A Unified Framework for Co-optimizing Activity, Selectivity, and Stability in Single-Atom Alloy Catalysts for CO₂...

Area of Science:

• Catalysis
• Materials Science
• Computational Chemistry

Background:

• Optimizing single-atom alloy (SAA) catalysts for CO2 electroreduction faces challenges due to vast design spaces and high computational costs.
• Achieving a balance between catalyst stability, activity, and selectivity is crucial for efficient CO2 conversion.

Purpose of the Study:

• To establish a unified computational framework for co-optimizing activity, selectivity, and stability in SAA catalysts.
• To rapidly identify high-performance SAA catalyst designs using data-efficient exploration.

Main Methods:

• Integrated literature-informed design-space construction with physically constrained, data-efficient first-principles exploration.
• Utilized a tightly controlled number of first-principles evaluations to identify optimal catalyst regions.

Main Results:

• Identified Pt1/Cu(100) as an optimal SAA catalyst for CO2 electroreduction.
• Achieved high activity for formic acid (HCOOH) formation and suppressed carbon monoxide (CO) production.
• Demonstrated intrinsic thermodynamic stability of the single-atom configuration.

Conclusions:

• The developed framework enables efficient co-optimization of stability, activity, and selectivity in SAA catalysts.
• Dopant-host electronic coupling at the atomic scale governs product selectivity by stabilizing specific intermediates.
• The study provides transferable design principles for selective CO2 electroreduction catalysts.