Enhancing the sustainable immobilization of laccase by amino-functionalized PMMA-reinforced graphene nanomaterial

Abstract

Human health and the environment are negatively affected by endocrine-disrupting chemicals (EDCs), such as bisphenol A. Therefore, developing appropriate remediation methods is essential for efficiently removing phenolic compounds from aqueous solutions. Enzymatic biodegradation is a potential biotechnological approach for responsibly addressing water pollution. With its high catalytic efficiency and few by-products, laccase is an eco-friendly biocatalyst with significant promise for biodegradation. Herein, two novel supporting materials (NH₂-PMMA and NH₂-PMMA-Gr) were fabricated via the functionalization of poly(methylmethacrylate) (PMMA) polymer using ethylenediamine and reinforced with graphene followed by glutaraldehyde activation. NH₂-PMMA and NH₂-PMMA-Gr were utilized for laccase immobilization with an immobilization yield (IY%) of 78.3% and 82.5% and an activity yield (AY%) of 81.2% and 85.9%, respectively. Scanning electron microscope (SEM) and Fourier-transform infrared (FTIR) were used to study the characteristics of fabricated material supports. NH₂-PMMA-Gr@laccase exhibited an optimal pH profile from 4.5 to 5.0, while NH₂-PMMA@laccase exhibited optimum pH at 5.0 compared to a value of 4.0 for free form. A wider temperature ranges of 40-50 °C was noted for both immobilized laccases compared to a value of 40 °C for the free form. Additionally, it was reported that immobilized laccase outperformed free laccase in terms of substrate affinity and storage stability. NH₂-PMMA@laccase and NH₂-PMMA-Gr@laccase improved stability by up to 3.9 and 4.6-fold when stored for 30 days at 4 °C and preserved up to 80.5% and 86.7% of relative activity after ten cycles of reuse. Finally, the degradation of BPA was achieved using NH₂-PMMA@laccase and NH₂-PMMA-Gr@laccase. After five cycles, NH₂-PMMA@laccase and NH₂-PMMA-Gr@laccase showed that the residual degradation of BPA was 77% and 84.5% using 50 μm of BPA. This study introduces a novel, high-performance material for organic pollution remediation in wastewater that would inspire further progress.

Keywords: Bisphenol A; Degradation; Graphene nanomaterial; Immobilization; Laccase; PMMA polymer; Reusability.