Sodion Induced Interfacial Polarization and π-π Synergy Enable Irreversible Dye Adsorption in g-C3N4 Quantum Dot-Embedded Hydrogels
摘要
Hydrogel-based adsorbents have attracted increasing attention for dye wastewater treatment due to their structural tunability and high water content. In this work, g-C3N4 quantum dot/polyacrylamide (CNQD/PAM) and TiO2 quantum dot/polyacrylamide (TDQD/PAM) hydrogels were constructed as interfacial model systems to investigate how quantum-dot chemistry influences adsorption strength and reversibility toward methylene blue (MB). Under identical conditions, CNQD/PAM exhibited a significantly higher adsorption capacity and markedly enhanced dye retention than TDQD/PAM, retaining approximately 86.9% of adsorbed MB after 24 h desorption, whereas TDQD/PAM retained only 22.2%. Dual-site diffusion-adsorption modeling indicated comparable mass-transfer resistance for both systems, while CNQD/PAM possessed a larger fraction of kinetically stable adsorption sites with strongly suppressed desorption. Spectroscopic and pH-dependent analyses suggest that nitrogen-rich and conjugated g-C3N4 domains provide cooperative noncovalent interactions, including π-π stacking and electrostatic effects. This study highlights the critical role of interfacial electronic characteristics in regulating adsorption reversibility and provides guidance for designing durable hydrogel adsorbents.
Graphical abstract