An Immobilized Rh-Based Solid Molecular Catalyst for the Reductive Hydroformylation of 1-Octene

Area of Science:

• Catalysis
• Organic Chemistry
• Materials Science

Background:

• Reductive hydroformylation is key for alcohol synthesis but often uses complex homogeneous catalysts.
• Homogeneous catalysts pose challenges in recycling and downstream processing, increasing energy demands.

Purpose of the Study:

• To develop a heterogeneous reductive hydroformylation catalyst for simplified alcohol production.
• To improve catalyst performance through iterative macroligand modification.

Main Methods:

• Immobilization of Rhodium (Rh) on polymeric amine macroligands to create solid molecular catalysts (SMCs).
• Iterative enhancement of macroligands by increasing basicity and amine group density.
• Testing SMC performance in solvent-free reductive hydroformylation of olefins.

Main Results:

• Olefins were fully converted to >99% alcohols using the optimized SMC.
• The process operated in a solvent-free environment, eliminating intermediate aldehyde isolation.
• The heterogeneous catalyst demonstrated successful recycling over 12 runs with low Rh leaching (1.2%).

Conclusions:

• Solid molecular catalysts (SMCs) offer an efficient and simplified route for reductive hydroformylation.
• Optimized macroligand design is crucial for catalyst performance and stability.
• The Rh to macroligand ratio is a critical parameter for minimizing metal loss in heterogeneous catalysis.