Atomic-scale strain engineering of atomically resolved Pt clusters transcending natural enzymes

Area of Science:

• Materials Science
• Nanotechnology
• Biocatalysis

Background:

• Strain engineering is crucial for optimizing biocatalyst electronic structure and catalytic performance.
• Precisely controlling atomic-scale strain for enzyme-like reactions remains a significant challenge.

Purpose of the Study:

• To investigate the relationship between atomic strain and enzyme-like catalytic activity.
• To design and evaluate platinum single atoms, small clusters, and atomically resolved clusters on palladium-gold biocatalysts.

Main Methods:

• Systematic design of platinum nanostructures (Pt1, Ptn, Ptc) on PdAu biocatalysts.
• Experimental characterization and Density Functional Theory (DFT) calculations.
• Evaluation of peroxidase (POD)-like, catalase (CAT)-like, and superoxide dismutase (SOD)-like activities.

Main Results:

• Atomically resolved platinum clusters on PdAu (Ptc-PA) with optimal strain upshifted the d-band center and increased active sites.
• Ptc-PA demonstrated exceptional POD-like activity (Kcat/Km = 1.50 × 10^9 mM^-1 min^-1), surpassing natural horseradish peroxidase (HRP) by four orders of magnitude.
• Comparable CAT-like and SOD-like activities were observed, alongside significant improvements in a cancer diagnostic system and mitigation of inflammatory damage.

Conclusions:

• Atomic strain engineering of platinum clusters on PdAu is an effective strategy for developing high-performance biocatalysts.
• Ptc-PA exhibits remarkable multi-enzyme-like activities with potential for advanced diagnostics and therapeutic applications.
• The Pd shell and Au core contribute by storing energetic charge carriers, enhancing overall performance.