Heterogeneous Bifunctional Ni Single-Atom Catalyst on Carbon Nitride for Selective C(sp²)-C(sp³) Coupling

Area of Science:

• Catalysis
• Materials Science
• Organic Chemistry

Background:

• Efficient C(sp2)-C(sp3) bond formation is crucial for pharmaceutical synthesis.
• Sustainable heterogeneous catalytic methods for C(sp2)-C(sp3) coupling are underdeveloped.

Purpose of the Study:

• To develop a ligand-tuned heterogeneous bifunctional catalytic system for visible-light-driven C(sp2)-C(sp3) coupling.
• To explore the versatility of single-atom catalysts in organic transformations.

Main Methods:

• Utilized nickel single atoms supported on carbon nitride (Ni1/CN) as the heterogeneous catalyst.
• Employed bidentate bipyridine ligands to tune the catalytic activity.
• Conducted experimental and computational studies to demonstrate catalytic efficiency.
• Investigated ligand modulation for alternative transformations like C-X coupling and aerobic oxidation.

Main Results:

• Achieved efficient C(sp2)-C(sp3) coupling of alkyl boronic esters with high activity and selectivity.
• Demonstrated the system's versatility through ligand modification, enabling C-X coupling (X = O, N) and aerobic oxidation.
• Validated the catalytic performance through experimental and computational analyses.

Conclusions:

• The ligand-tuned Ni1/CN system represents a significant advancement in heterogeneous catalysis for C(sp2)-C(sp3) bond formation.
• This tunable catalytic platform streamlines pharmaceutical synthesis and highlights the potential of single-atom catalysts in green chemistry.
• The catalyst's adaptability opens avenues for diverse complex organic transformations.