Dimensionality Engineering of Single-Atom Nanozyme for Efficient Peroxidase-Mimicking

Area of Science:

• Materials Science
• Nanotechnology
• Catalysis

Background:

• Enzymatic reactions rely on 3D catalytic pockets for substrate binding and reaction.
• Single-atom nanozymes (SAzymes) mimic natural metalloenzymes but often have 2D active sites.
• Current 2D SAzymes face limitations due to restricted substrate-binding and collaborative features.

Purpose of the Study:

• To engineer dimensionality of 2D Fe-N-4 centers in SAzymes into 3D structures.
• To enhance catalytic activity by overcoming limitations of 2D SAzyme architectures.
• To investigate the role of oxidized sulfur functionalities in SAzyme catalysis.

Main Methods:

• Dimensionality engineering strategy.
• Integration of oxidized sulfur functionalities onto carbon plane.
• Fabrication of 3D Fe-N-4 SAzymes.

Main Results:

• Successfully converted 2D Fe-N-4 centers to 3D structures.
• Oxidized sulfur functionalities facilitated substrate orientation and H2O desorption.
• Achieved a specific activity of 119.77 U mg-1, 6.8 times higher than conventional FeN4C SAzymes.

Conclusions:

• 3D SAzymes with oxidized sulfur exhibit significantly enhanced catalytic activity.
• Dimensionality engineering is a viable strategy for designing high-performance SAzymes.
• This approach offers a pathway for developing advanced nanozyme catalysts.