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<p>A novel biopolymer-based hydrogel composite (KC-g-PIAV/Pa) was developed by grafting κ-carrageenan with itaconic acid, acrylamide, and sodium styrene sulfonate and reinforcing the network with 15 wt% palygorskite (Pa) clay via free radical copolymerization. Structural and morphological characterizations using FTIR, XRD, FESEM/EDX, HRTEM, BET, and TGA confirmed successful grafting, enhanced thermal stability, and the formation of a highly porous, crosslinked architecture. The inclusion of clay significantly improved the hydrogel’s gel content and mechanical integrity, while reducing the swelling ratio due to stronger interfacial interactions. The optimal hydrogel exhibited a BET surface area of 45.6 m<sup>2</sup>·g<sup>−1</sup> and a thermal degradation onset above 300&#xa0;°C. Adsorption experiments using Safranin T (ST) as a model cationic dye showed rapid uptake kinetics following a pseudo-second-order model (R<sup>2</sup> = 0.998), and equilibrium data best fit the Freundlich isotherm (R<sup>2</sup> = 0.991), indicating multilayer adsorption on a heterogeneous surface. The maximum adsorption capacity reached 1223.22&#xa0;mg/g at 25&#xa0;°C and pH 6. Thermodynamic analysis revealed a spontaneous and endothermic process (Δ<i>H</i>° = 14.8&#xa0;kJ·mol<sup>−1</sup>, Δ<i>G</i>° &lt; 0). Density functional theory (DFT) studies supported the involvement of hydrogen bonding, electrostatic attractions, and π–π stacking as dominant adsorption mechanisms. The hydrogel maintained over 80% removal efficiency after five regeneration cycles. These results demonstrate the potential of KC-g-PIAV/Pa as a renewable, high-capacity, and reusable adsorbent for dye-contaminated wastewater treatment.</p>

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Development of a Regenerable κ-Carrageenan/Clay Hydrogel for Sustainable Cationic Dye Removal: A Solution Chemistry and DFT-Guided Study

  • 期刊论文

  • 发表日期：

    2025年12月5日

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  • Aseel M. Aljeboree,
  • Uday Abdul-Reda Hussein,
  • Forat H. Alsultany,
  • Ali Fawzi Al-Hussainy,
  • Salman Khalaf Issa,
  • Ayad F. Alkaim

摘要

A novel biopolymer-based hydrogel composite (KC-g-PIAV/Pa) was developed by grafting κ-carrageenan with itaconic acid, acrylamide, and sodium styrene sulfonate and reinforcing the network with 15 wt% palygorskite (Pa) clay via free radical copolymerization. Structural and morphological characterizations using FTIR, XRD, FESEM/EDX, HRTEM, BET, and TGA confirmed successful grafting, enhanced thermal stability, and the formation of a highly porous, crosslinked architecture. The inclusion of clay significantly improved the hydrogel’s gel content and mechanical integrity, while reducing the swelling ratio due to stronger interfacial interactions. The optimal hydrogel exhibited a BET surface area of 45.6 m2·g−1 and a thermal degradation onset above 300 °C. Adsorption experiments using Safranin T (ST) as a model cationic dye showed rapid uptake kinetics following a pseudo-second-order model (R2 = 0.998), and equilibrium data best fit the Freundlich isotherm (R2 = 0.991), indicating multilayer adsorption on a heterogeneous surface. The maximum adsorption capacity reached 1223.22 mg/g at 25 °C and pH 6. Thermodynamic analysis revealed a spontaneous and endothermic process (ΔH° = 14.8 kJ·mol−1, ΔG° < 0). Density functional theory (DFT) studies supported the involvement of hydrogen bonding, electrostatic attractions, and π–π stacking as dominant adsorption mechanisms. The hydrogel maintained over 80% removal efficiency after five regeneration cycles. These results demonstrate the potential of KC-g-PIAV/Pa as a renewable, high-capacity, and reusable adsorbent for dye-contaminated wastewater treatment.