Bioinspired Allosteric Peroxidase-like Enzyme with Dynamic 3D Catalytic Centers for Advanced Water Treatment

Area of Science:

• Biomimetic catalysis
• Advanced water treatment
• Nanomaterials

Background:

• Natural enzymes utilize precise 3D active site coordination for efficient catalysis.
• Transition metals are often over-relied upon in advanced water treatment processes.
• Developing biomimetic catalysts can offer sustainable alternatives.

Purpose of the Study:

• To engineer a biomimetic enzyme mimicking heme peroxidase (POD) functionality.
• To create a dynamic 3D catalytic center using hemin and C3N4 nanosheets.
• To reduce reliance on transition metals in water purification.

Main Methods:

• Scalable self-assembly of hemin with C3N4 nanosheets via π-π stacking and Fe-N coordination.
• Characterization of the biomimetic catalyst's structure and coordination environment.
• Activity assays using hydrogen peroxide (H2O2) and peroxymonosulfate (PMS) activation.

Main Results:

• The biomimetic catalyst exhibited 150-fold and 40-fold activity enhancements with H2O2 and PMS, respectively, compared to free hemin.
• Axial coordination induced nonplanar hemin deformation, weakening Fe d-π conjugation and enabling biomimetic allosteric regulation.
• The catalyst demonstrated high stability, sustained performance (>80% pollutant removal over 150 h), and effectiveness in complex water matrices.

Conclusions:

• The engineered biomimetic catalyst effectively mimics natural enzyme pockets for enhanced POD-like activity.
• Biomimetic allosteric regulation was proposed as a mechanism to accelerate PMS activation.
• This nature-inspired catalytic design offers a scalable solution for advanced water purification, bridging biocatalysis and synthetic catalysis.