Dual Physically Crosslinked Hydrogels via Multi-Dimensional Carbon Materials for Methylene Blue Adsorption

The development of high-performance adsorbents for treating dye-laden wastewater necessitates a deep understanding of structure–property relationships. This study presents a systematic investigation into the role of carbon material dimensionality (0D biochar, BC; 1D carbon nanotubes, CNT; 2D graphene oxide, GO) in modulating the properties of a dual physically crosslinked sodium alginate/polyacrylamide (SA/PAM) hydrogel for methylene blue (MB) adsorption. A series of composite hydrogels was fabricated via a sequential physical crosslinking strategy. Comprehensive characterization confirmed the successful incorporation and dispersion of carbon materials within the dual network. The three hydrogels showed good mechanical properties. Under the conditions of 25 °C, an initial MB concentration of 100 mg/L, and pH 10–11, the incorporation of carbon materials enhanced the adsorption capacity, with maximum adsorption capacities of 411.5, 410.6, and 422.8 mg/g for BC-H, GO-H, and CNT-H, respectively. Coexisting constituents in real water samples reduce adsorption capacity via competitive adsorption and interfacial interference. After five consecutive adsorption–desorption cycles, the adsorption capacities of BC-H, GO-H, and CNT-H decreased to 57.7%, 67.2%, and 61.7% of their initial values, respectively. Adsorption isotherm and kinetic studies revealed that the process followed the Langmuir model and pseudo-second-order kinetics, indicative of monolayer chemisorption. Mechanistic analysis identified synergistic contributions from electrostatic attraction, π-π stacking, and physical entrapment. Physical structural changes and chemical site occupation are the main reasons for the decrease in the adsorption performance of hydrogels during cyclic use. This work provides a rational design strategy for advanced adsorbents and a theoretical foundation for efficient dye wastewater remediation.