Pushing the Performance Limit of Cu/CeO₂ Catalyst in CO₂ Electroreduction: A Cluster Model Study for Loading Single...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Single-atom catalysts offer high efficiency for CO2 electroreduction but face challenges with loading and stability.
• Developing a suitable model system is crucial for optimizing single-atom catalyst design.
• Cerium oxide (CeO2) clusters present a promising support material due to their high surface-to-volume ratio.

Purpose of the Study:

• To establish a model system for loading single copper (Cu) atoms onto ultrasmall CeO2 clusters.
• To determine the optimal configuration of Cu single atoms on CeO2 for enhanced CO2 electroreduction.
• To investigate the performance limits and stability of the developed single-atom catalyst.

Main Methods:

• Synthesis of ultrasmall CeO2 clusters (2.4 nm) with atomic precision.
• Loading of single Cu atoms onto the CeO2 cluster support.
• Characterization using multiple techniques and theoretical calculations to identify loading sites and limits.
• Electrochemical testing for CO2 electroreduction to methane (CH4).

Main Results:

• An optimal configuration for Cu single atoms on CeO2 clusters was identified.
• The optimized catalyst achieved a maximum Faradaic efficiency (FE) of 67% for CH4 production.
• High CH4 FE (>50%) was maintained across a broad range of current densities (-50 to -600 mA/cm2).

Conclusions:

• Ultrasmall CeO2 clusters serve as an effective model system for loading single Cu atoms.
• The developed single-atom catalyst significantly enhances CO2 electroreduction performance for CH4 generation.
• This work provides a pathway for designing high-performance single-atom catalysts for practical CO2 utilization.