their high mechanical stability, outstanding adsorption performance, good reusability, and adaptability to diverse environmental conditions.