An atomically precise Au₁₀(DPPF)₄PPh₃ cluster catalyst for N-hydroformylation of amines

Area of Science:

• Heterogeneous Catalysis
• Nanomaterials Chemistry
• Sustainable Chemistry

Background:

• Catalysis is vital for societal well-being, driving continuous innovation in chemical processes.
• Developing efficient catalysts for CO2 utilization is a key challenge in sustainable chemistry.
• Atomically precise metal clusters offer unique catalytic properties.

Purpose of the Study:

• To report a novel catalytic system for N-hydroformylation of pyrrolidine using CO2 and H2.
• To investigate the synergistic roles of ligands and a gold metal core in catalysis.
• To achieve high activity and stability in CO2 conversion.

Main Methods:

• Synthesis of an atomically precise gold cluster catalyst: Au10(DPPF)4PPh3.
• Utilizing the catalyst for N-hydroformylation of pyrrolidine with CO2 and H2.
• Characterization of catalytic intermediates and reaction mechanisms.

Main Results:

• The Au10 cluster catalyst demonstrated efficient N-hydroformylation of pyrrolidine.
• The catalyst's dual functional units (ligands and Au10 core) contributed to stability and activity.
• The reaction proceeds via hydrogenation of CO2 to a formic acid intermediate, followed by formylation.
• The catalyst outperformed existing systems under similar conditions.

Conclusions:

• The developed Au10 cluster catalyst offers a promising route for CO2 valorization.
• Synergy between catalyst components is crucial for optimal performance.
• This catalytic system advances sustainable chemical synthesis through efficient CO2 conversion.