CO₂ reduction on single-atom Ir catalysts with chemical functionalization

Area of Science:

• Materials Science
• Catalysis
• Surface Chemistry

Background:

• Single-atom catalysts (SACs) offer enhanced performance for electrochemical reactions.
• Current methods for stabilizing SACs often rely on defects, limiting their application.
• Developing defect-free stabilization strategies is crucial for advancing SAC technology.

Purpose of the Study:

• To theoretically demonstrate a defect-free functionalization method for attaching IrX3 (X = F or Cl) complexes onto MoS2 monolayers.
• To investigate the efficacy of this ligand-based approach for stabilizing SACs on 2D materials.
• To evaluate the catalytic performance of the resulting MoS2-IrX3 system for CO2 reduction.

Main Methods:

• Theoretical demonstration of defect-free functionalization.
• Utilizing IrX3 (X = F or Cl) complexes for ligand-based stabilization.
• Computational analysis of CO2 reduction pathways on MoS2-IrX3.

Main Results:

• Successfully demonstrated defect-free attachment of IrX3 complexes on MoS2 monolayers.
• The ligand-based method provides a damage-free route for SAC stabilization.
• The MoS2-IrX3 system exhibited efficient CO2 reduction with a small free energy change and low onset potential.
• The Ir d6 shell facilitated adsorption of reaction intermediates due to universal orbital orientations.

Conclusions:

• Defect-free functionalization using SAC-ligand complexes is a superior strategy for stabilizing catalysts on 2D materials.
• This approach opens new avenues for designing advanced catalysts for electrochemical applications, such as CO2 reduction.
• The Ir-based SACs on MoS2 show significant potential for efficient and stable catalytic processes.