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<p>The continuous release of cationic dyes such as methylene blue (MB) into aquatic systems poses serious environmental concerns due to their chemical stability, persistence, and potential toxicity. In this study, a novel ternary hybrid adsorbent (CS-UiO66-NH<sub>2</sub>/TpPa-1) was rationally engineered by integrating chitosan with a metal–organic framework (UiO-66-NH<sub>2</sub>) and a covalent organic framework (TpPa-1) to enhance adsorption performance through synergistic effects. The composite structure combines the functional groups of chitosan, the high surface area and stability of the MOF, and the π-conjugated framework of the COF, enabling multiple interaction pathways. Comprehensive characterization (FTIR, XRD, SEM, BET, TGA, XRF, and zeta potential) confirmed successful hybridisation and the formation of a hierarchical micro–mesoporous architecture with pH-responsive surface charge (pH<sub>PZC</sub> ≈ 6.4). Batch adsorption studies demonstrated that MB removal is strongly influenced by pH, contact time, initial concentration, and temperature, with optimal performance at pH 7 and 25&#xa0;°C. The composite achieved a high adsorption capacity of 476.64 ± 3.6&#xa0;mg g⁻<sup>1</sup> and a removal efficiency of 98.34 ± 0.7% at 400&#xa0;mg L⁻<sup>1</sup>. Kinetic and isotherm analyses were best described by pseudo-second-order and Langmuir models, respectively, indicating rate control by surface interactions and monolayer adsorption behaviour. Thermodynamic results revealed a spontaneous and endothermic process. The material retained over 90% efficiency after six cycles, demonstrating excellent stability. Collectively, the developed hybrid provides an efficient and robust platform for advanced dye removal driven by synergistic interfacial interactions and hierarchical porosity.</p>

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Supramolecular Chitosan-Based MOF–COF Polymeric Hybrid with Coordinately Assembled UiO-66-NH2 and TpPa-1 Frameworks for Methylene Blue Adsorption

  • 期刊论文

  • 发表日期：

    2026年5月20日

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  • Nuha Y. Elamin,
  • Mohamed Hemdan,
  • Mahmoud F. Mubarak

摘要

The continuous release of cationic dyes such as methylene blue (MB) into aquatic systems poses serious environmental concerns due to their chemical stability, persistence, and potential toxicity. In this study, a novel ternary hybrid adsorbent (CS-UiO66-NH2/TpPa-1) was rationally engineered by integrating chitosan with a metal–organic framework (UiO-66-NH2) and a covalent organic framework (TpPa-1) to enhance adsorption performance through synergistic effects. The composite structure combines the functional groups of chitosan, the high surface area and stability of the MOF, and the π-conjugated framework of the COF, enabling multiple interaction pathways. Comprehensive characterization (FTIR, XRD, SEM, BET, TGA, XRF, and zeta potential) confirmed successful hybridisation and the formation of a hierarchical micro–mesoporous architecture with pH-responsive surface charge (pHPZC ≈ 6.4). Batch adsorption studies demonstrated that MB removal is strongly influenced by pH, contact time, initial concentration, and temperature, with optimal performance at pH 7 and 25 °C. The composite achieved a high adsorption capacity of 476.64 ± 3.6 mg g⁻1 and a removal efficiency of 98.34 ± 0.7% at 400 mg L⁻1. Kinetic and isotherm analyses were best described by pseudo-second-order and Langmuir models, respectively, indicating rate control by surface interactions and monolayer adsorption behaviour. Thermodynamic results revealed a spontaneous and endothermic process. The material retained over 90% efficiency after six cycles, demonstrating excellent stability. Collectively, the developed hybrid provides an efficient and robust platform for advanced dye removal driven by synergistic interfacial interactions and hierarchical porosity.