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<p>Metal-organic frameworks (MOFs), with their highly tunable molecular architecture, offer remarkable opportunities for sustainable material design and biomedical applications. Building on this potential, this study demonstrates that MIL-101(Cr), prepared via a sustainable synthesis route, serves as an efficient platform for immobilizing bovine hemoglobin (BHb). Here, we report an eco-friendly hydrothermal synthesis of MIL-101(Cr) utilizing terephthalic acid (TPA) upcycled from polyethylene terephthalate (PET) waste. This approach represents a safe and environmentally conscious alternative to traditional methods. The resulting MIL-101(Cr) was comprehensively characterized using XRD, FT-IR, FESEM, EDX, DLS, BET, and TGA analyses. BHb was immobilized onto the MIL-101(Cr) surface, and the dependence of its adsorption capacity on various environmental conditions, pH, initial BHb concentration, temperature, and ionic strength, was investigated. Adsorption studies of Hb@MIL-101(Cr) composite demonstrated a maximum monolayer capacity of 296.49&#xa0;mg g<sup>−1</sup> at optimal conditions (pH 6.0), which further increased to 655.89&#xa0;mg g<sup>−1</sup> under elevated ionic strength (1.0&#xa0;M NaCl) due to electrostatic screening. The adsorption process, best described by the Langmuir isotherm and pseudo-second-order kinetics, was thermodynamically spontaneous and endothermic. Successful surface-mediated immobilization was directly confirmed by the emergence of an Fe 2p signal (0.3 At.%) in XPS and the retention of characteristic amide bands in FT-IR. Furthermore, SDS-PAGE analysis verified that MIL-101(Cr) preserved the structural integrity of the BHb polypeptide chains without inducing proteolytic degradation. Retaining 77.7% of its initial adsorption performance after three consecutive cycles, the composite exhibited robust reusability. These findings highlight the potential of integrating PET upcycling with MOF chemistry to deliver sustainable, high-capacity platforms for bio-macromolecule immobilization.</p>

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The Sustainable Synthesis of MIL-101(Cr) from Upcycled PET Waste and Its Adsorption Capacity for Bovine Hemoglobin Immobilization

  • 期刊论文

  • 发表日期：

    2026年6月28日

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  • Öznur Ölmez Nalcıoğlu,
  • Berna Kavakcıoğlu Yardımcı,
  • Koray Şarkaya,
  • Ayşe Gül Caniklioğlu

摘要

Metal-organic frameworks (MOFs), with their highly tunable molecular architecture, offer remarkable opportunities for sustainable material design and biomedical applications. Building on this potential, this study demonstrates that MIL-101(Cr), prepared via a sustainable synthesis route, serves as an efficient platform for immobilizing bovine hemoglobin (BHb). Here, we report an eco-friendly hydrothermal synthesis of MIL-101(Cr) utilizing terephthalic acid (TPA) upcycled from polyethylene terephthalate (PET) waste. This approach represents a safe and environmentally conscious alternative to traditional methods. The resulting MIL-101(Cr) was comprehensively characterized using XRD, FT-IR, FESEM, EDX, DLS, BET, and TGA analyses. BHb was immobilized onto the MIL-101(Cr) surface, and the dependence of its adsorption capacity on various environmental conditions, pH, initial BHb concentration, temperature, and ionic strength, was investigated. Adsorption studies of Hb@MIL-101(Cr) composite demonstrated a maximum monolayer capacity of 296.49 mg g−1 at optimal conditions (pH 6.0), which further increased to 655.89 mg g−1 under elevated ionic strength (1.0 M NaCl) due to electrostatic screening. The adsorption process, best described by the Langmuir isotherm and pseudo-second-order kinetics, was thermodynamically spontaneous and endothermic. Successful surface-mediated immobilization was directly confirmed by the emergence of an Fe 2p signal (0.3 At.%) in XPS and the retention of characteristic amide bands in FT-IR. Furthermore, SDS-PAGE analysis verified that MIL-101(Cr) preserved the structural integrity of the BHb polypeptide chains without inducing proteolytic degradation. Retaining 77.7% of its initial adsorption performance after three consecutive cycles, the composite exhibited robust reusability. These findings highlight the potential of integrating PET upcycling with MOF chemistry to deliver sustainable, high-capacity platforms for bio-macromolecule immobilization.